Abstract

Stimulated Raman scattering (SRS) is a powerful tool for obtaining background-free chemical information about a material without extrinsic labeling. Background-free spectra are particularly important in the fingerprint region (~800 and 1800 cm−1) where peaks are narrow, closely-spaced, and may be in abundance for a particular chemical. We demonstrate a method for obtaining SRS spectra using a single femtosecond laser oscillator. A photonic crystal fiber is used to create a supercontinuum to provide a range of Stokes shifts from ~300 to 3400 cm−1. This SRS approach provides for collection capabilities that are easily modified between obtaining broadband spectra and single-frequency images.

©2011 Optical Society of America

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References

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  1. J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
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    [Crossref]
  3. M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
    [Crossref]
  4. B. D. Patel and P. J. Mehta, “An overview: application of Raman spectroscopy in pharmaceutical field,” Curr. Pharm. Anal. 6(2), 131–141 (2010).
    [Crossref]
  5. A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
    [Crossref]
  6. J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
    [Crossref]
  7. 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]
  8. 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).
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    [Crossref] [PubMed]
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    [Crossref]
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    [Crossref]
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    [Crossref] [PubMed]
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    [Crossref] [PubMed]
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2010 (2)

B. D. Patel and P. J. Mehta, “An overview: application of Raman spectroscopy in pharmaceutical field,” Curr. Pharm. Anal. 6(2), 131–141 (2010).
[Crossref]

S. H. Parekh, Y. J. Lee, K. A. Aamer, and M. T. Cicerone, “Label-free cellular imaging by broadband coherent anti-Stokes Raman scattering microscopy,” Biophys. J. 99(8), 2695–2704 (2010).
[Crossref] [PubMed]

2009 (4)

A. F. Pegoraro, A. Ridsdale, D. J. Moffatt, Y. W. Jia, J. P. Pezacki, and A. Stolow, “Optimally chirped multimodal CARS microscopy based on a single Ti:sapphire oscillator,” Opt. Express 17(4), 2984–2996 (2009).
[Crossref] [PubMed]

Y. X. 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]

Y. X. Liu, Y. J. Lee, and M. T. Cicerone, “Fast extraction of resonant vibrational response from CARS spectra with arbitrary nonresonant background,” J. Raman Spectrosc. 40(7), 726–731 (2009).
[Crossref]

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[Crossref]

2008 (3)

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]

J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
[Crossref]

I. Rocha-Mendoza, W. Langbein, and P. Borri, “Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion,” Appl. Phys. Lett. 93(20), 201103 (2008).
[Crossref]

2006 (3)

2004 (1)

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85(1), 25–27 (2004).
[Crossref]

2002 (1)

T. C. Bakker Schut, R. Wolthuis, P. J. Caspers, and G. J. Puppels, “Real-time tissue characterization on the basis of in vivo Raman spectra,” J. Raman Spectrosc. 33(7), 580–585 (2002).
[Crossref]

2001 (2)

J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
[Crossref]

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]

1999 (1)

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[Crossref]

1995 (1)

M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
[Crossref]

1992 (1)

Aamer, K. A.

S. H. Parekh, Y. J. Lee, K. A. Aamer, and M. T. Cicerone, “Label-free cellular imaging by broadband coherent anti-Stokes Raman scattering microscopy,” Biophys. J. 99(8), 2695–2704 (2010).
[Crossref] [PubMed]

Bakker Schut, T. C.

T. C. Bakker Schut, R. Wolthuis, P. J. Caspers, and G. J. Puppels, “Real-time tissue characterization on the basis of in vivo Raman spectra,” J. Raman Spectrosc. 33(7), 580–585 (2002).
[Crossref]

Bonn, M.

Book, L. D.

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]

J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
[Crossref]

Borri, P.

I. Rocha-Mendoza, W. Langbein, and P. Borri, “Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion,” Appl. Phys. Lett. 93(20), 201103 (2008).
[Crossref]

Caspers, P. J.

T. C. Bakker Schut, R. Wolthuis, P. J. Caspers, and G. J. Puppels, “Real-time tissue characterization on the basis of in vivo Raman spectra,” J. Raman Spectrosc. 33(7), 580–585 (2002).
[Crossref]

Chan, J.

J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
[Crossref]

Cheng, J.

J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
[Crossref]

Cheng, J. X.

Cicerone, M. T.

S. H. Parekh, Y. J. Lee, K. A. Aamer, and M. T. Cicerone, “Label-free cellular imaging by broadband coherent anti-Stokes Raman scattering microscopy,” Biophys. J. 99(8), 2695–2704 (2010).
[Crossref] [PubMed]

Y. X. Liu, Y. J. Lee, and M. T. Cicerone, “Fast extraction of resonant vibrational response from CARS spectra with arbitrary nonresonant background,” J. Raman Spectrosc. 40(7), 726–731 (2009).
[Crossref]

Y. X. 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]

Enejder, A. M. K.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85(1), 25–27 (2004).
[Crossref]

Evans, C. L.

Fore, S.

J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
[Crossref]

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.

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]

Hellerer, T.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85(1), 25–27 (2004).
[Crossref]

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]

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[Crossref]

Huser, T.

J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
[Crossref]

Jia, Y. W.

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]

Karakatsanis, C. G.

M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
[Crossref]

Kovalev, A.

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[Crossref]

Langbein, W.

I. Rocha-Mendoza, W. Langbein, and P. Borri, “Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion,” Appl. Phys. Lett. 93(20), 201103 (2008).
[Crossref]

Lau, C. J.

M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
[Crossref]

Lee, Y. J.

S. H. Parekh, Y. J. Lee, K. A. Aamer, and M. T. Cicerone, “Label-free cellular imaging by broadband coherent anti-Stokes Raman scattering microscopy,” Biophys. J. 99(8), 2695–2704 (2010).
[Crossref] [PubMed]

Y. X. Liu, Y. J. Lee, and M. T. Cicerone, “Fast extraction of resonant vibrational response from CARS spectra with arbitrary nonresonant background,” J. Raman Spectrosc. 40(7), 726–731 (2009).
[Crossref]

Y. X. 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]

Liu, Y. X.

Y. X. 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]

Y. X. Liu, Y. J. Lee, and M. T. Cicerone, “Fast extraction of resonant vibrational response from CARS spectra with arbitrary nonresonant background,” J. Raman Spectrosc. 40(7), 726–731 (2009).
[Crossref]

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]

Mehta, P. J.

B. D. Patel and P. J. Mehta, “An overview: application of Raman spectroscopy in pharmaceutical field,” Curr. Pharm. Anal. 6(2), 131–141 (2010).
[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]

Moffatt, D. J.

Motzkus, M.

Müller, M.

Nandakumar, P.

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[Crossref]

Parekh, S. H.

S. H. Parekh, Y. J. Lee, K. A. Aamer, and M. T. Cicerone, “Label-free cellular imaging by broadband coherent anti-Stokes Raman scattering microscopy,” Biophys. J. 99(8), 2695–2704 (2010).
[Crossref] [PubMed]

Patel, B. D.

B. D. Patel and P. J. Mehta, “An overview: application of Raman spectroscopy in pharmaceutical field,” Curr. Pharm. Anal. 6(2), 131–141 (2010).
[Crossref]

Pegoraro, A. F.

Pezacki, J. P.

Puppels, G. J.

T. C. Bakker Schut, R. Wolthuis, P. J. Caspers, and G. J. Puppels, “Real-time tissue characterization on the basis of in vivo Raman spectra,” J. Raman Spectrosc. 33(7), 580–585 (2002).
[Crossref]

Ridsdale, A.

Rinia, H. A.

Rocha-Mendoza, I.

I. Rocha-Mendoza, W. Langbein, and P. Borri, “Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion,” Appl. Phys. Lett. 93(20), 201103 (2008).
[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]

Schaeberle, M. D.

M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
[Crossref]

Stolow, A.

Treado, P. J.

M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
[Crossref]

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]

Vartiainen, E. M.

Volkmer, A.

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[Crossref]

J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
[Crossref]

von Vacano, B.

Wachsmann-Hogiu, S.

J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
[Crossref]

Wohlleben, W.

Wolthuis, R.

T. C. Bakker Schut, R. Wolthuis, P. J. Caspers, and G. J. Puppels, “Real-time tissue characterization on the basis of in vivo Raman spectra,” J. Raman Spectrosc. 33(7), 580–585 (2002).
[Crossref]

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]

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. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
[Crossref]

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]

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[Crossref]

Zumbusch, A.

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85(1), 25–27 (2004).
[Crossref]

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[Crossref]

Anal. Chem. (1)

M. D. Schaeberle, C. G. Karakatsanis, C. J. Lau, and P. J. Treado, “Raman chemical imaging—noninvasive visualization of polymer blend architecture,” Anal. Chem. 67(23), 4316–4321 (1995).
[Crossref]

Appl. Phys. Lett. (2)

T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85(1), 25–27 (2004).
[Crossref]

I. Rocha-Mendoza, W. Langbein, and P. Borri, “Coherent anti-Stokes Raman microspectroscopy using spectral focusing with glass dispersion,” Appl. Phys. Lett. 93(20), 201103 (2008).
[Crossref]

Biophys. J. (1)

S. H. Parekh, Y. J. Lee, K. A. Aamer, and M. T. Cicerone, “Label-free cellular imaging by broadband coherent anti-Stokes Raman scattering microscopy,” Biophys. J. 99(8), 2695–2704 (2010).
[Crossref] [PubMed]

Curr. Pharm. Anal. (1)

B. D. Patel and P. J. Mehta, “An overview: application of Raman spectroscopy in pharmaceutical field,” Curr. Pharm. Anal. 6(2), 131–141 (2010).
[Crossref]

J. Opt. Soc. Am. B (1)

J. Phys. Chem. B (1)

J. Cheng, A. Volkmer, L. D. Book, and X. S. Xie, “An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscopy with high spectral resolution and high sensitivity,” J. Phys. Chem. B 105(7), 1277–1280 (2001).
[Crossref]

J. Raman Spectrosc. (2)

T. C. Bakker Schut, R. Wolthuis, P. J. Caspers, and G. J. Puppels, “Real-time tissue characterization on the basis of in vivo Raman spectra,” J. Raman Spectrosc. 33(7), 580–585 (2002).
[Crossref]

Y. X. Liu, Y. J. Lee, and M. T. Cicerone, “Fast extraction of resonant vibrational response from CARS spectra with arbitrary nonresonant background,” J. Raman Spectrosc. 40(7), 726–731 (2009).
[Crossref]

Laser Photon. Rev. (1)

J. Chan, S. Fore, S. Wachsmann-Hogiu, and T. Huser, “Raman spectroscopy and microscopy of individual cells and cellular components,” Laser Photon. Rev. 2(5), 325–349 (2008).
[Crossref]

N. J. Phys. (1)

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
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[Crossref]

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Figures (4)

Fig. 1
Fig. 1 Diagram of our coherent Raman setup. FI is a Faraday isolator, HWP are achromatic half waveplates, Pol. are Glan-laser polarizers, BS is a plate beam splitter, PCF is the photonic crystal fiber, EOM is the electro-optical modulator.

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Fig. 2
Fig. 2 CARS (a, blue), ME phase (b, red), retrieved Raman (c, green), and SRS (d, black) fingerprint region spectra of trans-stilbene. The CARS signal suffers from a non-resonant background that distorts the spectrum, making peak identification difficult. Maximum entropy phase extraction and removal of the estimated background phase produce a retrieved signal similar to the spontaneous Raman spectrum (inset). The SRS spectrum is an even closer match to the spontaneous Raman spectrum. Peak labels on the SRS spectrum are known vibrational modes.

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Fig. 3
Fig. 3 (a) Correlation between pump delay and vibrational frequency of known resonances demonstrating a linear dependence. (b) Lorenzian fit of several vibrational resonances to determine the spectral bandwidth.

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Fig. 4
Fig. 4 SRS and CARS images of polystyrene microspheres. a) and e) are at the maximum of the 1003 cm−1 resonance. b) and f) are red-shifted from the resonance peak by ~100 cm−1. c) and g) are blue-shifted to the minimum between resonances at 1003 and 1034 cm−1. d) and h) were recorded when the two beams were not temporally overlapped. Scale bar is 5 µm.

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