**Experimental Aspect**

[23] Kotlyar, A. V., & Feodosyev, S. B. (2006). Local Vibrational Modes in Crystal Lattices with a Simply Connected Region of the Quasi-continuous Phonon Spectrum. *Low*

[24] Gospodarev, I. A., Eremenko, V. V., Kravchenko, K. V., Sirenko, V. A., Syrkin, E. S., & Feodos'ev, S. B. (2010). Vibrational Charakteristics of Niobium Diselenide and

[25] Novoselov, K. S. (2010). Grafen: Materialy Flatlandii. *Uspehi Fizicheskih Nauk (in Rus‐*

[26] Dahal Hari, P., Balatsky, A. V., & Zhu, J-X. (2008). Tuning Impurity States in Bilayer

[27] Wang, Z. F., Li, Q., Su, H., Wang, H., Shi, Q. W., Chen, J., Yang, J., & Hou, J. G. (2007). Electronic Sructure of Bilayer Graphene; Areal-Space Green's Function Study.

[28] Castro, E. V., Peres, N. M., Lopes dos Santos, J. M. B., Castro Neto, A. H., & Guinea, F. (2008). Localized States at Zigzag Edges of Bilayer Graphene. *Physical Review Let‐*

Graphite Nanofilms. *Low Temperature Physics*, 36(4), 344-350.

Graphene. *Physical Review*, 77(11), B 115114, 1-10.

*Temperature Physics*, 32(3), 256-269.

*Physical Review*, 78(8), B 085424, 1-8.

*sian)*, 181(12), 1299-1311.

158 New Progress on Graphene Research

*ters*, 100(26), 026802, 1-4.

**Chapter 6**

**Quantum Transport in Graphene Quantum Dots**

Graphene exhibits unique electrical properties and offers substantial potential as building blocks of nanodevices owing to its unique two-dimensional structure (Geim et al., 2007; Geim et al., 2009; Ihn et al., 2010). Besides being a promising candidate for high performance electronic devices, graphene may also be used in the field of quantum computation, which involves explo‐ ration of the extra degrees of freedom provided by electron spin, in addition to those due to elec‐ tron charge. During the past few years, significant progress has been achieved in implementation of electron spin qubits in semiconductor quantum dots (Hanson et al., 2007; Hanson et al., 2008). To realize quantum computation, the effects of interactions between qubits and their environment must be minimized (Fischer et al., 2009). Because of the weak spin-orbit coupling and largely eliminated hyperfine interaction in graphene, it is highly desirable to co‐ herently control the spin degree of freedom in graphene nanostructures for quantum computa‐ tion (Trauzettel et al., 2007; Guo et al., 2009). However, the low energy quasiparticles in single layer grapheme behave as massless Dirac fermions (Geim et al., 2007; Geim et al., 2009), and the relativistic Klein tunneling effect leads to the fact that it is hard to confine electrons within a small region to form quantum dot in graphene using traditional electrostatical gates (Ihn et al., 2010; Trauzettel et al., 2007). It is now possible to etch a grapheme flake into nano-constrictions in size, which can obtain electron bound states and thus act as quantum dots. As a result, usually a dia‐ mond-like characteristic of suppressed conductance consisting of a number of sub-diamonds is clearly seen (Stampfer et al., 2009; Gallagher et al., 2010), indicating that charge transport in the single graphene quantum dot device may be described by the model of multiple graphene quan‐ tum dots in series along the nanoribbon. The formation of multiple quantum dot structures in the nanoribbons may be attributed to edge roughness or local potential. The rough edges also lift the valley degeneracy, which could suppress the exchange coupling between spins in the gra‐ pheme quantum dots (Trauzettel et al., 2007; Ponomarenko et al., 2008). Recently, there was a

> © 2013 Li et al.; licensee InTech. This is an open access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use,

© 2013 Li et al.; licensee InTech. This is a paper distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

distribution, and reproduction in any medium, provided the original work is properly cited.

Hai-Ou Li, Tao Tu, Gang Cao, Lin-Jun Wang,

Additional information is available at the end of the chapter

Guang-Can Guo and Guo-Ping Guo

http://dx.doi.org/10.5772/52873

**1. Introduction**

## **Quantum Transport in Graphene Quantum Dots**

Hai-Ou Li, Tao Tu, Gang Cao, Lin-Jun Wang, Guang-Can Guo and Guo-Ping Guo

Additional information is available at the end of the chapter

http://dx.doi.org/10.5772/52873

#### **1. Introduction**

Graphene exhibits unique electrical properties and offers substantial potential as building blocks of nanodevices owing to its unique two-dimensional structure (Geim et al., 2007; Geim et al., 2009; Ihn et al., 2010). Besides being a promising candidate for high performance electronic devices, graphene may also be used in the field of quantum computation, which involves explo‐ ration of the extra degrees of freedom provided by electron spin, in addition to those due to elec‐ tron charge. During the past few years, significant progress has been achieved in implementation of electron spin qubits in semiconductor quantum dots (Hanson et al., 2007; Hanson et al., 2008). To realize quantum computation, the effects of interactions between qubits and their environment must be minimized (Fischer et al., 2009). Because of the weak spin-orbit coupling and largely eliminated hyperfine interaction in graphene, it is highly desirable to co‐ herently control the spin degree of freedom in graphene nanostructures for quantum computa‐ tion (Trauzettel et al., 2007; Guo et al., 2009). However, the low energy quasiparticles in single layer grapheme behave as massless Dirac fermions (Geim et al., 2007; Geim et al., 2009), and the relativistic Klein tunneling effect leads to the fact that it is hard to confine electrons within a small region to form quantum dot in graphene using traditional electrostatical gates (Ihn et al., 2010; Trauzettel et al., 2007). It is now possible to etch a grapheme flake into nano-constrictions in size, which can obtain electron bound states and thus act as quantum dots. As a result, usually a dia‐ mond-like characteristic of suppressed conductance consisting of a number of sub-diamonds is clearly seen (Stampfer et al., 2009; Gallagher et al., 2010), indicating that charge transport in the single graphene quantum dot device may be described by the model of multiple graphene quan‐ tum dots in series along the nanoribbon. The formation of multiple quantum dot structures in the nanoribbons may be attributed to edge roughness or local potential. The rough edges also lift the valley degeneracy, which could suppress the exchange coupling between spins in the gra‐ pheme quantum dots (Trauzettel et al., 2007; Ponomarenko et al., 2008). Recently, there was a

© 2013 Li et al.; licensee InTech. This is an open access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. © 2013 Li et al.; licensee InTech. This is a paper distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

striking advance on experimental production of graphene single (Ponomarenko et al., 2008; Stampfer et al., 2008a; Stampfer et al., 2008 b; Schenz et al., 2009; Wang et al., 2010; Guttinger et al., 2011) or double quantum dots (Molitor et al., 2009; Molitor et al., 2010; Liu et al., 2010; Wang et al., 2011a; Volk et al., 2011; Wang et al., 2012;) which is an important first step towards such promise.

tween the QD and the detector. However, in our device reported here, the QD and the SET in the same material are defined in a single etching step, and the distance between the graphene nano‐ structures is determined by the etched area, which enables optimized coupling and sensing abili‐ ty. The SET is placed in close proximity to the QD giving rise to a strong capacitive coupling between the two systems. Once an additional electron occupies the QD, the potential in the neigh‐ boring SET is modified by capacitive interaction that gives rise to a measurable conductance change. Even if charge transport through the QD is too small to be measured by conventional transport means, the SET charge sensor also allows measurements. These devices demonstrated

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163

The graphene flakes were produced by mechanical cleaving of graphite crystallites by Scotch tape and then were transferred to a highly doped Si substrate with a 100 nm SiO2 top layer. Thin flakes were found by optical microscopy, and single layer graphene flakes were selected by the Raman spectroscopy measurement. We used the standard electron beam lith‐ ography and lift off technique to make the Ohmic contact (Ti/Au) on the present graphene devices. Next, a new layer of polymethyl methacrylate is exposed by electron beam to form a designed pattern. Then, the unprotected areas are removed by oxygen reactive ion etching. One of our defined sample structures with a quantum dot and proximity SET is shown in Fig. 1. The quantum dot is an isolated central island of diameter 90 nm, connected by 30nm wide tunneling barriers to source and drain contacts. Here, the Si wafer was used as the back gate and there is also a graphene side gate near the small dot. The SET has a similar pattern while the conducting island has a much larger diameter (180nm). Electronic trans‐ port through both the devices exhibits Coulomb blockade (CB) characteristics with back/side gate voltage. The distance between the CB peaks is determined by the sum of charging and quantum confinement energies, and the former contribution becomes dominant for our de‐ vices with diameter >100nm (Kouwenhoven et al., 1997). Accordingly, we refer to it as a SET rather than a QD. The device was first immersed into a liquid helium storage Dewar at 4.2K to test the functionality of the gates. The experiment was carried out in a top-loading dilu‐ tion refrigerator equipped with filtered wiring and low-noise electronics at the base temper‐

ature of 10 mK. In the measurement, we employed the standard ac lock-in technique.

Fig. 2(a) shows the conductance through the dot Al/AlOx/Al for applied side gate voltage Vsg. Clear CB peaks are observed related to charging of the tunable dot on the graphene. The dashed green lines in the range of 0.2-0.7V for side gate voltages show that the current through the dot be‐ comes too small to be seen clearly. Fig. 2(b) shows the conductance through the SET versus side gate voltage Vsg. The SET is as close as possible to the QD and in this way charging signals of the dot were detected by tracking the change in the SET current. The addition of one electron to the QD leads to a pronounced change of the conductance of the charge detector by typically 30%. The slope of the SET conductance is the steepest at both sides of its CB resonances giving the best charge read-out signal. To offset the large current background, we used a lock-in detection meth‐ od developed earlier for GaAs dot (Elzerman et al., 2004b). A square shaped pulse was superim‐ posed on the dc bias on side gate voltage Vsg. A lock-in detector in sync with the pulse frequency measured the change of SET current due to the pulse modulation. Fig. 2(c) shows a typical trace of the lock-in signal of the transconductance through the SET *dI*SET/*dV*sg. These sharp spikes or dips originate from the change of the charge on the dot by one electron. It shows essentially the same features as Fig. 2(a), but is much richer, especially in the regime where the direct dot current is too

here provide robust building blocks in a practical quantum information processor.

In this chapter, we introduce the design and fabrication of etched gate tunable single and double quantum dots in single-layer and bilayer graphene and present several important quantum transport measurements in these systems. A quantum dot with an integrated charge sensor is becoming a common architecture for a spin or charge based solid state qu‐ bit. To implement such a structure in graphene, we have fabricated a twin-dot structure in which the larger QD serves as a single electron transistor (SET) to read out the charge state of the nearby gate controlled small QD. A high SET sensitivity allowed us to probe Coulomb charging as well as excited state spectra of the QD, even in the regime where the current through the QD is too small to be measured by conventional transport means (Wang et al., 2010; Wang et al., 2011b). We also have measured quantum transport properties of gates controlled parallel-coupled double quantum dots (PDQD) and series-coupled double quan‐ tum dots (SDQD) device on both single layer and bilayer graphene (Wang et al., 2011a; Wang et al., 2012). The inter-dot coupling strength can be effectively tuned from weak to strong by in-plane plunger gates. All the relevant energy scales and parameters can be ex‐ tracted from the honeycomb charge stability diagrams. We precisely extract a large inter-dot tunnel coupling strength for the series-coupled quantum dots (SDQD) allowing for the ob‐ servation of tunnel-coupled molecular states extending over the whole double dot. The present method of designing and fabricating graphene QD is demonstrated to be general and reliable and will enhance the realization of graphene nanodevice and desirable study of rich QD physical phenomena in grapheme. These results demonstrate that both single and double quantum dots in single-layer and bilayer graphene bode well for future quantum transport study and quantum computing applications. The clean, highly controllable sys‐ tems serves as an essential building block for quantum devices in a nuclear-spin-free world.

## **2. A graphene quantum dot with a single electron transistor as an integrated charge sensor**

The measurement of individual electrons or its spins in GaAs quantum dots (QDs) has been real‐ ized by so-called charge detection via a nearby quantum point contact (QPC) or single electron transistor (SET) (Lu et al., 2003; Elzerman et al., 2004a). In particular, the combination of high speed and high charge sensitivity has made SET useful in studying a wide range of physical phe‐ nomena such as discrete electron transport (Lu et al., 2003; Bylander et al., 2005; Gotz et al., 2008), qubit read out (Lehnert et al., 2003; Duty et al., 2004; Vijay et al., 2009) and nanomechanical oscil‐ lators (Knobel et al., 2003; Lahaye et al., 2004). So far, most SETs have been using Al/AlOx/Altun‐ nel junctions. However, the graphene SET reported here is technologically simple and reliable, making it an attractive substitute for use in various charge detector applications.

In this section, we realize an all graphene nanocircuit integration with a SET as charge read out for a QD. In conventional semiconductor systems, the gate-defined structure limits the distance be‐ tween the QD and the detector. However, in our device reported here, the QD and the SET in the same material are defined in a single etching step, and the distance between the graphene nano‐ structures is determined by the etched area, which enables optimized coupling and sensing abili‐ ty. The SET is placed in close proximity to the QD giving rise to a strong capacitive coupling between the two systems. Once an additional electron occupies the QD, the potential in the neigh‐ boring SET is modified by capacitive interaction that gives rise to a measurable conductance change. Even if charge transport through the QD is too small to be measured by conventional transport means, the SET charge sensor also allows measurements. These devices demonstrated here provide robust building blocks in a practical quantum information processor.

striking advance on experimental production of graphene single (Ponomarenko et al., 2008; Stampfer et al., 2008a; Stampfer et al., 2008 b; Schenz et al., 2009; Wang et al., 2010; Guttinger et al., 2011) or double quantum dots (Molitor et al., 2009; Molitor et al., 2010; Liu et al., 2010; Wang et al., 2011a; Volk et al., 2011; Wang et al., 2012;) which is an important first step towards such promise.

In this chapter, we introduce the design and fabrication of etched gate tunable single and double quantum dots in single-layer and bilayer graphene and present several important quantum transport measurements in these systems. A quantum dot with an integrated charge sensor is becoming a common architecture for a spin or charge based solid state qu‐ bit. To implement such a structure in graphene, we have fabricated a twin-dot structure in which the larger QD serves as a single electron transistor (SET) to read out the charge state of the nearby gate controlled small QD. A high SET sensitivity allowed us to probe Coulomb charging as well as excited state spectra of the QD, even in the regime where the current through the QD is too small to be measured by conventional transport means (Wang et al., 2010; Wang et al., 2011b). We also have measured quantum transport properties of gates controlled parallel-coupled double quantum dots (PDQD) and series-coupled double quan‐ tum dots (SDQD) device on both single layer and bilayer graphene (Wang et al., 2011a; Wang et al., 2012). The inter-dot coupling strength can be effectively tuned from weak to strong by in-plane plunger gates. All the relevant energy scales and parameters can be ex‐ tracted from the honeycomb charge stability diagrams. We precisely extract a large inter-dot tunnel coupling strength for the series-coupled quantum dots (SDQD) allowing for the ob‐ servation of tunnel-coupled molecular states extending over the whole double dot. The present method of designing and fabricating graphene QD is demonstrated to be general and reliable and will enhance the realization of graphene nanodevice and desirable study of rich QD physical phenomena in grapheme. These results demonstrate that both single and double quantum dots in single-layer and bilayer graphene bode well for future quantum transport study and quantum computing applications. The clean, highly controllable sys‐ tems serves as an essential building block for quantum devices in a nuclear-spin-free world.

**2. A graphene quantum dot with a single electron transistor as an**

making it an attractive substitute for use in various charge detector applications.

The measurement of individual electrons or its spins in GaAs quantum dots (QDs) has been real‐ ized by so-called charge detection via a nearby quantum point contact (QPC) or single electron transistor (SET) (Lu et al., 2003; Elzerman et al., 2004a). In particular, the combination of high speed and high charge sensitivity has made SET useful in studying a wide range of physical phe‐ nomena such as discrete electron transport (Lu et al., 2003; Bylander et al., 2005; Gotz et al., 2008), qubit read out (Lehnert et al., 2003; Duty et al., 2004; Vijay et al., 2009) and nanomechanical oscil‐ lators (Knobel et al., 2003; Lahaye et al., 2004). So far, most SETs have been using Al/AlOx/Altun‐ nel junctions. However, the graphene SET reported here is technologically simple and reliable,

In this section, we realize an all graphene nanocircuit integration with a SET as charge read out for a QD. In conventional semiconductor systems, the gate-defined structure limits the distance be‐

**integrated charge sensor**

162 New Progress on Graphene Research

The graphene flakes were produced by mechanical cleaving of graphite crystallites by Scotch tape and then were transferred to a highly doped Si substrate with a 100 nm SiO2 top layer. Thin flakes were found by optical microscopy, and single layer graphene flakes were selected by the Raman spectroscopy measurement. We used the standard electron beam lith‐ ography and lift off technique to make the Ohmic contact (Ti/Au) on the present graphene devices. Next, a new layer of polymethyl methacrylate is exposed by electron beam to form a designed pattern. Then, the unprotected areas are removed by oxygen reactive ion etching. One of our defined sample structures with a quantum dot and proximity SET is shown in Fig. 1. The quantum dot is an isolated central island of diameter 90 nm, connected by 30nm wide tunneling barriers to source and drain contacts. Here, the Si wafer was used as the back gate and there is also a graphene side gate near the small dot. The SET has a similar pattern while the conducting island has a much larger diameter (180nm). Electronic trans‐ port through both the devices exhibits Coulomb blockade (CB) characteristics with back/side gate voltage. The distance between the CB peaks is determined by the sum of charging and quantum confinement energies, and the former contribution becomes dominant for our de‐ vices with diameter >100nm (Kouwenhoven et al., 1997). Accordingly, we refer to it as a SET rather than a QD. The device was first immersed into a liquid helium storage Dewar at 4.2K to test the functionality of the gates. The experiment was carried out in a top-loading dilu‐ tion refrigerator equipped with filtered wiring and low-noise electronics at the base temper‐ ature of 10 mK. In the measurement, we employed the standard ac lock-in technique.

Fig. 2(a) shows the conductance through the dot Al/AlOx/Al for applied side gate voltage Vsg. Clear CB peaks are observed related to charging of the tunable dot on the graphene. The dashed green lines in the range of 0.2-0.7V for side gate voltages show that the current through the dot be‐ comes too small to be seen clearly. Fig. 2(b) shows the conductance through the SET versus side gate voltage Vsg. The SET is as close as possible to the QD and in this way charging signals of the dot were detected by tracking the change in the SET current. The addition of one electron to the QD leads to a pronounced change of the conductance of the charge detector by typically 30%. The slope of the SET conductance is the steepest at both sides of its CB resonances giving the best charge read-out signal. To offset the large current background, we used a lock-in detection meth‐ od developed earlier for GaAs dot (Elzerman et al., 2004b). A square shaped pulse was superim‐ posed on the dc bias on side gate voltage Vsg. A lock-in detector in sync with the pulse frequency measured the change of SET current due to the pulse modulation. Fig. 2(c) shows a typical trace of the lock-in signal of the transconductance through the SET *dI*SET/*dV*sg. These sharp spikes or dips originate from the change of the charge on the dot by one electron. It shows essentially the same features as Fig. 2(a), but is much richer, especially in the regime where the direct dot current is too small to be seen clearly. The vertical dashed lines in Fig. 2 illustrate the SET sensor signals corre‐ spond to the QD transport measurements perfectly and indicate the SET is reliable. We also note‐ that the individual charge events measurement has been demonstrated in a graphene QD with a QPC detector based on graphene nanoribbon (Güttinger et al., 2008).

**Figure 1.** a) Scanning electron microscope image of the etched sample structure. The bar has a length of 200 nm. The upper small quantum dot as the main device has a diameter of 90 nm while the bottom single electron transistor as charge sensor has a diameter of 180 nm. The bright lines define barriers and the graphene side gate. (b) Schematic of a representative device.

**Figure 2.** a) Conductance through the quantum dot vs the side gate voltage. (b) The example of conductance through the single electron transistor for the same parameter ranges as in panel (a). The steps in conductance have about 30% change of the total signal and are well aligned with the CB in panel (a). (c) Transconductance of the single electron transistor for the same parameters as in panel (a). The spikes and dips indicate the transitions in the charge states by addition of single electron in quantum dot. In particular, the dashed green lines show that the charge detection can allow measurement in the regime where the current through the dot is too small to be seen clearly by direct means.

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The vertical dashed red lines are a guide for the eyes to relate features in these graphs.

small to be seen clearly. The vertical dashed lines in Fig. 2 illustrate the SET sensor signals corre‐ spond to the QD transport measurements perfectly and indicate the SET is reliable. We also note‐ that the individual charge events measurement has been demonstrated in a graphene QD with a

**Figure 1.** a) Scanning electron microscope image of the etched sample structure. The bar has a length of 200 nm. The upper small quantum dot as the main device has a diameter of 90 nm while the bottom single electron transistor as charge sensor has a diameter of 180 nm. The bright lines define barriers and the graphene side gate. (b) Schematic of

a representative device.

QPC detector based on graphene nanoribbon (Güttinger et al., 2008).

164 New Progress on Graphene Research

**Figure 2.** a) Conductance through the quantum dot vs the side gate voltage. (b) The example of conductance through the single electron transistor for the same parameter ranges as in panel (a). The steps in conductance have about 30% change of the total signal and are well aligned with the CB in panel (a). (c) Transconductance of the single electron transistor for the same parameters as in panel (a). The spikes and dips indicate the transitions in the charge states by addition of single electron in quantum dot. In particular, the dashed green lines show that the charge detection can allow measurement in the regime where the current through the dot is too small to be seen clearly by direct means. The vertical dashed red lines are a guide for the eyes to relate features in these graphs.

**Figure 3.** The magnitude of the SET signal *dISET/dVsg* as a function of the modulating pulse frequency. The dashed green line illustrates that the bandwidth of the SET device is about 800 Hz corresponding to a gain of 0.707(-3 dB). Due to the stray capacitances, the response decreases rapidly after 800 Hz.

**Figure 4.** a) Plot of the differential conductance of the quantum dot as a function of the bias voltage and the side gate voltage applied on the dot. From the lines parallel to the edges of Coulomb diamonds, we can identify the excit‐ ed states. (b) Transconductance of the single electron transistor with the same parameters as in panel (a). Perfect matching with panel (a) and resolving more excited states spectra indicate that the single electron transistor can be used as a highly sensitive charge detector. Data in panels (a) and (b) were recorded simultaneously during a single

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sweep. Dashed green lines are the guide for identifying the excited states.

**Figure 4.** a) Plot of the differential conductance of the quantum dot as a function of the bias voltage and the side gate voltage applied on the dot. From the lines parallel to the edges of Coulomb diamonds, we can identify the excit‐ ed states. (b) Transconductance of the single electron transistor with the same parameters as in panel (a). Perfect matching with panel (a) and resolving more excited states spectra indicate that the single electron transistor can be used as a highly sensitive charge detector. Data in panels (a) and (b) were recorded simultaneously during a single sweep. Dashed green lines are the guide for identifying the excited states.

**Figure 3.** The magnitude of the SET signal *dISET/dVsg* as a function of the modulating pulse frequency. The dashed green line illustrates that the bandwidth of the SET device is about 800 Hz corresponding to a gain of 0.707(-3 dB).

Due to the stray capacitances, the response decreases rapidly after 800 Hz.

166 New Progress on Graphene Research

More quantitative information on the system can be obtained from the measurement of the height response of the peak at 0.152 V in Fig. 2(c) as a function of the modulating pulse fre‐ quency on the side gate. The resulting diagram for the SET *dI*SET/*dV*sg gain magnitude is shown in Figure 3.The dashed green line indicates the gain of 0.707 (-3 dB), corresponding approximately to the bandwidth of 800 Hz of the SET device. By applying a signal of 5×10-2 electrons on back gate of the SET and measuring the signal with a signal-to-noise ratio of 1, we achieved a charge sensitivity 10-3*e* / *Hz*of which is similar to that obtained previously in a GaAs QD and superconducting Al SET detector system (Berman et al., 1999). The system can be simply considered as a resistor-capacitor circuit (RC circuit), and the bandwidth is limited by the resistor and capacitance of the cable connecting the SET and the room temper‐ ature equipments. As a result, we would expect the bandwidth can be greatly improved by adding a cold amplifier (Vink et al., 2007). It is also expected that adding a side gate near the SET to independently set the SET operating point to about 25 kΩ can obviously enhance the bandwidth.

**3. Controllable tunnel coupling and molecular states in a graphene**

Previously, the charge stability diagram in coupled quantum-dot systems has been studied by the classical capacitance model (van der Wiel et al., 2003). However the quantum effect should also manifest itself (Yang et al., 2011). In particular, the tunnel coupling *t* between the two dots in a double dot is an important quantity, because it can affect the geometry of the overall charge stability diagram. Furthermore, several different spin qubit operations can be performed by controlling this tunnel rate as a function of time. For approaches based on single electron spin qubit, utilizing t enables the SWAPgate operations between two qu‐ bits (Petta et al., 2005). In an architecture in which each qubit is composed of two-electron single-triplet states, control of t in the presence of a non-uniform magnetic field enables uni‐

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In this Section, we report an experimental demonstration and electrical transport measure‐ ment in a tunable graphene double quantum dot device. Depending on the strength of the inter-dot coupling, the device can form atomic like states on the individual dots (weak tunnel coupling) or molecular like states of the two dots (strong tunnel coupling). We also extract the inter-dot tunnel coupling t by identifying and characterizing the molecule states with wave functions extending over the whole graphene double dot. The result im‐ plies that this artificial grapheme device may be useful for implementing two-electron

**Figure 5.** a) Scanning electron microscope image of the structure of the designed multiple gated sample studied in this work. The double quantum dot have two isolated central islands of diameter 100 nm in series, connected by 20*×*20 nm tunneling barriers to source and drain contacts (S and D) and 30*×*20 nm tunneling barrier with each other. These gates are labeled by G1, GL, GM, GR, G2, in which gate GM, G1 and G2, are used to control the coupling barriers between the dots as well as the leads. Gates GL and GR are used to control and adjust the energy level of each dot. (b)

A scanning electron microscope image of our defined sample structure with double quan‐ tum dot is shown in Fig. 5(a) and Fig. 5(b). The double quantum dot has two isolated central

**double quantum dot**

spin manipulation.

Schematic of a representative device.

versal single qubit rotations (Foletti et al., 2009).

The information contained in the signal goes beyond simple charge counting. For instance, the stability diagram measurement can reveal excited states, which is crucial to get informa‐ tion of the spin state of electrons on a quantum dot (Hanson et al., 2003). Fig. 4(a) shows Coulomb diamonds for the conductance through the dot GQD versus bias voltage Vsd and side gate voltage Vsg. For comparison, Fig. 4(b) shows the transconductance of the SET *dI*SET/*dV*sg as a function of the same parameters. A perfect match between the QD transport measurements and the detector signal is observed. Moreover, the discrete energy spectra of the graphene quantum dot are revealed by the presence of additional lines parallel to the diamond edges. These lines indicate the quantum dot is in the high bias regime where the source-drain bias is high enough that the excited states can participate in electron tunneling (Hanson et al., 2007). The excited states become much more visible in the SET charge detec‐ tor signal than the direct measurement. All of these features have been seen in GaAs QD with QPC (Hanson et al., 2007), but here we achieve the goal with an all graphene nanocir‐ cuit of QD with SET. In the previous reports, the QD and QPC detector are separated by typically 100 nm in width. In the present case, the SET detector is 50 nm from the edge of the QD. Therefore it is expected that the capacitance coupling between QD and SET is enhanced compared to the conventional case realized in semiconductor QD and QPC. This enhanced coupling leads to a larger signal-to-noise ratio of the SET detector signal that can be exploit‐ ed for time resolved charge measurement or charge/spin qubit read out on the QD.

In summary, we have presented a simple fabrication process that produces a quantum dot and highly sensitive single electron transistor charge detector with the same material, gra‐ phene. Typically the addition of a single electron in QD would result in a change in the SET conductance of about 30%. The charging events measured by both the charge detector and direct transport through the dot perfectly match and more excited states information be‐ yond the conventional transport means is also obtained. The devices demonstrated here rep‐ resent a fascinating avenue towards realizing a more complex and highly controllable electronic nanostructure formed from molecular conductors such as graphene.

## **3. Controllable tunnel coupling and molecular states in a graphene double quantum dot**

More quantitative information on the system can be obtained from the measurement of the height response of the peak at 0.152 V in Fig. 2(c) as a function of the modulating pulse fre‐ quency on the side gate. The resulting diagram for the SET *dI*SET/*dV*sg gain magnitude is shown in Figure 3.The dashed green line indicates the gain of 0.707 (-3 dB), corresponding approximately to the bandwidth of 800 Hz of the SET device. By applying a signal of 5×10-2 electrons on back gate of the SET and measuring the signal with a signal-to-noise ratio of 1, we achieved a charge sensitivity 10-3*e* / *Hz*of which is similar to that obtained previously in a GaAs QD and superconducting Al SET detector system (Berman et al., 1999). The system can be simply considered as a resistor-capacitor circuit (RC circuit), and the bandwidth is limited by the resistor and capacitance of the cable connecting the SET and the room temper‐ ature equipments. As a result, we would expect the bandwidth can be greatly improved by adding a cold amplifier (Vink et al., 2007). It is also expected that adding a side gate near the SET to independently set the SET operating point to about 25 kΩ can obviously enhance the

The information contained in the signal goes beyond simple charge counting. For instance, the stability diagram measurement can reveal excited states, which is crucial to get informa‐ tion of the spin state of electrons on a quantum dot (Hanson et al., 2003). Fig. 4(a) shows Coulomb diamonds for the conductance through the dot GQD versus bias voltage Vsd and side gate voltage Vsg. For comparison, Fig. 4(b) shows the transconductance of the SET *dI*SET/*dV*sg as a function of the same parameters. A perfect match between the QD transport measurements and the detector signal is observed. Moreover, the discrete energy spectra of the graphene quantum dot are revealed by the presence of additional lines parallel to the diamond edges. These lines indicate the quantum dot is in the high bias regime where the source-drain bias is high enough that the excited states can participate in electron tunneling (Hanson et al., 2007). The excited states become much more visible in the SET charge detec‐ tor signal than the direct measurement. All of these features have been seen in GaAs QD with QPC (Hanson et al., 2007), but here we achieve the goal with an all graphene nanocir‐ cuit of QD with SET. In the previous reports, the QD and QPC detector are separated by typically 100 nm in width. In the present case, the SET detector is 50 nm from the edge of the QD. Therefore it is expected that the capacitance coupling between QD and SET is enhanced compared to the conventional case realized in semiconductor QD and QPC. This enhanced coupling leads to a larger signal-to-noise ratio of the SET detector signal that can be exploit‐

ed for time resolved charge measurement or charge/spin qubit read out on the QD.

electronic nanostructure formed from molecular conductors such as graphene.

In summary, we have presented a simple fabrication process that produces a quantum dot and highly sensitive single electron transistor charge detector with the same material, gra‐ phene. Typically the addition of a single electron in QD would result in a change in the SET conductance of about 30%. The charging events measured by both the charge detector and direct transport through the dot perfectly match and more excited states information be‐ yond the conventional transport means is also obtained. The devices demonstrated here rep‐ resent a fascinating avenue towards realizing a more complex and highly controllable

bandwidth.

168 New Progress on Graphene Research

Previously, the charge stability diagram in coupled quantum-dot systems has been studied by the classical capacitance model (van der Wiel et al., 2003). However the quantum effect should also manifest itself (Yang et al., 2011). In particular, the tunnel coupling *t* between the two dots in a double dot is an important quantity, because it can affect the geometry of the overall charge stability diagram. Furthermore, several different spin qubit operations can be performed by controlling this tunnel rate as a function of time. For approaches based on single electron spin qubit, utilizing t enables the SWAPgate operations between two qu‐ bits (Petta et al., 2005). In an architecture in which each qubit is composed of two-electron single-triplet states, control of t in the presence of a non-uniform magnetic field enables uni‐ versal single qubit rotations (Foletti et al., 2009).

In this Section, we report an experimental demonstration and electrical transport measure‐ ment in a tunable graphene double quantum dot device. Depending on the strength of the inter-dot coupling, the device can form atomic like states on the individual dots (weak tunnel coupling) or molecular like states of the two dots (strong tunnel coupling). We also extract the inter-dot tunnel coupling t by identifying and characterizing the molecule states with wave functions extending over the whole graphene double dot. The result im‐ plies that this artificial grapheme device may be useful for implementing two-electron spin manipulation.

**Figure 5.** a) Scanning electron microscope image of the structure of the designed multiple gated sample studied in this work. The double quantum dot have two isolated central islands of diameter 100 nm in series, connected by 20*×*20 nm tunneling barriers to source and drain contacts (S and D) and 30*×*20 nm tunneling barrier with each other. These gates are labeled by G1, GL, GM, GR, G2, in which gate GM, G1 and G2, are used to control the coupling barriers between the dots as well as the leads. Gates GL and GR are used to control and adjust the energy level of each dot. (b) Schematic of a representative device.

A scanning electron microscope image of our defined sample structure with double quan‐ tum dot is shown in Fig. 5(a) and Fig. 5(b). The double quantum dot has two isolated central island of diameter 100 nm in series, connected by 20× 20 nm narrow constriction to source and drain contacts (S and D electrodes) and 30× 20 nm narrow constriction with each other. These constrictions are expected to act as tunnel barriers due to the quantum size effect. In addition, the highly P-doped Si substrate is used as a back gate and five lateral side gates, labeled the left gate G1, right gate G2, center gate GM and GL(R), which are expected for local control. All of side gates are effective, in which gates GL, GR and G2 have very good effect on two dots and middle barrier, while gates G1 and GM have weak effect on those. The device was first immersed into a liquid helium storage dewar at 4.2K to test the func‐ tionality of the gates. The experiment was carried out in a He3 cryostat equipped with fil‐ tered wiring and low-noise electronics at the base temperature of 300mK. In the measurement, we employed the standard AC lock-in technique with an excitation voltage 20 *μ*Vat 11.3 Hz.

Vsd= 20*μ*V, VG1 = 0V, VGM = 0V, VG2 = 0V and Vbg = 2.5 V. The honeycomb pattern is clearly visible and uniforms over many times. Each cell of the honeycomb corresponds to a welldefined charge configuration (NL,NR) in the nearly independent dots, where NL and NR denote the number of electrons on the left and right dot, respectively. The conductance is large at the vertices, where the electrochemical potentials in both dots are aligned with each other and the Fermi energy in the leads and resonant sequential tunneling is available. These vertices are connected by faint lines of much smaller conductance along the edges of the honeycomb cells. At these lines, the energy level in one dot is aligned with the electro‐ chemical potential in the corresponding lead and inelastic cotunneling processes occur. The observed honeycomb pattern resembles the charge stability diagram found for weakly cou‐ pled GaAs double quantum dot (van der Wiel et al., 2003). Such similarities indicate that graphene quantum dot devices will continue to share features with well-studied semicon‐ ductor quantum dot systems. The energy-level statistics of single graphene quantum dot was probed and shown to agree well with the theory of chaotic Dirac billiards (Ponomaren‐ ko et al., 2008). It is interesting and important to know whether these Dirac fermions' behav‐ iors can be realized and observed in grapheme double quantum dot. Nevertheless, it will be

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More quantitative information such as double dot capacitances can be extracted using a elec‐ trostatic model as shown in Fig. 6(b) (van der Wiel et al., 2003). First, the capacitance of the dot to the side gate can be determined from measuring the size of the honeycomb in Fig. 6(c) as *CGL* =*e* / *ΔVGL* ≈1.27aF and*C*GR =*e* / *ΔV*GR ≈1.49aF. Next, the capacitance ratios can be de‐ termined from measuring the size of the vertices in Fig. 6(d) at finite bias *Vsd* =900*μ*V as *α<sup>L</sup>* = |*Vsd* | / *δVGL* =0.029 and*α<sup>R</sup>* = |*Vsd* | / *δVGR* =0.035. Using the relation *CGL* / *CL* =*α<sup>L</sup>* and *CGR* / *CR* =*αR*, we can obtain the typical values of dot capacitances as *CL* =44.8aFand *CR* =44.1aF, respectively. The amount of interdot coupling can be achieved by measuring the vertices splitting in Fig. 6(c). Assuming the capacitively coupling is dominant in the weakly coupled dots regime (van der Wiel et al., 2003; Mason et al., 2004), the mutual capacitance

It has been expected that opening the interdot constriction by gate voltage will cause the tunnel coupling to increase exponentially faster than the capacitive coupling (Kouwenhoven et al., 1997). Fig. 7(a)-(c) represent a selection of such measurements by holding the same VGR and Vbg and scanning different ranges of VGL between -0.5 V to 0.35 V. An evolution of con‐ ductance pattern indicates that the stability diagram changes from weak to strong tunneling regimes (van der Wiel et al., 2003; Mason et al., 2004). The conductance near the vertices de‐ pends on the relative contributions of the capacitive coupling and tunnel coupling. For the former, the vertices become a sharpened point, while for the latter, the vertices become blur‐ red along the edges of the honeycomb cell (Graber et al., 2007). In Fig. 7(b), the vertices is not obvious as those in Fig. 7(a), which indicates a stronger tunnel coupling. The results suggest that two graphene dots are interacting with each other through the large quantum mechani‐ cal tunnel coupling, which is analogous to covalent bonding. We will analyze it in details

studied in the future work.

between dots is calculated as

*<sup>m</sup> CGL CR* / *<sup>e</sup>* <sup>=</sup>*ΔVGR*

*<sup>m</sup> CGRCL* / *<sup>e</sup>* =9.2aF

*CM* =*ΔVGL*

**Figure 6.** a) Color scale plot of the differential conductance versus voltage applied on gate GL (VGL) and gate GR (VGR) at Vsd= 20μV, VG1 = 0V, VGM = 0V, VG2 = 0V and Vbg = 2.5 V. The honeycomb pattern we got stands for the typical charge stability diagram of coupled double quantum dots. (b) Pure capacitance model of a graphene double dot system. Zoom in of a honeycomb structure (c) and a vertex pair (d) at Vsd = 900μV.

Fig. 6(a) displays the differential conductance through the graphene double quantum dot circuit as a function of gate voltages VGL and VGR. Here the measurement was recorded at Vsd= 20*μ*V, VG1 = 0V, VGM = 0V, VG2 = 0V and Vbg = 2.5 V. The honeycomb pattern is clearly visible and uniforms over many times. Each cell of the honeycomb corresponds to a welldefined charge configuration (NL,NR) in the nearly independent dots, where NL and NR denote the number of electrons on the left and right dot, respectively. The conductance is large at the vertices, where the electrochemical potentials in both dots are aligned with each other and the Fermi energy in the leads and resonant sequential tunneling is available. These vertices are connected by faint lines of much smaller conductance along the edges of the honeycomb cells. At these lines, the energy level in one dot is aligned with the electro‐ chemical potential in the corresponding lead and inelastic cotunneling processes occur. The observed honeycomb pattern resembles the charge stability diagram found for weakly cou‐ pled GaAs double quantum dot (van der Wiel et al., 2003). Such similarities indicate that graphene quantum dot devices will continue to share features with well-studied semicon‐ ductor quantum dot systems. The energy-level statistics of single graphene quantum dot was probed and shown to agree well with the theory of chaotic Dirac billiards (Ponomaren‐ ko et al., 2008). It is interesting and important to know whether these Dirac fermions' behav‐ iors can be realized and observed in grapheme double quantum dot. Nevertheless, it will be studied in the future work.

More quantitative information such as double dot capacitances can be extracted using a elec‐ trostatic model as shown in Fig. 6(b) (van der Wiel et al., 2003). First, the capacitance of the dot to the side gate can be determined from measuring the size of the honeycomb in Fig. 6(c) as *CGL* =*e* / *ΔVGL* ≈1.27aF and*C*GR =*e* / *ΔV*GR ≈1.49aF. Next, the capacitance ratios can be de‐ termined from measuring the size of the vertices in Fig. 6(d) at finite bias *Vsd* =900*μ*V as *α<sup>L</sup>* = |*Vsd* | / *δVGL* =0.029 and*α<sup>R</sup>* = |*Vsd* | / *δVGR* =0.035. Using the relation *CGL* / *CL* =*α<sup>L</sup>* and *CGR* / *CR* =*αR*, we can obtain the typical values of dot capacitances as *CL* =44.8aFand *CR* =44.1aF, respectively. The amount of interdot coupling can be achieved by measuring the vertices splitting in Fig. 6(c). Assuming the capacitively coupling is dominant in the weakly coupled dots regime (van der Wiel et al., 2003; Mason et al., 2004), the mutual capacitance between dots is calculated as

$$\mathbf{C}\_{M} = \Delta V\_{GL}^{\mathfrak{m}} \mathbf{C}\_{GL}^{\mathfrak{m}} \mathbf{C}\_{R} \left/ e \right. = \Delta V\_{GR}^{\mathfrak{m}} \mathbf{C}\_{GR} \mathbf{C}\_{L} \left/ e \right. = \mathbf{9.2aF}$$

island of diameter 100 nm in series, connected by 20× 20 nm narrow constriction to source and drain contacts (S and D electrodes) and 30× 20 nm narrow constriction with each other. These constrictions are expected to act as tunnel barriers due to the quantum size effect. In addition, the highly P-doped Si substrate is used as a back gate and five lateral side gates, labeled the left gate G1, right gate G2, center gate GM and GL(R), which are expected for local control. All of side gates are effective, in which gates GL, GR and G2 have very good effect on two dots and middle barrier, while gates G1 and GM have weak effect on those. The device was first immersed into a liquid helium storage dewar at 4.2K to test the func‐ tionality of the gates. The experiment was carried out in a He3 cryostat equipped with fil‐ tered wiring and low-noise electronics at the base temperature of 300mK. In the measurement, we employed the standard AC lock-in technique with an excitation voltage 20

**Figure 6.** a) Color scale plot of the differential conductance versus voltage applied on gate GL (VGL) and gate GR (VGR) at Vsd= 20μV, VG1 = 0V, VGM = 0V, VG2 = 0V and Vbg = 2.5 V. The honeycomb pattern we got stands for the typical charge stability diagram of coupled double quantum dots. (b) Pure capacitance model of a graphene double dot system.

Fig. 6(a) displays the differential conductance through the graphene double quantum dot circuit as a function of gate voltages VGL and VGR. Here the measurement was recorded at

Zoom in of a honeycomb structure (c) and a vertex pair (d) at Vsd = 900μV.

*μ*Vat 11.3 Hz.

170 New Progress on Graphene Research

It has been expected that opening the interdot constriction by gate voltage will cause the tunnel coupling to increase exponentially faster than the capacitive coupling (Kouwenhoven et al., 1997). Fig. 7(a)-(c) represent a selection of such measurements by holding the same VGR and Vbg and scanning different ranges of VGL between -0.5 V to 0.35 V. An evolution of con‐ ductance pattern indicates that the stability diagram changes from weak to strong tunneling regimes (van der Wiel et al., 2003; Mason et al., 2004). The conductance near the vertices de‐ pends on the relative contributions of the capacitive coupling and tunnel coupling. For the former, the vertices become a sharpened point, while for the latter, the vertices become blur‐ red along the edges of the honeycomb cell (Graber et al., 2007). In Fig. 7(b), the vertices is not obvious as those in Fig. 7(a), which indicates a stronger tunnel coupling. The results suggest that two graphene dots are interacting with each other through the large quantum mechani‐ cal tunnel coupling, which is analogous to covalent bonding. We will analyze it in details below. An increase in inter-dot coupling also leads to much larger separation of vertices in Fig. 7(b) (Mason et al., 2004), and finally, to a smearing of honeycomb features in Fig. 7(c). In this case, the double dots behave like a single dot, as illustrated in Fig. 7(g). We note that a similar evolution is observed for four different values of Vbg from 2.5 V to 2.0 V at the same VGL and VGR regimes as shown in Fig. 7(d)-(f). Thus the inter-dot tunnel coupling could also be changed by VGL or Vbg. This can be explained by the fact that the side gates and back gate may influence the central barrier through the existing capacitances between the gates and the central barrier.

with tunnel couplings which offers us a method to measure the contribution of the interdot tunneling to the splitting of the vertex. In our double-dot sample, a clear evolution of *f* is obtained through scanning different regimes of VGL with fixed VGR (Fig. 7(a)-(c)). Through extracting *ΔVS* and*ΔVP*, we get *f* =0.5 for (a) and *f* =0.65 for (b) and *f* =1 for (c) respective‐ ly. These values indicate that control of tunnel coupling as a function of such a gate voltage

Having understood the qualitative behavior of the graphene device in the strong coupling regime, we extract the quantitative properties based on a quantum model of graphene artifi‐ cial molecule states (Yang et al., 2003; Graber et al., 2007; Hatano et al., 2005). Here we only take into account the topmost occupied state in each dot and treat the other electrons as an inert core (van der Wiel et al., 2003; Golovach et al., 2004). In the case of neglected tunnel coupling, the nonzero conductance can only occur right at the vertices which are energy de‐ generate points as *E*(*NL +* 1*,NR*) *= E*(*NL, NR +* 1). When an electron can tunnel coherently be‐ tween the two dots, the eigenstates of the double dot system become the superposed states

> 2 2 sin 1, cos , 1 2 2 *i i <sup>B</sup> L R L R e N N e NN*

2 2 cos 1, sin , 1 2 2 *i i <sup>A</sup> L R L R e N N e NN*


Provided that the graphene double-dot molecule eigenstate |*ψ* participates in the transport process, sequential tunneling is also possible along the honeycomb edges. In Fig. 8(a) and Fig. 8(b), a colorscale plot of the differential conductance is shown at *V*sd = 20 *μ*Vin the vicin‐ ity of a vertex. As expected the visible conductance is observed at both the position of the vertex and the honeycomb edges extending from the vertex. Fig. 8(c) shows a fit of the ener‐ gy difference*EΔ*from the measured mount of splitting of the positions of the differential con‐ ductance resonance peak in the *ε*-direction. Here we use *ε*=*EL* − *ER* =*eα<sup>L</sup> VGL* −*eαRVGR* to

2 2 *E t* U (2 ) e

 j

 j

*<sup>ε</sup>* ), *ε*=*EL* − *ER*, *EL* and*ER*are the energies of state | *NL* + 1, *NR* and

<sup>2</sup> is the contribution from electrostatic coupling between dots (Ziegler et

=- + + + (1)

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= ++ + (2)

<sup>D</sup> = ¢+ + (3)

 q

 q

j

j

q

q



is conceivable.

Where*θ* =arctan(

pressed by

Here U′ <sup>=</sup> <sup>2</sup>*<sup>e</sup>* <sup>2</sup>

al., 2000).

of two well-separated dot states with the form

y

y

2*t*

*Cm CL CR* − *Cm*

**Figure 7.** a)-(c) Colorscale plot of the differential conductance versus voltage applied on gate GL (VGL) and gate GR (VGR) at Vbg = 2*.*5 V for different VGL regimes. (d)-(f) Color scale plot of the differential conductance versus voltage ap‐ plied on gate L (VGL) and gate R(VGR) for different back gate voltage Vbg. The trend of interdot tunnel coupling chang‐ ing from weak to strong can be seen clearly. (g) Sketches of the characteristic electronic configurations with interdot tunnel coupling *t*.

Similar to the definitions in Ref. (Livermore et al., 1996), we define *f* =2*ΔVS* / *ΔVP*with*ΔVS* representing the splitting between vertices in the diagonal direction and *ΔVP* the vertex pairs distance (Fig. 7(e)). Thus, the case *f* =1 stands for strong coupling limit where the dou‐ ble dots behave like a single dot, while the case *f* =0 represents weak coupling limit where the double dots behave like two isolated dots. This way, f should have a certain relationship with tunnel couplings which offers us a method to measure the contribution of the interdot tunneling to the splitting of the vertex. In our double-dot sample, a clear evolution of *f* is obtained through scanning different regimes of VGL with fixed VGR (Fig. 7(a)-(c)). Through extracting *ΔVS* and*ΔVP*, we get *f* =0.5 for (a) and *f* =0.65 for (b) and *f* =1 for (c) respective‐ ly. These values indicate that control of tunnel coupling as a function of such a gate voltage is conceivable.

below. An increase in inter-dot coupling also leads to much larger separation of vertices in Fig. 7(b) (Mason et al., 2004), and finally, to a smearing of honeycomb features in Fig. 7(c). In this case, the double dots behave like a single dot, as illustrated in Fig. 7(g). We note that a similar evolution is observed for four different values of Vbg from 2.5 V to 2.0 V at the same VGL and VGR regimes as shown in Fig. 7(d)-(f). Thus the inter-dot tunnel coupling could also be changed by VGL or Vbg. This can be explained by the fact that the side gates and back gate may influence the central barrier through the existing capacitances between the gates and

**Figure 7.** a)-(c) Colorscale plot of the differential conductance versus voltage applied on gate GL (VGL) and gate GR (VGR) at Vbg = 2*.*5 V for different VGL regimes. (d)-(f) Color scale plot of the differential conductance versus voltage ap‐ plied on gate L (VGL) and gate R(VGR) for different back gate voltage Vbg. The trend of interdot tunnel coupling chang‐ ing from weak to strong can be seen clearly. (g) Sketches of the characteristic electronic configurations with interdot

Similar to the definitions in Ref. (Livermore et al., 1996), we define *f* =2*ΔVS* / *ΔVP*with*ΔVS* representing the splitting between vertices in the diagonal direction and *ΔVP* the vertex pairs distance (Fig. 7(e)). Thus, the case *f* =1 stands for strong coupling limit where the dou‐ ble dots behave like a single dot, while the case *f* =0 represents weak coupling limit where the double dots behave like two isolated dots. This way, f should have a certain relationship

the central barrier.

172 New Progress on Graphene Research

tunnel coupling *t*.

Having understood the qualitative behavior of the graphene device in the strong coupling regime, we extract the quantitative properties based on a quantum model of graphene artifi‐ cial molecule states (Yang et al., 2003; Graber et al., 2007; Hatano et al., 2005). Here we only take into account the topmost occupied state in each dot and treat the other electrons as an inert core (van der Wiel et al., 2003; Golovach et al., 2004). In the case of neglected tunnel coupling, the nonzero conductance can only occur right at the vertices which are energy de‐ generate points as *E*(*NL +* 1*,NR*) *= E*(*NL, NR +* 1). When an electron can tunnel coherently be‐ tween the two dots, the eigenstates of the double dot system become the superposed states of two well-separated dot states with the form

$$\left| \left| \psi\_{B} \right> \right> = -\sin\frac{\theta}{2}\varepsilon^{-\frac{i\rho}{2}} \left| N\_{L} + 1, N\_{R} \right> + \cos\frac{\theta}{2}\varepsilon^{\frac{i\rho}{2}} \left| N\_{L'}, N\_{R} + 1 \right> \tag{1}$$

$$\left| \left| \nu\_{A} \right> \right> = \cos \frac{\theta}{2} \varepsilon^{-\frac{i\phi}{2}} \left| N\_{L} + 1\_{r} N\_{R} \right> + \sin \frac{\theta}{2} \varepsilon^{\frac{i\phi}{2}} \left| N\_{L'} N\_{R} + 1 \right> \tag{2}$$

Where*θ* =arctan( 2*t <sup>ε</sup>* ), *ε*=*EL* − *ER*, *EL* and*ER*are the energies of state | *NL* + 1, *NR* and | *NL* , *NR* + 1 , respectively. Thus |*ψB* and |*ψA* are the bonding and anti-bonding state in terms of the uncoupled dot, and the energy difference between these two states can be ex‐ pressed by

$$E\_{\Lambda} = \mathbb{U}^{r} + \sqrt{\varepsilon^{2} + (2t^{2})} \tag{3}$$

Here U′ <sup>=</sup> <sup>2</sup>*<sup>e</sup>* <sup>2</sup> *Cm CL CR* − *Cm* <sup>2</sup> is the contribution from electrostatic coupling between dots (Ziegler et al., 2000).

Provided that the graphene double-dot molecule eigenstate |*ψ* participates in the transport process, sequential tunneling is also possible along the honeycomb edges. In Fig. 8(a) and Fig. 8(b), a colorscale plot of the differential conductance is shown at *V*sd = 20 *μ*Vin the vicin‐ ity of a vertex. As expected the visible conductance is observed at both the position of the vertex and the honeycomb edges extending from the vertex. Fig. 8(c) shows a fit of the ener‐ gy difference*EΔ*from the measured mount of splitting of the positions of the differential con‐ ductance resonance peak in the *ε*-direction. Here we use *ε*=*EL* − *ER* =*eα<sup>L</sup> VGL* −*eαRVGR* to translate the gate voltage detuning *VGL* −*VGR* with the conversion factors *α<sup>L</sup>* and *αR*deter‐ mined above. The fitting with Eq. (3) yields the values of tunnel coupling strength *t* ≈727*μ*eVandU′ ≈209*μ*eV. Similar measurements have been performed in a carbon nano‐ tube double dots with *t* ≈358*μ*eV and U′ ≈16*μ*eV (Graber et al., 2007) and semiconductor double dots with *t* ≈80*μ*eV and U′ ≈175*μ*eV (Hatano et al., 2005). The fact that the tunnel coupling t is dominant than capacitive coupling U′implies the inter-dot tunnel barrier in the etched grapheme double dot is much more transparent than those gated carbon nanotube or semiconductor double dot.

(*μ*s) (Fischer et al., 2009). The results indicate the ability to carry out two-electron spin oper‐ ations in nanosecond timescales on a graphene device, four times faster than perviously

In summary, we have measured a graphene double quantum dot with multiple lectrostatic gates and observed the transport pattern evolution in different gate configurations. This way offers us a method to identify the molecular states as a quantum-mechanical superposi‐ tion of double dot and measure the contribution of the interdot tunneling to the splitting of the differential conductance vertex. The precisely extracted values of inter-dot tunnel cou‐ pling t for this system is much larger than those in previously reported semiconductor de‐ vice. These short operation times due to large tunneling strength together with the predicted very long coherence times suggest that the requirements for implementing quantum infor‐

**4. Gates controlled parallel-coupled double quantum dot on both single**

In contrast to DQD in series, where the applied current passes through the double dot in se‐ rial, the parallel-coupled double quantum dot (PDQD) requires two sets of entrances and ex‐ its, one for each dot. In addition, the source and drain must maintain coherence of the electron waves through both dots, in a manner analogous to a Young's double slit. Thus PDQD is an ideal artificial system for investigating the interaction and interference. Rich physical phenomena, such as Aharonov- Bohm (AB) effect, Kondo regimes and Fano effect, have been predicted to be observed in parallel DQD (Holleitner et al., 2001; Lo´pez et al., 2002; Ladro´n de Guevara et al., 2003; Orellana et al., 2004; Chen et al., 2004). Particularly excitement is the prospect of accessing theoretically predicted quantum critical points in quantum phase transitions (Dias da Silva et al., 2008). The grapheme PDQD is an attractive system for investigating the quantum phase transitions due to its intrinsically large energy separation between on-dot quantum levels, thus offering a significant advantage over con‐

In this section, we present the design, fabrication, and quantum transport measurement of double dot structure coupled in parallel, on both bilayer and single layer grapheme flakes, which may open a door to study the rich PDQD physical phenomena in this material the parallel graphene structure can be tuned from a strong-coupling resulted artificial molecule state to a weak-coupling resulted two-dot state by adjusting in plane plunger gates. The tun‐ ing is found to be very reliable and reproducible, with good long-term stability on the order

Graphene flakes are produced by mechanical cleaving of bulk graphite crystallites by Scotch tape (Novoselov et al., 2004). For this kind of exfoliated graphene flakes on SiO2

heavily doped Si substrate with 100 nm thick SiO2 on top, we can identify monolayer, bi‐ layer, and few layer graphenes through optical microscope. Monolayer and bilayer gra‐

/(Vs) (Geim et al., 2007). By using

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shown for semiconductor double dot.

**layer and bilayer grapheme**

of days.

mation processing in graphene nanodevice are within reach.

ventional systems as GaAs or silicon based quantum dots.

substrate, the mobility is normally about 15000 cm2

**Figure 8.** a) Colorscale plot of the differential conductance versus the energies of each dot*EL* and *ER* at Vsd = 20 μV near the selected two vertices with dashed lines as guides to the eye. (b) Schematic of a single anticrossing and the evolution from the state localized in each dot to a molecule state extending across both dots (Hatano et al., 2005). (c) *E*Δdependence of the detuning ε = *EL* − *ER E*Δ(circles) is measured from the separation of the two high conductance wings in Fig. 4(a). The line illustrates a fit of the data to Eq. (3).

Finally, we discuss the relevance of graphene double dot device for implementing a quan‐ tum gate and quantum entanglement of coupled electron spins. A SWAP operation has al‐ ready been demonstrated in a semiconductor double dot system using the fast control of exchange coupling *J*(Petta et al., 2005). The operation time*τ*is about 180 ps for *J* ≈0.4meV corresponding to*t* ≈0.16meV. In the present graphene device, we have obtained much larger *t* ≈0.72meV and the estimated *τ* ≈50ps is much shorter than the predicted decoherence time (*μ*s) (Fischer et al., 2009). The results indicate the ability to carry out two-electron spin oper‐ ations in nanosecond timescales on a graphene device, four times faster than perviously shown for semiconductor double dot.

translate the gate voltage detuning *VGL* −*VGR* with the conversion factors *α<sup>L</sup>* and *αR*deter‐ mined above. The fitting with Eq. (3) yields the values of tunnel coupling strength *t* ≈727*μ*eVandU′ ≈209*μ*eV. Similar measurements have been performed in a carbon nano‐ tube double dots with *t* ≈358*μ*eV and U′ ≈16*μ*eV (Graber et al., 2007) and semiconductor double dots with *t* ≈80*μ*eV and U′ ≈175*μ*eV (Hatano et al., 2005). The fact that the tunnel coupling t is dominant than capacitive coupling U′implies the inter-dot tunnel barrier in the etched grapheme double dot is much more transparent than those gated carbon nanotube or

**Figure 8.** a) Colorscale plot of the differential conductance versus the energies of each dot*EL* and *ER* at Vsd = 20 μV near the selected two vertices with dashed lines as guides to the eye. (b) Schematic of a single anticrossing and the evolution from the state localized in each dot to a molecule state extending across both dots (Hatano et al., 2005). (c) *E*Δdependence of the detuning ε = *EL* − *ER E*Δ(circles) is measured from the separation of the two high conductance

Finally, we discuss the relevance of graphene double dot device for implementing a quan‐ tum gate and quantum entanglement of coupled electron spins. A SWAP operation has al‐ ready been demonstrated in a semiconductor double dot system using the fast control of exchange coupling *J*(Petta et al., 2005). The operation time*τ*is about 180 ps for *J* ≈0.4meV corresponding to*t* ≈0.16meV. In the present graphene device, we have obtained much larger *t* ≈0.72meV and the estimated *τ* ≈50ps is much shorter than the predicted decoherence time

wings in Fig. 4(a). The line illustrates a fit of the data to Eq. (3).

semiconductor double dot.

174 New Progress on Graphene Research

In summary, we have measured a graphene double quantum dot with multiple lectrostatic gates and observed the transport pattern evolution in different gate configurations. This way offers us a method to identify the molecular states as a quantum-mechanical superposi‐ tion of double dot and measure the contribution of the interdot tunneling to the splitting of the differential conductance vertex. The precisely extracted values of inter-dot tunnel cou‐ pling t for this system is much larger than those in previously reported semiconductor de‐ vice. These short operation times due to large tunneling strength together with the predicted very long coherence times suggest that the requirements for implementing quantum infor‐ mation processing in graphene nanodevice are within reach.

## **4. Gates controlled parallel-coupled double quantum dot on both single layer and bilayer grapheme**

In contrast to DQD in series, where the applied current passes through the double dot in se‐ rial, the parallel-coupled double quantum dot (PDQD) requires two sets of entrances and ex‐ its, one for each dot. In addition, the source and drain must maintain coherence of the electron waves through both dots, in a manner analogous to a Young's double slit. Thus PDQD is an ideal artificial system for investigating the interaction and interference. Rich physical phenomena, such as Aharonov- Bohm (AB) effect, Kondo regimes and Fano effect, have been predicted to be observed in parallel DQD (Holleitner et al., 2001; Lo´pez et al., 2002; Ladro´n de Guevara et al., 2003; Orellana et al., 2004; Chen et al., 2004). Particularly excitement is the prospect of accessing theoretically predicted quantum critical points in quantum phase transitions (Dias da Silva et al., 2008). The grapheme PDQD is an attractive system for investigating the quantum phase transitions due to its intrinsically large energy separation between on-dot quantum levels, thus offering a significant advantage over con‐ ventional systems as GaAs or silicon based quantum dots.

In this section, we present the design, fabrication, and quantum transport measurement of double dot structure coupled in parallel, on both bilayer and single layer grapheme flakes, which may open a door to study the rich PDQD physical phenomena in this material the parallel graphene structure can be tuned from a strong-coupling resulted artificial molecule state to a weak-coupling resulted two-dot state by adjusting in plane plunger gates. The tun‐ ing is found to be very reliable and reproducible, with good long-term stability on the order of days.

Graphene flakes are produced by mechanical cleaving of bulk graphite crystallites by Scotch tape (Novoselov et al., 2004). For this kind of exfoliated graphene flakes on SiO2 substrate, the mobility is normally about 15000 cm2 /(Vs) (Geim et al., 2007). By using heavily doped Si substrate with 100 nm thick SiO2 on top, we can identify monolayer, bi‐ layer, and few layer graphenes through optical microscope. Monolayer and bilayer gra‐ phenes were further checked by Raman spectrum. Firstly, graphene flakes are transferred to the substrate with gold markers. Then, a layer of 50nm thick polymethyl methacrylate (PMMA) is spun on the substrate for electron beam lithography (EBL) to form a designed pattern. After that, O2/Ar (50:50) plasma is used to remove unprotected parts of graphene. Next, an area of over exposed PMMA is used to separate a bridge plunger gate from the drain part of graphene (Chen et al., 2004; Huard et al., 2007). The final step is to make the metal contacts, which are defined by the standardized EBL process, followed by the Ebeam evaporation of Ti/Au (2 nm/50 nm).

n-type heavily doped silicon substrate is used as a global back gate. The bridge plunger gate GM is separated from the drain part of graphene by a layer of over exposed PMMA. All the devices were primarily tested to check the functionality of all the gates in a liquid helium storage dewar at 4.2 K. Then the samples were mounted on a dilution refrigerator equipped with filtering wirings and low-noise electronics at the base temperature of 10 mK. To main‐

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**Figure 10.** Color online) (a), (b), and (c) PDQD differential conductance as a function of plunger gate voltage VGL and VGR. The red dash lines are guides to the eyes showing the honeycomb pattern. (N,M) represents the carriers in the left and right dot, respectively. (b) Zoom-in of the area (N,M) of the honeycomb pattern. (c) Zoom-in of a vertex pair with white dash lines. (d) Capacitance model for the analysis of the double dot system. Graphene nanoconstrictions behave as tunneling barriers, which are presented, for example, as RSL, CSL (a capacitance and a resistance coupled in paral‐

lel). Gate GL and GR are capacitively coupled to the dots; CGL and CGR represent the capacitance.

tain consistency, we will use the data from one sample only in the following.

**Figure 9.** Color online) (a) Scanning electron microscope image of the etched parallel coupled graphene double dot sample structure. The bar has a length of 500 nm. The diameters of the two dots are both 100 nm, constriction be‐ tween the two dots is 35 nm in width and length. The four narrow parts connecting the dot to source and drain parts have a width of 30 nm. Seven in-plane plunger gates labeled as GL, GR, GM, PSL, PDL, PSR, and PDR are integrated around the dot for fine tuning. (b) Schematic picture of the device. N-type heavily doped silicon substrate is used as a global back gate. A layer of overexposed PMMA is used as a bridge to make gate GM separated from the drain part of graphene.

Fig. 9(a) shows a scanning electron microscope (SEM) image of one sample with the same structure as the bilayer device we measured. Two central islands with diameter of 100 nm connect through 30 nm wide narrow constrictions to the source and the drain regions. An‐ other narrow constriction (35nm in both width and length) connects the two central islands. Seven in-plane plunger gates labeled as GL, GR, GM, PSL, PDL, PSR, and PDR are integrat‐ ed in close proximity to the dots. GL, GR, and GM are, respectively, designed to adjust the energy level of left dot, right dot, and inter-dot coupling strength. And PSL, PDL (PSR, PDR) are used for the tuning of the coupling of the left (right) dot to source and drain. The n-type heavily doped silicon substrate is used as a global back gate. The bridge plunger gate GM is separated from the drain part of graphene by a layer of over exposed PMMA. All the devices were primarily tested to check the functionality of all the gates in a liquid helium storage dewar at 4.2 K. Then the samples were mounted on a dilution refrigerator equipped with filtering wirings and low-noise electronics at the base temperature of 10 mK. To main‐ tain consistency, we will use the data from one sample only in the following.

phenes were further checked by Raman spectrum. Firstly, graphene flakes are transferred to the substrate with gold markers. Then, a layer of 50nm thick polymethyl methacrylate (PMMA) is spun on the substrate for electron beam lithography (EBL) to form a designed pattern. After that, O2/Ar (50:50) plasma is used to remove unprotected parts of graphene. Next, an area of over exposed PMMA is used to separate a bridge plunger gate from the drain part of graphene (Chen et al., 2004; Huard et al., 2007). The final step is to make the metal contacts, which are defined by the standardized EBL process, followed by the E-

**Figure 9.** Color online) (a) Scanning electron microscope image of the etched parallel coupled graphene double dot sample structure. The bar has a length of 500 nm. The diameters of the two dots are both 100 nm, constriction be‐ tween the two dots is 35 nm in width and length. The four narrow parts connecting the dot to source and drain parts have a width of 30 nm. Seven in-plane plunger gates labeled as GL, GR, GM, PSL, PDL, PSR, and PDR are integrated around the dot for fine tuning. (b) Schematic picture of the device. N-type heavily doped silicon substrate is used as a global back gate. A layer of overexposed PMMA is used as a bridge to make gate GM separated from the drain part of

Fig. 9(a) shows a scanning electron microscope (SEM) image of one sample with the same structure as the bilayer device we measured. Two central islands with diameter of 100 nm connect through 30 nm wide narrow constrictions to the source and the drain regions. An‐ other narrow constriction (35nm in both width and length) connects the two central islands. Seven in-plane plunger gates labeled as GL, GR, GM, PSL, PDL, PSR, and PDR are integrat‐ ed in close proximity to the dots. GL, GR, and GM are, respectively, designed to adjust the energy level of left dot, right dot, and inter-dot coupling strength. And PSL, PDL (PSR, PDR) are used for the tuning of the coupling of the left (right) dot to source and drain. The

beam evaporation of Ti/Au (2 nm/50 nm).

176 New Progress on Graphene Research

graphene.

**Figure 10.** Color online) (a), (b), and (c) PDQD differential conductance as a function of plunger gate voltage VGL and VGR. The red dash lines are guides to the eyes showing the honeycomb pattern. (N,M) represents the carriers in the left and right dot, respectively. (b) Zoom-in of the area (N,M) of the honeycomb pattern. (c) Zoom-in of a vertex pair with white dash lines. (d) Capacitance model for the analysis of the double dot system. Graphene nanoconstrictions behave as tunneling barriers, which are presented, for example, as RSL, CSL (a capacitance and a resistance coupled in paral‐ lel). Gate GL and GR are capacitively coupled to the dots; CGL and CGR represent the capacitance.

Fig. 10(a) shows color scale plot of the measured differential conductance of the double dot as a function of VGL and VGR detected in standard ac lock-in technique with anexcitation ac voltage 20*μ*V at frequency of 11.3 Hz. A dc bias of 0.3 mV is applied, the back gate voltage Vbg is fixed at 5 V and the middle plunger gate VGM is -0.45 V. The hexagon pattern characteristic for double dot coupled in parallel is clearly visible. Figure 2(b) Zoom-in of the area (N, M) of the honey‐ comb pattern, Figure 2(c) Zoom-in of a vertex pair with white dashed lines. From the model of purely capacitively coupled dots as illuminated by Figure 2(d), the energy scales of the system can be extracted (van der Wiel et al., 2003; Molitor et al., 2010; Moriyama et al., 2009). The capac‐ itance of the dot to the side gate can be determined from measuring the size of the honeycomb as shown in Fig. 10(a) and 10(b), *ΔVGL* =0.087V, *ΔVGR* =0.053V ,*ΔVGL <sup>m</sup>* =0.0261V *ΔVGR <sup>m</sup>* =0.0133V, therefore, *CGL* <sup>=</sup>*<sup>e</sup>* / *<sup>Δ</sup>VGL* =1.84aF,*CGR* <sup>=</sup>*<sup>e</sup>* / *<sup>Δ</sup>VGR* =3.0aF. With a large DC bias of 0.3 mV, we can get *δVGL* =0.013Vand *δVGR* =0.01V as shown in Figure 2(c). The lever arm be‐ tween the left (right) gate *V*GLand the left (right) dot can be calculated as *αGL* =*Vbias* / *δVGL* =0.023(*αGR* =*Vbias* / *δVGR* =0.03). The total capacitances of the dots can then be calculated as *CL* =*CGL* / *α<sup>L</sup>* =79.8aFand*CR* =*CGR* / *α<sup>R</sup>* =100.4aF, the corresponding charging en‐ ergy*ECL* =*αGL* .*ΔVGL* =2.0meVand*ECR* =*αGR*.*ΔVGR* =1.6meV, the coupling energy between the two dots*ECM* =*αGL* .*ΔVGL <sup>m</sup>* =0.3meV. It is also noted that the lever arms between the left gate and the right dot and vice versa can be determined from the slope of the co-tunneling lines de‐ limiting the hexagons. These crossing couplings only modify the results slightly and are ne‐ glected usually (Molitor et al., 2010; Moriyama et al., 2009; Liu et al., 2010). Here, by calculating dots area and carrier density (related to VBG), or from the Coulomb charging period, we esti‐ mate each dot contains more than 20 electrons when VBG=5V.

By applying voltage to the middle plunger gate GM, the interdot coupling can be tuned effi‐ ciently. Fig.11(a), 11(b),and 11(c) show the charge stability diagrams of the PDQD in three different coupling regimes. [(a) weak, (b) medium, and (c) strong]. In these measurements, back gate voltage VBG =3V, Source-Drain DC bias Vbias is set to-1.0mV, the scan regions of GL and GR are the same. Only the voltage applied to the gate GM is adjusted as (a) VGM= -0.15 V, (b) VGM=0.2 V, and (c) VGM=0.45 V. By using the same model as in Figure 2, we can calcu‐ late the corresponding coupling energy between the dots: (a) ECM=0.58 meV, (b) ECM=1.34 meV, and (c) ECM=4.07 meV. The honeycomb diagrams of the parallel and serial DQD look similar except for the weak coupling regime, as shown in Figure3(a). In this case, the lines delimiting the hexagons are more visible in comparison with serial DQD, because the leads have two parallel accesses to the dots in parallel DQD, which also enables correlated tunnel‐ ing of two valence electrons simultaneously (Holleitner et al., 2002). Fig. 11(d) indicates the coupling energy changes with the gate voltage VGM. As in the previous reports of graphene DQD in series (Molitor et al., 2010; Liu et al., 2010), the inter-dot coupling is non-monotoni‐ cally depended on the applied gate voltage. Although the detailed reasons for this non-mo‐ notony are undetermined, we assumed that one key factor will be the disorders in graphene introduced by either fabrication steps or substrate (Todd et al., 2009). Many more efforts are still needed to address this issue for the realization of practical graphene based nanodevices.

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**Figure 12.** Color online) (a) SEM image of single layer graphene PDQD integrated with two QPCs. The bar has a length of 500 nm. (b) Characteristic honeycomb structure of the conductance through the PDQD as a function of two in-

We have designed and fabricated an alternative structure of a PDQD integrated with two quantum point contact sensors (QPCs) in single layer graphene, as shown in Figure 4(a). The integrated QPCs can be used as a non-invasive charge detector which may have various ap‐ plications (van der Wiel et al., 2003; Hanson et al., 2007; Guo et al., 2001; Zhang et al., 2007). As primary tests of the present structure, we can get similar charge stability diagram of the PDQD as in Fig.12 (b) by the direct quantum transport tests at 4.2 K. Although the non-inva‐ sive measurements by QPC are still under processing, no remarkable difference is founded between PDQD in bilayer and monolayer graphenes from direct transport measurement. Making tunable coupling double dot is the first step towards the quantum dot based quan‐ tum computation bits, the architectonics with integrated charge detector around double quantum dot demonstrated here offers the chance to achieve the charge or spin reading out,

plane plunger gates voltage VGL and VGR, revealed by direct transport measurement of the PDQD at 4.2 K.

**Figure 11.** Color online) Interdot coupling vs middle gate voltage VGM. Conductance as a function of gate voltage VGL and VGR at VBG=3 V, Vbias=- 1 mV, the scan regions of GL and GR are the same. (a), (b), and (c) represent three different coupling regimes of the two dots. (a) weak coupling regime, VGM= -0.15 V, (b) medium coupling regime, VGM= -0.2 V (c) strong coupling regime, VGM= 0.45 V. (d) shows coupling energy ECM (V) as a non-monotonic function of the middle gate voltage VGM. A, B, C point here represent the corresponding coupling energy in (a), (b), and (c).

By applying voltage to the middle plunger gate GM, the interdot coupling can be tuned effi‐ ciently. Fig.11(a), 11(b),and 11(c) show the charge stability diagrams of the PDQD in three different coupling regimes. [(a) weak, (b) medium, and (c) strong]. In these measurements, back gate voltage VBG =3V, Source-Drain DC bias Vbias is set to-1.0mV, the scan regions of GL and GR are the same. Only the voltage applied to the gate GM is adjusted as (a) VGM= -0.15 V, (b) VGM=0.2 V, and (c) VGM=0.45 V. By using the same model as in Figure 2, we can calcu‐ late the corresponding coupling energy between the dots: (a) ECM=0.58 meV, (b) ECM=1.34 meV, and (c) ECM=4.07 meV. The honeycomb diagrams of the parallel and serial DQD look similar except for the weak coupling regime, as shown in Figure3(a). In this case, the lines delimiting the hexagons are more visible in comparison with serial DQD, because the leads have two parallel accesses to the dots in parallel DQD, which also enables correlated tunnel‐ ing of two valence electrons simultaneously (Holleitner et al., 2002). Fig. 11(d) indicates the coupling energy changes with the gate voltage VGM. As in the previous reports of graphene DQD in series (Molitor et al., 2010; Liu et al., 2010), the inter-dot coupling is non-monotoni‐ cally depended on the applied gate voltage. Although the detailed reasons for this non-mo‐ notony are undetermined, we assumed that one key factor will be the disorders in graphene introduced by either fabrication steps or substrate (Todd et al., 2009). Many more efforts are still needed to address this issue for the realization of practical graphene based nanodevices.

Fig. 10(a) shows color scale plot of the measured differential conductance of the double dot as a function of VGL and VGR detected in standard ac lock-in technique with anexcitation ac voltage 20*μ*V at frequency of 11.3 Hz. A dc bias of 0.3 mV is applied, the back gate voltage Vbg is fixed at 5 V and the middle plunger gate VGM is -0.45 V. The hexagon pattern characteristic for double dot coupled in parallel is clearly visible. Figure 2(b) Zoom-in of the area (N, M) of the honey‐ comb pattern, Figure 2(c) Zoom-in of a vertex pair with white dashed lines. From the model of purely capacitively coupled dots as illuminated by Figure 2(d), the energy scales of the system can be extracted (van der Wiel et al., 2003; Molitor et al., 2010; Moriyama et al., 2009). The capac‐ itance of the dot to the side gate can be determined from measuring the size of the honeycomb

as shown in Fig. 10(a) and 10(b), *ΔVGL* =0.087V, *ΔVGR* =0.053V ,*ΔVGL*

*<sup>m</sup>* =0.0133V, therefore, *CGL* <sup>=</sup>*<sup>e</sup>* / *<sup>Δ</sup>VGL* =1.84aF,*CGR* <sup>=</sup>*<sup>e</sup>* / *<sup>Δ</sup>VGR* =3.0aF. With a large DC bias of 0.3 mV, we can get *δVGL* =0.013Vand *δVGR* =0.01V as shown in Figure 2(c). The lever arm be‐ tween the left (right) gate *V*GLand the left (right) dot can be calculated as *αGL* =*Vbias* / *δVGL* =0.023(*αGR* =*Vbias* / *δVGR* =0.03). The total capacitances of the dots can then be calculated as *CL* =*CGL* / *α<sup>L</sup>* =79.8aFand*CR* =*CGR* / *α<sup>R</sup>* =100.4aF, the corresponding charging en‐ ergy*ECL* =*αGL* .*ΔVGL* =2.0meVand*ECR* =*αGR*.*ΔVGR* =1.6meV, the coupling energy between the

and the right dot and vice versa can be determined from the slope of the co-tunneling lines de‐ limiting the hexagons. These crossing couplings only modify the results slightly and are ne‐ glected usually (Molitor et al., 2010; Moriyama et al., 2009; Liu et al., 2010). Here, by calculating dots area and carrier density (related to VBG), or from the Coulomb charging period, we esti‐

**Figure 11.** Color online) Interdot coupling vs middle gate voltage VGM. Conductance as a function of gate voltage VGL and VGR at VBG=3 V, Vbias=- 1 mV, the scan regions of GL and GR are the same. (a), (b), and (c) represent three different coupling regimes of the two dots. (a) weak coupling regime, VGM= -0.15 V, (b) medium coupling regime, VGM= -0.2 V (c) strong coupling regime, VGM= 0.45 V. (d) shows coupling energy ECM (V) as a non-monotonic function of the middle

gate voltage VGM. A, B, C point here represent the corresponding coupling energy in (a), (b), and (c).

mate each dot contains more than 20 electrons when VBG=5V.

*<sup>m</sup>* =0.3meV. It is also noted that the lever arms between the left gate

*ΔVGR*

two dots*ECM* =*αGL* .*ΔVGL*

178 New Progress on Graphene Research

*<sup>m</sup>* =0.0261V

**Figure 12.** Color online) (a) SEM image of single layer graphene PDQD integrated with two QPCs. The bar has a length of 500 nm. (b) Characteristic honeycomb structure of the conductance through the PDQD as a function of two inplane plunger gates voltage VGL and VGR, revealed by direct transport measurement of the PDQD at 4.2 K.

We have designed and fabricated an alternative structure of a PDQD integrated with two quantum point contact sensors (QPCs) in single layer graphene, as shown in Figure 4(a). The integrated QPCs can be used as a non-invasive charge detector which may have various ap‐ plications (van der Wiel et al., 2003; Hanson et al., 2007; Guo et al., 2001; Zhang et al., 2007). As primary tests of the present structure, we can get similar charge stability diagram of the PDQD as in Fig.12 (b) by the direct quantum transport tests at 4.2 K. Although the non-inva‐ sive measurements by QPC are still under processing, no remarkable difference is founded between PDQD in bilayer and monolayer graphenes from direct transport measurement. Making tunable coupling double dot is the first step towards the quantum dot based quan‐ tum computation bits, the architectonics with integrated charge detector around double quantum dot demonstrated here offers the chance to achieve the charge or spin reading out, which is essential for the quantum computation device. Therefore, a lot of extended and fol‐ low-up works can be done on this basis in the future. Both bilayer and single layer graphe‐ nes can be exploited in this application.

**Acknowledgments**

**Author details**

**References**

(1999).

153304 (2008).

This work was supported by the National Basic Research Program of China (Grants No. 2011CBA00200 and 2011CB921200), and the National Natural Science Foundation of China

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181

Key Laboratory of Quantum Information, University of Science and Technology of China,

[1] Berman D, Zhitenev N. B, Ashoori R. C, and Shayegan M, Phys. Rev. Lett. 82, 161

[4] Dias da Silva L. G. G. V, Ingersent K, Sandler N, and Ulloa S. E, Phy. Rev. B 78,

[6] Elzerman J. M, Hanson R, L. van Beveren H. W, L. Vandersypen M. K, and Kouwen‐

[7] Elzerman J. M, Hanson R, van Beveren L. H. Witkamp W, B, Vandersypen L. M. K,

[10] Foletti S, Bluhm H, Mahalu D, Umansky V, and Yacoby A, Nat. Phys. 5, 903 (2009). [11] Gallagher P., Todd K., and Goldhaber-Gordon D., Phys. Rev. B 81, 115409 (2010).

[15] Gotz G, Steele G. A, Vos W. J, and Kouwenhoven L. P, Nano Lett. 8, 4039 (2008).

[5] Duty T, Gunnarsson D, Bladh K, and Delsing P, Phys. Rev. B 69, 40503(R) (2004).

Hai-Ou Li, Tao Tu, Gang Cao, Lin-Jun Wang, Guang-Can Guo and Guo-Ping Guo

[2] Bylander J, Duty T, and Delsing P, Nature London 434, 361 (2005).

hoven L. P, Appl. Phys. Lett. 84, 4617 (2004b).

[9] Fischer J. and Loss D, Science 324, 1277 (2009).

[13] Geim A. K., Science 324, 1530 (2009).

and L. P. Kouwenhoven, Nature London 430, 431 (2004a).

[12] Geim A. K and Novoselov K. S, Nature Mater. 6, 183 (2007).

[14] Golovach V. N, and Loss D, Phys. Rev. B 69, 245327 (2004).

[8] Fischer J, Trauzettel B, and Loss D, Phys. Rev. B 80, 155401 (2009).

[3] Chen J. C, Chang A. M, and Melloch M. R., Phys. Rev. Lett. 92, 176801 (2004).

(Grants No. 10934006, 11074243, 11174267, 91121014, and 60921091)

Chinese Academy of Sciences, Hefei, P.R. China

In summary, we have discussed low temperature quantum transport measurement of gatecontrolled parallel coupled double quantum dot on both bilayer and single layer graphenes. The inter-dot coupling strength can be largely tuned by graphene in-plane gates. With the quantum transport honeycomb charge stability diagrams, a common model of purely capac‐ itively coupled double dot is used to extract all the relevant energy scales and parameters of grapheme PDQD. Although many more effects are still needed to further upgrade and ex‐ ploit the present designed grapheme quantum dot system, the results have intensively dem‐ onstrated the promise of the realization of graphene nanodevice and desirable study of rich PDQD physical phenomena in graphene.

### **5. Conclusion**

To conclude, we have discussed the design and fabrication of etched gate tunable single and double quantum dots in single-layer and bilayer graphene and present several important quantum transport measurements in these systems. A quantum dot with an integrated charge sensor is becoming a common architecture for a spin or charge based solid state qu‐ bit. To implement such a structure in graphene, we have fabricated a twin-dot structure in which the larger QD serves as a single electron transistor (SET) to read out the charge state of the nearby gate controlled small QD. A high SET sensitivity of 10-3*e* / *Hz*allowed us to probe Coulomb charging as well as excited state spectra of the QD, even in the regime where the current through the QD is too small to be measured by conventional transport means. We also have measured quantum transport properties of gates controlled parallelcoupled double quantum dots (PDQD) and series-coupled double quantum dots (SDQD) device on both single layer and bilayer graphene with multiple electrostatic gates that are used to enhance control to investigate it. At low temperatures, the transport measurements reveal honeycomb charge stability diagrams which can be tuned from weak to strong interdot tunnel coupling regimes. We precisely extract a large inter-dot tunnel coupling strength for this system allowing for the observation of tunnel-coupled molecular states extending over the whole series-coupled double dot. The inter-dot coupling strength also can be effec‐ tively tuned from weak to strong by in-plane plunger gates for parallel-coupled double quantum dots. All the relevant energy scales

and parameters can be extracted from the honeycomb charge stability diagrams. The present method of designing and fabricating graphene DQD is demonstrated to be general and relia‐ ble and will enhance the realization of graphene nanodevice and desirable study of rich DQD physical phenomena in graphene, and highly controllable system serves as an essen‐ tial building block for quantum devices in a nuclear-spin-free world.

### **Acknowledgments**

which is essential for the quantum computation device. Therefore, a lot of extended and fol‐ low-up works can be done on this basis in the future. Both bilayer and single layer graphe‐

In summary, we have discussed low temperature quantum transport measurement of gatecontrolled parallel coupled double quantum dot on both bilayer and single layer graphenes. The inter-dot coupling strength can be largely tuned by graphene in-plane gates. With the quantum transport honeycomb charge stability diagrams, a common model of purely capac‐ itively coupled double dot is used to extract all the relevant energy scales and parameters of grapheme PDQD. Although many more effects are still needed to further upgrade and ex‐ ploit the present designed grapheme quantum dot system, the results have intensively dem‐ onstrated the promise of the realization of graphene nanodevice and desirable study of rich

To conclude, we have discussed the design and fabrication of etched gate tunable single and double quantum dots in single-layer and bilayer graphene and present several important quantum transport measurements in these systems. A quantum dot with an integrated charge sensor is becoming a common architecture for a spin or charge based solid state qu‐ bit. To implement such a structure in graphene, we have fabricated a twin-dot structure in which the larger QD serves as a single electron transistor (SET) to read out the charge state of the nearby gate controlled small QD. A high SET sensitivity of 10-3*e* / *Hz*allowed us to probe Coulomb charging as well as excited state spectra of the QD, even in the regime where the current through the QD is too small to be measured by conventional transport means. We also have measured quantum transport properties of gates controlled parallelcoupled double quantum dots (PDQD) and series-coupled double quantum dots (SDQD) device on both single layer and bilayer graphene with multiple electrostatic gates that are used to enhance control to investigate it. At low temperatures, the transport measurements reveal honeycomb charge stability diagrams which can be tuned from weak to strong interdot tunnel coupling regimes. We precisely extract a large inter-dot tunnel coupling strength for this system allowing for the observation of tunnel-coupled molecular states extending over the whole series-coupled double dot. The inter-dot coupling strength also can be effec‐ tively tuned from weak to strong by in-plane plunger gates for parallel-coupled double

and parameters can be extracted from the honeycomb charge stability diagrams. The present method of designing and fabricating graphene DQD is demonstrated to be general and relia‐ ble and will enhance the realization of graphene nanodevice and desirable study of rich DQD physical phenomena in graphene, and highly controllable system serves as an essen‐

tial building block for quantum devices in a nuclear-spin-free world.

nes can be exploited in this application.

180 New Progress on Graphene Research

PDQD physical phenomena in graphene.

quantum dots. All the relevant energy scales

**5. Conclusion**

This work was supported by the National Basic Research Program of China (Grants No. 2011CBA00200 and 2011CB921200), and the National Natural Science Foundation of China (Grants No. 10934006, 11074243, 11174267, 91121014, and 60921091)

## **Author details**

Hai-Ou Li, Tao Tu, Gang Cao, Lin-Jun Wang, Guang-Can Guo and Guo-Ping Guo

Key Laboratory of Quantum Information, University of Science and Technology of China, Chinese Academy of Sciences, Hefei, P.R. China

### **References**


[16] Graber M. R, Coish W. A, Hoffmann C, Weiss M, Furer J, Oberholzer S, Loss D, and Scho°nenberger C, Phys. Rev. B 74, 075427 (2007).

[36] Livermore C, Crouch C. H, Westervelt R. M, Campman K. L, and A. Gossard C, Sci‐

Quantum Transport in Graphene Quantum Dots

http://dx.doi.org/10.5772/52873

183

[38] Lu W, Ji Z. Q, Pfeiffer L, K. W. West, and A. J. Rimberg, Nature London 423, 422

[40] Molitor F, Droscher S, Guttinger J, Jacobson A, Stampfer C, Ihn T, and Ensslin K,

[41] Molitor F, Knowles H, Droscher S, Gasser U, Choi T, Roulleau P, Guttinger J, Jacob‐

[42] Moriyama S, Tsuya D, Watanabe E, Uji S, Shimizu M, T. Mori, T. Yamaguchi, and

[43] Novoselov K. S, Geim A. K, Morozov S. V, Jiang D, Zhang Y, Dubonos S. V, Grigorie‐

[44] Orellana P. A, Ladron de Guevara M. L, and Claro F, Phys. Rev. B 70, 233315 (2004).

[45] Petta J. R, Johnson A. C, Taylor J. M, Laird E. A, Yacoby A, Lukin M. D , Marcus C.

[46] Ponomarenko L, Schedin F, Katsnelson M, Yang R. Hill E, Novoselov K, and Geim A.

[47] Schnez S, Molitor F, Stampfer C, Guttinger J, Shorubalko I, Ihn T, and Ensslin K,

[48] Stampfer C, Guttinger J, F. Molitor, D. Graf, T. Ihn, and K. Ensslin, Appl. Phys. Lett.

[49] Stampfer C, Schurtenberger E, Molitor F, Guettinger J, Ihn T, and Ensslin K, Nano

[50] Stampfer C., Güttinger J., Hellmüller S., Molitor F., Ensslin K., and Ihn T., Phys. Rev.

[51] Todd K, Chou H. Amasha T, S, and Goldhaber-Gordon D, Nano Lett. 9, 416 (2009).

[53] van der Wiel W. de Francheschi G, S, Elzermann J. M, Fujisawa T, Tarucha S, and

[55] Vink I. T, Nooitgedagt T, Schouten R. N, and Vandersypen L. M. K, Appl. Phys. Lett.

[52] Trauzettel B, Bulaev D. V, Loss D, and Burkard G, Nat. Phys. 3, 192 (2007).

[54] Vijay R, M. H. Devoret, and I. Siddiqi, Rev. Sci. Instrum. 80, 111101 (2009).

Kouwenhoven L P, Rev. Mod. Phys. 75, 1 (2003).

sen A, Stampfer C, Ensslin K. et al., Europhys. Lett. 89, 67005 (2010).

[37] Lo´pez R, Aguado R, and Platero G, Phys. Rev. Lett. 89, 136802 (2002).

[39] Mason N, Biercuk M. J, and Marcus C. M, Science 303, 655 (2004).

ence 274, 1332 (1996).

Appl. Phys. Lett. 94, 222107 (2009).

Ishibashi K, Nano Lett. 9, 2891 (2009).

K, Science 320, 356 (2008).

92, 012102 (2008a).

Lett. 8, 2378 (2008b).

91, 123512 (2007).

Lett. 102, 056403 (2009).

Appl. Phys. Lett. 94, 012107 (2009).

va I. V, and Firsov A. A, Science 306, 666 (2004).

M, Hanson M. P, and Gossard A. C, Science 309, 2180 (2005).

(2003).


[16] Graber M. R, Coish W. A, Hoffmann C, Weiss M, Furer J, Oberholzer S, Loss D, and

[18] Guo G. P, Lin Z. R, Tu T, Cao G, Li X. P, and Guo G. C, New J. Phys.11, 123005

[19] Güttinger J, Seif J, Stampfer C, Capelli A, Ensslin K, and Ihn T, Phys. Rev. B 83,

[20] Güttinger J, Stampfer C, Hellmüller S, Molitor F, Ihn T, and Ensslin K, Appl. Phys.

[21] Hanson R, Kouwenhoven L. P, Petta J. R, Tarucha S, and Vandersypen L. M. K, Rev.

[22] Hanson R, Witkamp B, Vandersypen L. M. K, van Beveren L. H. W, Elzerman J. M,

[25] Holleitner A. W, Blick R. H, Hu° ttel A. K, Eberl K, and Kotthaus J. P, Science 297, 70

[26] Holleitner A. W, Decker C. R, Qin H, Eberl K, and Blick R. H, Phys. Rev. Lett. 87,

[27] Huard B, Sulpizio J. Stander A, Todd N. K, Yang B, and Goldhaber Gordon D, Phys.

[28] Ihn T., Guttinger J, Molitor F, Schnez S. Schurtenberger E, Jacobsen A, Hellmu°ller S,

[30] Kouwenhoven L. P, Marcus C, McEuen P. L, Tarucha S, Westervelt R. M, and N. S. Wingreen, in Mesoscopic Electron Transport, Series E:Applied Sciences Vol. 345, edited by Sohn L. L, Kouwenhoven L. P, and Schon G, Dordrecht Kluwer, 1997, pp.

[31] L. Ponomarenko, F. Schedin, Katsnelson M, Yang R, Hill E, Novoselov K, and Geim

[32] Ladro´n de Guevara M. L, Claro F, and Orellanal P. A, Phys. Rev. B 67, 195335 (2003).

[34] Lehnert K. W, Bladh K, Spietz L. F, Gunnarsson D, Schuster D. I, Delsing P, and

[33] LaHaye D, Buu O, Camarota B, and Schwab K. C, Science 304, 74 (2004).

[35] Liu X. L, Hug D, and L. Vandersypen M. K. Nano Lett. 10, 1623 (2010).

Schoelkopf R. J, Phys. Rev. Lett. 90, 027002 (2003).

Frey T, Droscher S, Stampfer C. et al., Mater. Today 13, 44 (2010).

[29] Knobel G. and Cleland A. N., Nature London 424, 291 (2003).

Scho°nenberger C, Phys. Rev. B 74, 075427 (2007).

(2009).

182 New Progress on Graphene Research

(2002).

105–214.

256802 (2001).

165445 (2011).

Lett. 93, 212102 (2008).

Mod. Phys. 79, 1217 (2007).

Rev. Lett. 98, 236803 (2007).

A, Science 320, 356 (2008).

[17] Guo G. P, Li C. F, and Guo G. C, Phys. Lett. A 286, 401 (2001).

and Kouwenhoven L. P, Phys. Rev. Lett. 91, 196802 (2003).

[23] Hanson R. and Awschalom D, Nature 453, 1043 (2008)

[24] Hatano T, Stopa M, and Tarucha S, Science 309, 268 (2005).


[56] Volk C, Fringes S, Terres B, Dauber J, Engels S, Trellenkamp S, and Stampfer C,.Nano Lett. 11, 3581 (2011).

**Chapter 7**

**Advances in Resistive Switching Memories Based on**

Memory devices are a prerequisite for today's information technology. In general, two dif‐ ferent segments can be distinguished. Random access type memories are based on semicon‐ ductor technology. These can be divided into static random access memories (SRAM) and dynamic random access memories (DRAM). In the following, only DRAM will be consid‐ ered, because it is the main RAM technology for standalone memory products. Mass storage devices are traditionally based on magnetic- and optical storage. But also here semiconduc‐ tor memories are gaining market share. The importance of semiconductor memories is con‐ sequently increasing (Mikolajick et al., 2009). Though SRAM and DRAM are very fast, both of them are volatile, which is a huge disadvantage, costing energy and additional periphery circuitry. Si-based Flash memory devices represent the most prominent nonvolatile data memory (NVM) because of their high density and low fabrication costs. However, Flash suf‐ fers from low endurance, low write speed, and high voltages required for the write opera‐ tions. In addition, further scaling, i.e., a continuation in increasing the density of Flash is expected to run into physical limits in the near future. Ferroelectric random access memory (FeRAM) and magnetoresistive random access memory (MRAM) cover niche markets for special applications. One reason among several others is that FeRAM as well as convention‐ al MRAM exhibit technological and inherent problems in the scalability, i.e., in achieving the same density as Flash today. In this circumstance, a renewed nonvolatile memory concept called resistance-switching random access memory (RRAM), which is based on resistance change modulated by electrical stimulus, has recently inspired scientific and commercial in‐ terests due to its high operation speed, high scalability, and multibit storage potential (Beck et al., 2000; Lu & Lieber, 2007; Dong et al., 2008). The reading of resistance states is nondes‐ tructive, and the memory devices can be operated without transistors in every cell (Lee et

> © 2013 Zhuge et al.; licensee InTech. This is an open access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use,

© 2013 Zhuge et al.; licensee InTech. This is a paper distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

distribution, and reproduction in any medium, provided the original work is properly cited.

**Graphene Oxide**

http://dx.doi.org/10.5772/51260

**1. Introduction**

Fei Zhuge, Bing Fu and Hongtao Cao

Additional information is available at the end of the chapter

