**6. Conclusion**

In this chapter we present our results on fabrication and optimization of photonic structures exploiting the photo-, thermo- and electro-induced changes in thin chalcogenide films. It is demonstrated that the irreversible and reversible changes of the optical properties of chalcogenide glasses can be used for modification of the optical contrast of materials in 1D photon photonic crystal and shift of the reflectance stop band. It was observed that the exposure to light leads to significant red shift of the resonant band (17 nm or 30 nm for asdeposited or annealed samples, respectively), while the annealing of the samples causes the stop band to move to shorter wavelengths - with 14 and 28 nm for exposed and as-deposited samples, respectively.

High electric voltage induces reversible changes of the refractive index of the sublayers in the photonic structure. It was observed a 3 nm red shift of the photonic stop band and decrease of the transmittance, ΔT = 2 % during the applying of the dc electric voltage. Although the electric voltage of 100 V is considerably high for applications in optolectronics, our initial results indicate for a possible path for the implementation of reversible tuning of the stop band in 1 D photonic crystals.

Chalcogenide glasses possess peculiar optical properties such as high linear and non-linear refractive index and transmittance in wide range of the infrared region. These unique properties make them irreplaceable materials for mid-infrared sensing, integrated optics and ultrahigh-bandwidth signal processing; recently, a new term –"chalcogenide photonics' (Eggleton et al., 2011), has been introduced. Good knowledge of the properties of the chalcogenide glasses and their changes under influence of external factors such as exposure to light, annealing or electric field has a key role in understanding the processes in these materials and would support manufacturing of chalcogenide photonic crystals.

## **7. References**

162 Photonic Crystals – Innovative Systems, Lasers and Waveguides

considerably high for applications in modern optoelectronic devices such as electrooptical modulators for high-speed time-domain-multiplexing (TDM) and wavelength-divisionmultiplexing systems (WDM). Further investigations would involve determination of the dependence of the elеctroabsorption effect on the composition of the chalcogenide glasses

23

24

25

Transmission [%]

Fig. 13. Transmission spectrum of As2S3/PMMA multilayer slab between thin transparent chromium electrodes. In the inset the transmission spectrum of the same sample in wide spectral range - 800-2500 nm - is presented (a); Evolution of the transmission coefficient at λ = 500 nm in cyclic switching on and off of dc electric voltage U = 100 V. The exponential

In this chapter we present our results on fabrication and optimization of photonic structures exploiting the photo-, thermo- and electro-induced changes in thin chalcogenide films. It is demonstrated that the irreversible and reversible changes of the optical properties of chalcogenide glasses can be used for modification of the optical contrast of materials in 1D photon photonic crystal and shift of the reflectance stop band. It was observed that the exposure to light leads to significant red shift of the resonant band (17 nm or 30 nm for asdeposited or annealed samples, respectively), while the annealing of the samples causes the stop band to move to shorter wavelengths - with 14 and 28 nm for exposed and as-deposited

High electric voltage induces reversible changes of the refractive index of the sublayers in the photonic structure. It was observed a 3 nm red shift of the photonic stop band and decrease of the transmittance, ΔT = 2 % during the applying of the dc electric voltage. Although the electric voltage of 100 V is considerably high for applications in optolectronics, our initial results indicate for a possible path for the implementation of reversible tuning of

Chalcogenide glasses possess peculiar optical properties such as high linear and non-linear refractive index and transmittance in wide range of the infrared region. These unique properties make them irreplaceable materials for mid-infrared sensing, integrated optics and ultrahigh-bandwidth signal processing; recently, a new term –"chalcogenide photonics' (Eggleton et al., 2011), has been introduced. Good knowledge of the properties of the chalcogenide glasses and their changes under influence of external factors such as exposure

26

27

El. field ON

(U = 100 V)

0 20 40 60

Time [min]

(U = 0 V)

El. field OFF El. field OFF

(U = 0 V)

(U = 100 V)

El. field ON

striving to reduce the voltage of the applied electric field.

= 1915 nm

1750 1800 1850 1900 1950

extrapolations are given with a dashed line (b).

Wavelength [nm]

 as-deposited applied electric voltage U = 100 V

1000 1500 2000 2500 <sup>0</sup>

Wavelength [nm]

0

**6. Conclusion** 

samples, respectively.

the stop band in 1 D photonic crystals.

20

40

20 40 60 Transmission [%]

Transmission [%]

60


Thin Chalcogenide Films for Photonic Applications 165

Freeman, D., Madden, S. & Luther-Davies, B. (2005). Fabrication of planar photonic crystals

Fritzsche. H. (1998). Toward understanding the photoinduced changes in chalcogenide glasses. *Semiconductors*, Vol.32, No.8, (August 1998), pp. 850-854, ISSN 1063-7826 Ganjoo, A., Jain, H., Yu, C., Song, R., Ryan, J.V., Irudayaraj, J., Ding, Y.J. & Pantano, C.G.

Ho, K., Chan, C. & Soukoulis, C. (1990). Existence of a photonic gap in periodic dielectric structures. *Phys. Rew. Lett.* Vol.65, No.23, pp. 3152-3155, ISSN 1079-7114 Houizot, P., Boussard-Plédel, C., Faber, A. J., Cheng, L. K., Bureau, B., Van Nijnatten, P. A.,

Joanopoulus, J.D., Meade, R.D. & Winn, J.N. (1995). *Photonic crystals: Molding the Flow of Light*, Princeton University Press, ISBN: 9781400828241, Princeton, USA John, S. (1987). Strong localization of photons in certain disordered dielectric superlattices,

Kastner, M., Adler, D., Fritzsche, H. (1976), Valence-Alternation Model for Localized Gap

Kawata, S., Sun, H.B., Tanaka, T., & Tanaka, K. (2001). Finer features for functional microdevices, *Nature*, 412, No. 6848, (August 2001), pp. 697-698, ISSN: 0028-0836 Kim, S.H & C K. Hwangbo, C.K. (2002). Design of omnidirectional high reflectors with

Kincl, M., Tasseva, J., Petkov, K., Knotek, P., Tichy, L., (2009) On the photo-induced shift of

Kohoutek, T., Wagner, T., Orava, J., Krbal, M., Ilavsky, J., Vesely, D. & Frumar, M. (2007a).

Kohoutek, T., Orava, J., Hrdlicka, M., Wagner, T., Vlcek, Mil., Frumar, M, (2007b). Planar

Kolomiets, B.T., Mazets, T.F. & Efendief, Sh.M. (1970), On The Energy Spectrum Of Vitreous

Konstantinov, I.; Babeva, Tz.; & Kitova, S. (1998), Analysis of errors in thin-film optical

Kovalskiy, A., Vlček, M., Jain, H., Fiserova, A., Waits, C.M. & Dubey, M. (2006).

*Cryst. Solids*, Vol.352, No.6-7, (May 2006), pp. 589 – 594, ISSN 0022-3093 Knotek, P., Tasseva, J., Petkov, K., Kincl, M. & Tichy, L. (2009). Optical properties and

*Films*, Vol.517, No.20, (August 2009), pp. 5943-5947, ISSN 0040-6090

*Solids,* Vol.68, No.5, (May 2007), pp. 1268-1271, ISSN: 0022-3697

Vol.355, No.28-30, (August 2009), pp.1521-1525, ISSN: 0022-3093

incidence, *Appl. Opt.* Vol.37, No.19, pp.4260 -4267, ISSN: 0003-6935

*Non-Cryst. Solids*, Vol.352, (May 2006), pp. 584-588, ISSN 0022-3093

*Phys. Rew. Lett.* Vol.58, No.23, pp. 2486–2489, ISSN 1079-7114

41, No. 16, (June 2002), pp. 3187-3192, ISSN: 0003-6935

No.4, (April 2009), pp. 395-398, ISSN 1454-4164

pp.3079-3086, ISSN 1094-4087

ISSN 0031-9007

in a chalcogenide glass using a focused ion beam. *Opt. Express*, Vol.13, No.8,

(2006). Planar chalcogenide glass waveguides for IR evanescent wave sensors. *J.* 

Gielesen, W. L. M., Pereira do Carmo, J., Lucas, J. (2007). Infrared single mode chalcogenide glass fiber for space. *Opt. Express* Vol.15, (Sep. 2007), pp. 12529-12538.

States in Lone-Pair Semiconductors. *Phys. Rev. Lett.* Vol.37, No.22, pp. 1504-1507,

quarter-wave dielectric stacks for optical telecommunication bands. *Appl. Opt.* Vol.

the optical gap in amorphous Ge6As43S35Se16 film., *J. Optoelectron. Adv. M.*, Vol.11

Multilayer systems of alternating chalcogenide As-Se and polymer thin films prepared using thermal evaporation and spin-coating techniques. *J. Phys. Chem.* 

quarter wave stacks prepared from chalcogenide Ge-Se and polymer polystyrene thin films. *J. Phys. Chem. Solids* Vol.68 No.12, (December 2007), pp. 2376-2380 Kohoutek, T., Orava, J., Prikryl, J., Wagner, T., Vlcek, Mil., Knotek, P. & Frumar, M. (2009b).

Planar chalcogenide quarter wave stack filter for near-infrared. *J. Non-Cryst. Solids,*

Arsenic Sulphide, *J. Non-Cryst. Solids*, Vol.4, (April 1970), pp.45-56, ISSN: 0022-3093

parameters derived from spectrophotometric measurements at normal light

Development of chalcogenide glass photoresists for gray scale lithography. *J. Non-*

scanning probe microscopy study of some Ag-As-S-Se amorphous films. *Thin Solid* 


Bureau, B., Zhang, X.H., Smektala, F., Adam, J.-L., Lucas, J., Troles, J., Ma, H.-L., Boussard-

Cai, L.Z., Yang, X.L. & Y.R. Wang, Y.R. (2002). All fourteen Bravais lattices can be formed by

Cardinal, T., Richardson, K.A., Shim, H., Shulte, A., Beatty, R., Le Foulgoc, K., Viens, J. F.,

DeCorby, R.G., Nguyen, H.T., Dwivedi, P.K. & Clement, T.J. (2005). Planar omnidirectional

De Neufville, J.P., Moss, S.C. & Ovshinsky, S.R. (1974), Photostructural transformations in

Divlianski, I., Mayer, T.S., Holliday, K.S. & Crespi, V.H. (2003). Fabrication of three-

Eggleton, B.J., Luther-Davies, B. & Richardson, K. (2011). Chalcogenide photonics. Nature

Egen, M., Zentel, R., Ferrand, P., Eiden, S, Maret, G., & Caruso, F. (2004), Preparation of 3D

Wiley – VCH, Weinheim, ISBN: 978-3-527-40432-2, Darmstadt, Germany Eisenberg, N.P., Manevich, M., Arsh, A., Klebanov, M. & Lyubin, V., (2005), Arrays of

Solid Films Vol.488, No.1-2, (September 2005), pp.185-188, ISSN: 0040-6090 Feigel, A., Veinger, M., Sfez, B., Arsh, A., Klebanov, M. & Lyubin, V. (2003). Three-

Fischer, W. (2001). A Second Note on the Term "Chalcogen". *J. Chem. Educ.* Vol.7, No.10, pp.

Photonics, Vol.5, No.3, (March 2011), pp.141-148, ISSN: 17494885

pp. 276-283, ISSN 0022-3093

pp.900-902, ISSN: 0146-9592

2011), pp. 2480-2483, ISSN 0022-3093

6233, ISSN: 1094-4087

1169, ISSN: 0003-6951

1679-1682, ISSN: 00368075

1333, ISSN 0021-9584

pp. 191-223, ISSN: 0022-3093

Pledel, C., Lucas, P., Le Coq, D., Riley, M.R. & Simmons, J.H. (2004). Recent advances in chalcogenide glasses. *J. Non-Cryst. Solids*, Vol.345&346, (October 2004),

interference of four noncoplanar beams. *Opt. Lett.* Vol. 27, No.11, (June 2002),

Villeneuve, A. (1999). Non-linear optical properties of chalcogenide glasses in the system As-S-Se. *J. Non-Cryst. Solids*, Vol.256&257, pp.353-360, ISSN 0022-3093 Charpentier, F., Bureau., B., Troles, J., Boussard-Plédel, C., Michel-Le Pierrès, K., Smektala,

F., Adam, J.-L. (2009). Infrared monitoring of underground CO2 storage using chalcogenide glass bers. *Opt. Mater.* Vol.31, No.3, pp.496–500, ISSN 0925-3467 Conseil, C., Coulombier, Q., Boussard-Plédel, C., Troles, J., Brilland, L., Renversez, G.,

Mechin, D., Bureau, B., Adam, J.L. & Lucas, J. (2011). Chalcogenide step index and microstructured single mode fibers. *J. Non-Cryst. Solids*, Vol.357, No.11-13, (June

reflectors in chalcogenide glass and polymer. *Opt. Express* Vol.13, No.16 pp.6228-

amorphous As2Se3 and As2S3 films, *J. Non-Cryst. Solids*, Vol.13, No.2, (January 1974),

dimensional polymer photonic crystal structures using single diffraction element interference lithography. *Appl. Phys. Lett.* Vol.82, No.11, (March 2003), pp.1667-

photonic crystal from opals, In: *Photonic crystals – advances in design, fabrication and characterization*, K. Busch, S. Lolkes, R.B. Wehrspohn, & H. Foll, (Ed.'s), 109-128,

micro-prisms and micro-mirrors for infrared light based on As2S3-As2Se3 photoresists., *J. Optoelectron. Adv. M.* Vol.7, No.5, pp. 2275-2280, ISSN 1454-4164 Feigel, A., Veinger, M., Sfez, B., Arsh, A., Klebanov, M., & Lyubin, V. (2005). Two

dimensional photonic band gap pattering in thin chalcogenide glassy films, Thin

dimensional simple cubic woodpile photonic crystals made from chalcogenide glasses. *Appl. Phys. Lett.* Vol.83, No.22, (Dec. 2003), pp.4480-4482, ISSN: 0003-6951 Fink, Y., Winn, J.N., Fan, S., Chen, C., Michel, J, Joannopoulos, J.D. & Thomas, E.L. (1998). A

dielectric omnidirectional reflector, *Science*, Vol.282, No. 20, (November 1998), pp.


Thin Chalcogenide Films for Photonic Applications 167

Ponnampalam, N. & DeCorby R. (2008). Analysis and fabrication of hybrid metal-dielectric omnidirectional Bragg reflectors. Appl. Opt. Vol. 47, pp. 30-37, ISSN 1464-4258 Raptis, C., Kotsalas, I.P., Papadimitriou, D., Vlcek, M., Frumar, M. (1997). *Physics and* 

Riley, B.J., Sundaram, S.K., Johnson, B.R., Saraf, L.V. (2008). Differential etching of

Rowlands, C.J., Su, L. & Elliott, S.R. (2010). Rapid prototyping of low-loss IR chalcogenide-

Saithoh A., Gotoh, T. & Tanaka, K. (2002). Chalcogenide-glass microlenses for optical fibers. *J Non-Cryst. Solids*, Vol.299-302, (April 2002), pp. 983-987, ISSN 0022-3093 Sakoda K. (2005) Optical Properties of Photonic Crystals, W. T. Rhodes (Ed), Springer-

Savović, S. & Djordjevich, A. (2011). Mode coupling in chalcogenide-glass optical fibers. *Opt.* 

Sheik-Bahae, M., Hagan, D. J., Van Stryland, E. W. (1990). Dispersion and band-gap scaling

Shimakawa, K., Kolobov, A. & Elliott, S.R. (1995). Photoinduced effects and metastability in

Skordeva, E., Arsova, D., Aneva, Z., Vuchkov, N., Astadjov, D. (2001). Laser induced

Su, L., Rowlands, C.J. & Elliott, S.R. (2009). Nanostructures fabricated in chalcogenide glass

Swanepoel, R. (1983). Determination of the thickness and optical constants of amorphous silicon, *J.Phys. E: Sci. Instrum.* Vol.16, No.12, pp.1214-1222, ISSN: 0022-3735 Tanaka, K. & Ohtsuka, Y. (1979). Composition dependence of photo-induced refractive

Tanaka, K. (2007). Nonlinear optics in glasses: How can we analyze? *J. Phys. Chem. Solids*,

Tasseva, J., Petkov, K., Kozhuharova, D. & Iliev, Tz. (2005). Light-induced changes in the

Tasseva, J., Lozanova, V., Todorov, R., Petkov, K. (2007). Optical Characterization of Ag/As-

*Adv. M.*, Vol.7, No.3, (March 2005), pp. 1287-1292, ISSN 1454-4164

Vol.68, No.5-6, (May 2007), pp. 896-900, ISSN 0022-3697

of the electronic Kerr effect in solids associated with two-photon absorption. *Phys.* 

amorphous semiconductors and insulators, *Adv. Phys.* Vol.44, No.6, (November

photodarkening and photobleaching in Ge-As-S thin films. *Proceedings of SPIE - The International Society for Optical Engineering*, Vol.4397, pp. 348-352, ISSN 0277786X Street, R.A. (1977). Non-radiative recombination in chalcogenide glasses. *Solid State Communications*, Vol.24, No.5, (November 1979), pp. 363-365, ISSN: 00381098 Su, L., Rowlands, C.J., Lee, T.H., Elliott, S.R. (2008). Fabrication of photonic waveguides in

sulfide chalcogenide glasses by selective wet-etching, *Electron. Lett.*, Vol.44, No.7,

for use as surface-enhanced Raman scattering substrates. *Opt. Lett.* Vol.34, No.11,

index changes in amorphous As-S films, *Thin Solid Films*, Vol.57 No. 1, (February

physico-chemical and optical properties of thin Ge–S– Se–As films. *J. Optoelectron.* 

S-Se thin films. *J. Optoelectron. Adv. M.*, Vol.9, No.10, pp. 3119-3124, ISSN 1454-4164

*High Technology*, 36, p. 291, M. Bertolotti, A. Andriesh (Eds.)

Verlag Berlin, Heidelberg, Germany, ISSN 0342-4111

*Rev. Lett.*, Vol.65, No.1, pp. 96-99, ISSN 0031-9007

2010), pp. 2393-2398, ISSN 1439-4235

1995), pp.475-588, ISSN: 00018732

pp. 472-474, ISSN 0013-5194

1979), pp. 59-64, ISSN 0040-6090

(June 2009), pp.1645-1647, ISSN: 0146-9592

Vol.354, No.10-11, (February 2008), pp. 813-816, ISSN 0022-3093

*Laser. Eng.* Vol.49, No.7, (July 2011), pp. 855-858, ISSN 0143-8166

*Applications of Non-crystalline Semiconductors in Optoelectronics, NATO ASI Series, 3.* 

chalcogenides for infrared photonic waveguide structures. *J. Non-Cryst. Solids*,

glass waveguides by controlled remelting. *Chem.Phys.Chem*., Vol.11, No.11, (August


Lai, N.D., Liang, W.P., Lin, J.H., Hsu, C.C. & Lin, C.H. (2005). Fabrication of two- and three-

Li, W., Seal, S., Rivero, C., Lopez, C., Richardson, K., Pope, A., Schulte, A., Myneni, S., Jain,

Liu, Q., Zhao, X., Gan, F., Mi, J., Qian, S. (2005). Ultrafast optical kerr effect in amorphous

Lopez, C. (2003). Materials Aspects of Photonic Crystals. *Adv. Mater.* Vol.15, No.20, (October

Lyubin, V. (1984). *Photographic processes on the base of the chalcogenide glassy semiconductors*, In:

Marquez, E., Gonzalez-Leal, J.M., Bernal-Oliva, A.M., Wágner, T., & Jimenez-Garay, R.

Milam, D. (1998) Review and Assessment of Measured Values of the Nonlinear Refractive-

Mizrahi, V., DeLong, K.W., Stegeman, G.I., Saifi, M. A., Andrejco, M. J., (1989), Two-photon

Nicoletti, E., Zhou, G., Jia, B., Ventura, M.J., Bulla, D., Luther-Davies, B. & Gu, M. (2008).

Okuda, M., Tri Nang, T. & Matsushita, T. (1979). Photo-induced absorption changes in

Ogusu, K., Maeda, S., Kitao, M., Li, H. & Minakata, M. (2004). Optical and structural

Petkov, K., Todorov, R., Tasseva, J. & Tsankov, D. (2009). Structure, linear and non-linear

*Phys.* Vol.92, No.12, (December 2002), pp. 7102-7108, ISSN: 00218979 Liao, M., Chaudhari, C., Qin, G., Yan, X., Kito, C., Suzuki, T., Ohishi, Y., Matsumoto, M. &

(November 2009), pp. 21608-21614, ISSN 1094-4087

2003), pp. 1679-1704, ISSN: 09359648

Vol.7, No.3, (March 2007), pp. 1323-1328, ISSN 1454-4164

Khimiyia, Leningrad (St. Petersburg), Russia (in Russian)

Vol.40, No.17, (September 2007), pp. 5351-5357, ISSN: 0022-3727

1285, ISSN: 094-4087

550, ISSN 1559-128X

1142, ISSN 0146-9592

pp.2311-2313, ISSN: 0146-9592

1979), pp. 403-406, ISSN 0040-6090

*Rev.* Vol.128, pp. 2093-2097, ISSN: 0031-899X

(December 2009), pp.2083-2091, ISSN 1454-4164

dimensional periodic structures by multi-exposure of two beam interference technique. *Opt. Express*, Vol.13, No.23, (Nov. 2005), pp. 9605-9611, ISSN: 094-4087 Lee, M.W.; Grillet, Ch; Smith, C.L.C.; Moss, D.J., Eggleton, B.J.; Freeman, D.; Luther-Davies,

B., Madden, S., Rode, A.; Ruan, Y. & Lee, Y-h. (2007). Photosensitive post tuning of chalcogenide photonic crystal waveguides, *Opt. Express* Vol. 15, No. 3, pp. 1277-

H., Antoine, K. & Miller, A.C. (2002). X-ray photoelectron spectroscopic investigation of surface chemistry of ternary As-S-Se chalcogenide glasses. *J. Appl.* 

Misumi, T. (2009). Fabrication and characterization of a chalcogenide-tellurite composite microstructure fiber with high nonlinearity. *Opt. Express*, Vol.17, No.24,

Ge10As40S30Se20 films induced by ultrashort laser pulses. *J. Optoelectron. Adv. M.*,

Non-silver photographic processes, A. Kartuzhanskovo (Ed.), pp. 188-208,

(2007), Preparation and optical dispersion and absorption of Ag-photodoped GexSb40-xS60 (x ≤ 10, 20 and 30) chalcogenide glass thin films, *J. Phys. D: Appl. Phys.*

Index Coefficient of Fused Silica. *Appl. Opt.* Vol.37, No.3, (January 1998), pp. 546-

absorption as a limitation to all-optical switching. *Opt. Lett.* Vol.14, No.20, pp.1140-

Observation of multiple higher-order stopgaps from three-dimensional chalcogenide glass photonic crystals. *Opt. Lett.* Vol.33, No.20, (October 2008),

selenium-based chalcogenide glass films. *Thin Solid Films*, Vol.58, No.2, (April

properties of Ag(Cu)–As2Se3 chalcogenide films prepared by a photodoping. *J. Non-Cryst. Solids* Vol.347, No.1-3, (November 2004), pp. 159-165, ISSN: 00223093 Penn, D.R. (1962). Wave-Number-Dependent Dielectric Function of Semiconductors, *Phys.* 

optical properties of thin AsxSe1-x films. *J. Optoelectron. Adv. M.*, Vol.11, No.12,


**10** 

*China* 

**Ultra-Broadband Time-Resolved Coherent** 

**and Microscopy with Photonic Crystal** 

*1College of Optoelectronic Engineering, Shenzhen University, Shenzhen* 

**Fiber Generated Supercontinuum** 

*Guangdong Province, Shenzhen University, Shenzhen* 

Hanben Niu1,2 and Jun Yin1,2

**Anti-Stokes Raman Scattering Spectroscopy** 

*2Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and* 

Optics, one of the oldest natural sciences, has been promoting the developments of sciences and technologies, especially the life science. The invention of the optical microscope eventually led to the discovery and study of cells and thus the birth of cellular biology, which now plays a more and more important role in the biology, medicine and life science. The greatest advantage of optical microscopy in the cellular biology is its ability to identify the distribution of different cellular components and further to map the cellular structure and monitor the dynamic process in cells with high specific contrast. In 1960's, with the invention of laser, an ideal coherent light source with high intensity was provided. Since then the combination of optical microscopy with laser has been expanded. Many novel optical microscopic methods and techniques were developed, such as various kinds of fluorescence microscopy. In fluorescence microscopy, the necessary chemical specificity is provided by the labeling samples with extrinsic fluorescent probes [1, 2]. With the developments of ultra-short laser, fluorescent labeling technique and modern microscopic imaging technique, the fluorescence spectroscopy and microscopy with high spatial resolution, sensitivity and chemical specificity has become the key promotion of the life science and unveiled many of the secrets of living cells and biological tissues [3, 4]. In particular, the confocal fluorescent microscope (CFM), with the confocal detection [5] and multi-photon excitation [6, 7], can obtain the 3D sectioning images of cells and tissues with high spatial resolution. Today, fluorescence microscopy has become a powerful research tool in life science and has achieved the great triumph. Nevertheless, the disadvantages of fluorescence microscopy, such as the photo-toxicity and photo-bleaching, can not be ignored [8]. Furthermore, some molecules in cells, such as water molecule and other small biomolecules, can not be labeled until now. Finally, for the biological species that do not fluoresce, the extrinsic fluorescent labels will unavoidablely disturb the original characteristics and functions of biological molecules, which will limit the applicability of fluorescence microscopy. Therefore, it is very necessary to develop some complementary

**1. Introduction** 

