Abstract

We introduce a novel configuration for broadband, time-resolved CARS spectroscopy/microscopy in which pump, Stokes and probe pulses are all derived from a single femtosecond Yb:KYW laser. The 1-MHz repetition rate of the system allows very intense CARS signals to be obtained over short acquisition times, while a delayed probe pulse ensures an efficient non-resonant background suppression.

© 2011 OSA

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  1. C. L. Evans and X. S. Xie, “Coherent anti-stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 883–909 (2008).
    [CrossRef] [PubMed]
  2. S. Roy, J. R. Gord, and A. K. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developments and applications in reacting flows,” Progr. in Energy & CombScience 36, 280–306 (2010).
    [CrossRef]
  3. H. Kano and H. Hamaguchi, “Ultrabroadband (>2500 cm−1) multiplex coherent anti-Stokes Raman scattering microspectroscopy using a supercontinuum generated from a photonic crystal fiber,” Appl. Phys. Lett. 86(12), 121113 (2005).
    [CrossRef]
  4. O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
    [CrossRef]
  5. J.-X. Cheng, L. D. Book, and X. S. Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26(17), 1341–1343 (2001).
    [CrossRef] [PubMed]
  6. F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006).
    [CrossRef] [PubMed]
  7. X. Wang, A. Zhang, M. Zhi, A. V. Sokolov, G. R. Welch, and M. O. Scully, “Heterodyne coherent anti-Stokes Raman scattering for spectral phase retrieval and signal amplification,” Opt. Lett. 35(5), 721–723 (2010).
    [CrossRef] [PubMed]
  8. H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
    [CrossRef] [PubMed]
  9. Y. Liu, Y. J. Lee, and M. T. Cicerone, “Broadband CARS spectral phase retrieval using a time-domain Kramers-Kronig transform,” Opt. Lett. 34(9), 1363–1365 (2009).
    [CrossRef] [PubMed]
  10. C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
    [CrossRef] [PubMed]
  11. E. Ploetz, B. Marx, T. Klein, R. Huber, and P. Gilch, “A 75 MHz light source for femtosecond stimulated raman microscopy,” Opt. Express 17(21), 18612–18620 (2009).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  15. H. Kano and H. Hamaguchi, “Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy,” J. Raman Spectrosc. 37(1-3), 411–415 (2006).
    [CrossRef]
  16. Y. J. Lee, S. H. Parekh, Y. H. Kim, and M. T. Cicerone, “Optimized continuum from a photonic crystal fiber for broadband time-resolved coherent anti-Stokes Raman scattering,” Opt. Express 18(5), 4371–4379 (2010).
    [CrossRef] [PubMed]
  17. R. Selm, M. Winterhalder, A. Zumbusch, G. Krauss, T. Hanke, A. Sell, and A. Leitenstorfer, “Ultrabroadband background-free coherent anti-Stokes Raman scattering microscopy based on a compact Er:fiber laser system,” Opt. Lett. 35(19), 3282–3284 (2010).
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  18. M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B 97(3), 561–574 (2009).
    [CrossRef]
  19. S.-H. Shim and M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
    [CrossRef] [PubMed]
  20. B. von Vacano, L. Meyer, and M. Motzkus, “Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy,” J. Raman Spectrosc. 38(7), 916–926 (2007).
    [CrossRef]
  21. M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
    [CrossRef] [PubMed]
  22. D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
    [CrossRef] [PubMed]

2010

2009

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B 97(3), 561–574 (2009).
[CrossRef]

S.-H. Shim and M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
[CrossRef] [PubMed]

Y. Liu, Y. J. Lee, and M. T. Cicerone, “Broadband CARS spectral phase retrieval using a time-domain Kramers-Kronig transform,” Opt. Lett. 34(9), 1363–1365 (2009).
[CrossRef] [PubMed]

E. Ploetz, B. Marx, T. Klein, R. Huber, and P. Gilch, “A 75 MHz light source for femtosecond stimulated raman microscopy,” Opt. Express 17(21), 18612–18620 (2009).
[CrossRef] [PubMed]

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

2008

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

C. L. Evans and X. S. Xie, “Coherent anti-stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 883–909 (2008).
[CrossRef] [PubMed]

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
[CrossRef]

2007

H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
[CrossRef] [PubMed]

B. von Vacano, L. Meyer, and M. Motzkus, “Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy,” J. Raman Spectrosc. 38(7), 916–926 (2007).
[CrossRef]

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

2006

2005

H. Kano and H. Hamaguchi, “Ultrabroadband (>2500 cm−1) multiplex coherent anti-Stokes Raman scattering microspectroscopy using a supercontinuum generated from a photonic crystal fiber,” Appl. Phys. Lett. 86(12), 121113 (2005).
[CrossRef]

2001

1980

Ariunbold, G. O.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Baum, P.

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B 97(3), 561–574 (2009).
[CrossRef]

Bonn, D.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

Bonn, M.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
[CrossRef] [PubMed]

Book, L. D.

Bradler, M.

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B 97(3), 561–574 (2009).
[CrossRef]

Cheng, J.-X.

Cicerone, M. T.

Dogariu, A.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Evans, C. L.

C. L. Evans and X. S. Xie, “Coherent anti-stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 883–909 (2008).
[CrossRef] [PubMed]

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006).
[CrossRef] [PubMed]

Freudiger, C. W.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Ganikhanov, F.

Gilch, P.

Gord, J. R.

S. Roy, J. R. Gord, and A. K. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developments and applications in reacting flows,” Progr. in Energy & CombScience 36, 280–306 (2010).
[CrossRef]

Hamaguchi, H.

H. Kano and H. Hamaguchi, “Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy,” J. Raman Spectrosc. 37(1-3), 411–415 (2006).
[CrossRef]

H. Kano and H. Hamaguchi, “Ultrabroadband (>2500 cm−1) multiplex coherent anti-Stokes Raman scattering microspectroscopy using a supercontinuum generated from a photonic crystal fiber,” Appl. Phys. Lett. 86(12), 121113 (2005).
[CrossRef]

Hanke, T.

He, C.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Herek, J. L.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Holtom, G. R.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Huang, Y.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Huber, R.

Jurna, M.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Kamga, F. M.

Kang, J. X.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Kano, H.

H. Kano and H. Hamaguchi, “Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy,” J. Raman Spectrosc. 37(1-3), 411–415 (2006).
[CrossRef]

H. Kano and H. Hamaguchi, “Ultrabroadband (>2500 cm−1) multiplex coherent anti-Stokes Raman scattering microspectroscopy using a supercontinuum generated from a photonic crystal fiber,” Appl. Phys. Lett. 86(12), 121113 (2005).
[CrossRef]

Katz, O.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
[CrossRef]

Kim, Y. H.

Klein, T.

Kleinebudde, P.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Krauss, G.

Lee, Y. J.

Leitenstorfer, A.

Liu, Y.

Lu, S.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Marx, B.

Meyer, L.

B. von Vacano, L. Meyer, and M. Motzkus, “Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy,” J. Raman Spectrosc. 38(7), 916–926 (2007).
[CrossRef]

Min, W.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Motzkus, M.

B. von Vacano, L. Meyer, and M. Motzkus, “Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy,” J. Raman Spectrosc. 38(7), 916–926 (2007).
[CrossRef]

Muller, M.

H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
[CrossRef] [PubMed]

Müller, M.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

Murawski, R. K.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Natan, A.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
[CrossRef]

Offerhaus, H. L.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Parekh, S. H.

Patnaik, A. K.

S. Roy, J. R. Gord, and A. K. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developments and applications in reacting flows,” Progr. in Energy & CombScience 36, 280–306 (2010).
[CrossRef]

Pestov, D.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Ploetz, E.

Riedle, E.

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B 97(3), 561–574 (2009).
[CrossRef]

Rinia, H. A.

H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
[CrossRef] [PubMed]

Rosenwaks, S.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
[CrossRef]

Rostovtsev, Y. V.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Roy, S.

S. Roy, J. R. Gord, and A. K. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developments and applications in reacting flows,” Progr. in Energy & CombScience 36, 280–306 (2010).
[CrossRef]

Saar, B. G.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006).
[CrossRef] [PubMed]

Sautenkov, V. A.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Sceats, M. G.

Schafer, D.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

Scully, M. O.

X. Wang, A. Zhang, M. Zhi, A. V. Sokolov, G. R. Welch, and M. O. Scully, “Heterodyne coherent anti-Stokes Raman scattering for spectral phase retrieval and signal amplification,” Opt. Lett. 35(5), 721–723 (2010).
[CrossRef] [PubMed]

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Sell, A.

Selm, R.

Serebryannikov, E. E.

Shim, S.-H.

S.-H. Shim and M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
[CrossRef] [PubMed]

Sidorov-Biryukov, D. A.

Silberberg, Y.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
[CrossRef]

Sokolov, A. V.

X. Wang, A. Zhang, M. Zhi, A. V. Sokolov, G. R. Welch, and M. O. Scully, “Heterodyne coherent anti-Stokes Raman scattering for spectral phase retrieval and signal amplification,” Opt. Lett. 35(5), 721–723 (2010).
[CrossRef] [PubMed]

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Squier, J. A.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

Strachan, C. J.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Tsai, J. C.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

van Maarseveen, J.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

Vartiainen, E. M.

H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
[CrossRef] [PubMed]

von Vacano, B.

B. von Vacano, L. Meyer, and M. Motzkus, “Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy,” J. Raman Spectrosc. 38(7), 916–926 (2007).
[CrossRef]

Wang, X.

X. Wang, A. Zhang, M. Zhi, A. V. Sokolov, G. R. Welch, and M. O. Scully, “Heterodyne coherent anti-Stokes Raman scattering for spectral phase retrieval and signal amplification,” Opt. Lett. 35(5), 721–723 (2010).
[CrossRef] [PubMed]

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Welch, G. R.

Windbergs, M.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Winterhalder, M.

Xie, X. S.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

C. L. Evans and X. S. Xie, “Coherent anti-stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 883–909 (2008).
[CrossRef] [PubMed]

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006).
[CrossRef] [PubMed]

J.-X. Cheng, L. D. Book, and X. S. Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26(17), 1341–1343 (2001).
[CrossRef] [PubMed]

Zanni, M. T.

S.-H. Shim and M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
[CrossRef] [PubMed]

Zhang, A.

Zheltikov, A. M.

Zhi, M.

Zhi, M. C.

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

Zumbusch, A.

Anal. Chem.

M. Windbergs, M. Jurna, H. L. Offerhaus, J. L. Herek, P. Kleinebudde, and C. J. Strachan, “Chemical imaging of oral solid dosage forms and changes upon dissolution using coherent anti-Stokes Raman scattering microscopy,” Anal. Chem. 81(6), 2085–2091 (2009).
[CrossRef] [PubMed]

Ann. Rev. Anal. Chem. (Palo Alto Calif)

C. L. Evans and X. S. Xie, “Coherent anti-stokes Raman scattering microscopy: chemical imaging for biology and medicine,” Ann. Rev. Anal. Chem. (Palo Alto Calif) 1(1), 883–909 (2008).
[CrossRef] [PubMed]

Appl. Phys. B

M. Bradler, P. Baum, and E. Riedle, “Femtosecond continuum generation in bulk laser host materials with sub-µJ pump pulses,” Appl. Phys. B 97(3), 561–574 (2009).
[CrossRef]

Appl. Phys. Lett.

H. Kano and H. Hamaguchi, “Ultrabroadband (>2500 cm−1) multiplex coherent anti-Stokes Raman scattering microspectroscopy using a supercontinuum generated from a photonic crystal fiber,” Appl. Phys. Lett. 86(12), 121113 (2005).
[CrossRef]

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, “Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses,” Appl. Phys. Lett. 92(17), 171116 (2008).
[CrossRef]

ChemPhysChem

H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition,” ChemPhysChem 8(2), 279–287 (2007).
[CrossRef] [PubMed]

J. Am. Chem. Soc.

D. Schafer, J. A. Squier, J. van Maarseveen, D. Bonn, M. Bonn, and M. Müller, “In situ quantitative measurement of concentration profiles in a microreactor with submicron resolution using multiplex CARS microscopy,” J. Am. Chem. Soc. 130(35), 11592–11593 (2008).
[CrossRef] [PubMed]

J. Raman Spectrosc.

B. von Vacano, L. Meyer, and M. Motzkus, “Rapid polymer blend imaging with quantitative broadband multiplex CARS microscopy,” J. Raman Spectrosc. 38(7), 916–926 (2007).
[CrossRef]

H. Kano and H. Hamaguchi, “Dispersion-compensated supercontinuum generation for ultrabroadband multiplex coherent anti-Stokes Raman scattering spectroscopy,” J. Raman Spectrosc. 37(1-3), 411–415 (2006).
[CrossRef]

Opt. Express

Opt. Lett.

F. M. Kamga and M. G. Sceats, “Pulse-sequenced coherent anti-Stokes Raman scattering spectroscopy: a method for suppression of the nonresonant background,” Opt. Lett. 5(3), 126–128 (1980).
[CrossRef] [PubMed]

D. A. Sidorov-Biryukov, E. E. Serebryannikov, and A. M. Zheltikov, “Time-resolved coherent anti-Stokes Raman scattering with a femtosecond soliton output of a photonic-crystal fiber,” Opt. Lett. 31(15), 2323–2325 (2006).
[CrossRef] [PubMed]

R. Selm, M. Winterhalder, A. Zumbusch, G. Krauss, T. Hanke, A. Sell, and A. Leitenstorfer, “Ultrabroadband background-free coherent anti-Stokes Raman scattering microscopy based on a compact Er:fiber laser system,” Opt. Lett. 35(19), 3282–3284 (2010).
[CrossRef] [PubMed]

Y. Liu, Y. J. Lee, and M. T. Cicerone, “Broadband CARS spectral phase retrieval using a time-domain Kramers-Kronig transform,” Opt. Lett. 34(9), 1363–1365 (2009).
[CrossRef] [PubMed]

J.-X. Cheng, L. D. Book, and X. S. Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26(17), 1341–1343 (2001).
[CrossRef] [PubMed]

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006).
[CrossRef] [PubMed]

X. Wang, A. Zhang, M. Zhi, A. V. Sokolov, G. R. Welch, and M. O. Scully, “Heterodyne coherent anti-Stokes Raman scattering for spectral phase retrieval and signal amplification,” Opt. Lett. 35(5), 721–723 (2010).
[CrossRef] [PubMed]

Phys. Chem. Chem. Phys.

S.-H. Shim and M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
[CrossRef] [PubMed]

Progr. in Energy & CombScience

S. Roy, J. R. Gord, and A. K. Patnaik, “Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developments and applications in reacting flows,” Progr. in Energy & CombScience 36, 280–306 (2010).
[CrossRef]

Science

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316(5822), 265–268 (2007).
[CrossRef] [PubMed]

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Figures (4)

Fig. 1
Fig. 1

Schematic diagram of the experimental setup for three-colour TR-CARS. BS: beam splitter; DBS: dichroic beam splitter; LBO: lithium triborate; WP: half-wave plate; OMA: optical multichannel analyzer.

Fig. 2
Fig. 2

(a): spectra of the pump (black), Stokes (blue) and probe (red) pulses. (b): zoom of the probe spectrum indicating a 13 cm−1 FWHM (9 cm−1 after deconvolution with the spectrometer response).

Fig. 3
Fig. 3

(a) Two-colour CARS spectra of different solvents; (b) three-colour TR-CARS spectra of methanol as a function of the delay of the probe pulse with respect to the pump/ Stokes pair.

Fig. 4
Fig. 4

(a) Three-colour TR-CARS spectra of different solvents at Δt = 330 fs; (b) TR-CARS spectrum of a 6.25% diluted solution of methanol in water.

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