Abstract

We demonstrate a scheme for efficient coherent anti-Stokes Raman scattering (CARS) microscopy free of nonresonant background. Our method is based on a compact Er:fiber laser source. Impulsive excitation of molecular resonances is achieved by an 11fs pulse at 1210nm. Broadband excitation gives access to molecular resonances from 0cm1 up to 4000cm1. Time-delayed narrowband probing at 775nm enables sensitive and high-speed spectral detection of the CARS signal free of nonresonant background with a resolution of 10cm1.

© 2010 Optical Society of America

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2009

2008

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Opt. Express 16, 15863 (2008).
[CrossRef] [PubMed]

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

C. Evans and X. S. Xie, Annu. Rev. Anal. Chem. 1, 883(2008).
[CrossRef]

2007

M. Müller and A. Zumbusch, Chem. Phys. Chem. 8, 2156(2007).
[CrossRef] [PubMed]

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

F. Adler, A. Sell, F. Sotier, R. Huber, and A. Leitenstorfer, Opt. Lett. 32, 3504 (2007).
[CrossRef] [PubMed]

2006

2005

A. Volkmer, J. Phys. D 38, R59 (2005).
[CrossRef]

2004

2002

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

2001

J.-X. Cheng, L. D. Book, and X. S. Xie, Opt. Lett. 26, 1341(2001).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, J. Phys. Chem. B 105, 1277 (2001).
[CrossRef]

1999

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

1978

A. Laubereau and W. Kaiser, Rev. Mod. Phys. 50, 607(1978).
[CrossRef]

Adler, F.

Ariunbold, G. O.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Book, L. D.

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

J.-X. Cheng, L. D. Book, and X. S. Xie, Opt. Lett. 26, 1341(2001).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, J. Phys. Chem. B 105, 1277 (2001).
[CrossRef]

Cerullo, G.

Cheng, J. X.

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, J. Phys. Chem. B 105, 1277 (2001).
[CrossRef]

Cheng, J.-X.

Cicerone, M. T.

Dogariu, A.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Evans, C.

C. Evans and X. S. Xie, Annu. Rev. Anal. Chem. 1, 883(2008).
[CrossRef]

Evans, C. L.

Gambetta, A.

Hanke, T.

Herek, J. L.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Phys. Rev. Lett. 103, 043905 (2009).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Opt. Express 16, 15863 (2008).
[CrossRef] [PubMed]

Holtom, G. R.

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Huang, Y.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Huber, R.

Jurna, M.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Phys. Rev. Lett. 103, 043905 (2009).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Opt. Express 16, 15863 (2008).
[CrossRef] [PubMed]

Kaiser, W.

A. Laubereau and W. Kaiser, Rev. Mod. Phys. 50, 607(1978).
[CrossRef]

Kee, T. W.

Korterik, J. P.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Phys. Rev. Lett. 103, 043905 (2009).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Opt. Express 16, 15863 (2008).
[CrossRef] [PubMed]

Krauss, G.

Kumar, V.

Laubereau, A.

A. Laubereau and W. Kaiser, Rev. Mod. Phys. 50, 607(1978).
[CrossRef]

Lee, Y. J.

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

Leitenstorfer, A.

Manzoni, C.

Marangoni, M.

Müller, M.

M. Müller and A. Zumbusch, Chem. Phys. Chem. 8, 2156(2007).
[CrossRef] [PubMed]

Murawski, R. K.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Offerhaus, H. L.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Phys. Rev. Lett. 103, 043905 (2009).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Opt. Express 16, 15863 (2008).
[CrossRef] [PubMed]

Otto, C.

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Phys. Rev. Lett. 103, 043905 (2009).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Opt. Express 16, 15863 (2008).
[CrossRef] [PubMed]

Pestov, D.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Potma, E. O.

Ramponi, R.

Rostovtsev, Y. V.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Sautenkov, V. A.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Scheu, R.

Scully, M. O.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Sell, A.

Selm, R.

Sokolov, A. V.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Sotier, F.

Tauser, F.

Träutlein, D.

Volkmer, A.

A. Volkmer, J. Phys. D 38, R59 (2005).
[CrossRef]

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, J. Phys. Chem. B 105, 1277 (2001).
[CrossRef]

Wang, X.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Winterhalder, M.

Xie, X. S.

C. Evans and X. S. Xie, Annu. Rev. Anal. Chem. 1, 883(2008).
[CrossRef]

E. O. Potma, C. L. Evans, and X. S. Xie, Opt. Lett. 31, 241(2006).
[CrossRef] [PubMed]

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, J. Phys. Chem. B 105, 1277 (2001).
[CrossRef]

J.-X. Cheng, L. D. Book, and X. S. Xie, Opt. Lett. 26, 1341(2001).
[CrossRef]

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Zhao, H. X.

Zhi, M.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

Zumbusch, A.

G. Krauss, T. Hanke, A. Sell, D. Träutlein, A. Leitenstorfer, R. Selm, M. Winterhalder, and A. Zumbusch, Opt. Lett. 34, 2847 (2009).
[CrossRef] [PubMed]

M. Müller and A. Zumbusch, Chem. Phys. Chem. 8, 2156(2007).
[CrossRef] [PubMed]

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Annu. Rev. Anal. Chem.

C. Evans and X. S. Xie, Annu. Rev. Anal. Chem. 1, 883(2008).
[CrossRef]

Appl. Phys. Lett.

A. Volkmer, L. D. Book, and X. S. Xie, Appl. Phys. Lett. 80, 1505 (2002).
[CrossRef]

Y. J. Lee and M. T. Cicerone, Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

Chem. Phys. Chem.

M. Müller and A. Zumbusch, Chem. Phys. Chem. 8, 2156(2007).
[CrossRef] [PubMed]

J. Phys. Chem. B

J. X. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, J. Phys. Chem. B 105, 1277 (2001).
[CrossRef]

J. Phys. D

A. Volkmer, J. Phys. D 38, R59 (2005).
[CrossRef]

Opt. Express

Opt. Lett.

Phys. Rev. Lett.

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

M. Jurna, J. P. Korterik, C. Otto, J. L. Herek, and H. L. Offerhaus, Phys. Rev. Lett. 103, 043905 (2009).
[CrossRef] [PubMed]

Rev. Mod. Phys.

A. Laubereau and W. Kaiser, Rev. Mod. Phys. 50, 607(1978).
[CrossRef]

Science

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, Science 316, 265 (2007).
[CrossRef] [PubMed]

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Figures (4)

Fig. 1
Fig. 1

(a) Time-resolved excitation scheme. (b) Excitation scheme in the frequency domain. Impulsive ex citation of the vibrational modes by an ultrashort broadband excitation pulse containing ω pump and ω S . A time-delayed narrowband flattop pulse ω probe probes the vibrational states oscillating at Ω. The CARS signal ω AS carries the spectral information of the Raman active resonances.

Fig. 2
Fig. 2

(a) Schematic setup: OSC, fs-Er:fiber oscillator; AMP, erbium-doped fiber amplifier; PC, silicon prism compressor; PC2, SF10 prism compressor; HNF, highly nonlinear germanosilicate fiber for frequency conversion; PM, parabolic mirror; PPLN, periodically poled lithium niobate crystal; VD, variable delay line; BC, dichroic beam combiner; T, telescope; O, objective; SS, scanning stage; S, spectrometer. (b) and (c) Spectrum and frequency-resolved optical gating data of excitation pulse. (d) Spectrum of probe pulse. (e) Probe pulse shape in time measured by a cross-correlation in the focus.

Fig. 3
Fig. 3

Time-resolved spectrum of Benzonitrile. Acquisition time 0.54 ms / spectrum , 0.97 s for all 1800 spectra with CCD recording.

Fig. 4
Fig. 4

Imaging of the lipid distribution of C. elegans. (a) Image recorded at the CH resonance at 2845 cm 1 with NRB. (b) Image recorded off resonance at 2645 cm 1 with NRB. (c) Profile plot with NRB along the line drawn in (a). (d) Image recorded at 2845 cm 1 with NRB suppression. (e) Image recorded off resonance at 2645 cm 1 with NRB suppression. (f) Profile plot with NRB suppression along the line drawn in (a).

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