Abstract

We report chemical imaging using Fourier transform coherent anti-Stokes Raman scattering (FTCARS) microscopy. Adding a passively phase-stable local field to amplify the weak FTCARS signal, we also demonstrate interferometric FTCARS microscopy, permitting reduced incident power to be used for imaging. We discuss signal-to-noise considerations and the conditions necessary to effectively suppress background noise, allowing FTCARS microscopy that is limited by the shot noise of the detector. We also discuss differences between the signal-to-noise obtainable by time and frequency domain coherent anti-Stokes Raman scattering (CARS) methods.

© 2008 Optical Society of America

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    [CrossRef]
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    [CrossRef] [PubMed]

2008 (3)

B. C. Chen and S. H. Lim, “Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy,” J. Phys. Chem. B 112, 3653-3661 (2008).
[CrossRef] [PubMed]

F. Lu, W. Zheng, and Z. Huang, “Heterodyne polarization coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. Lett. 92, 123901 (2008).
[CrossRef]

Y. J. Lee and M. T. Cicerone, “Vibrational dephasing time imaging by time-resolved broadband coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. Lett. 92, 041108(2008).
[CrossRef]

2007 (4)

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, “Shot noise limited heterodyne detection of CARS signals,” Opt. Express 15, 15,207-15,213 (2007).
[CrossRef]

C. L. Evans, X. Y. Xu, S. Kesari, X. S. Xie, S. T. C. Wong, and G. S. Young, “Chemically-selective imaging of brain structures with CARS microscopy,” Opt. Express 15, 12,076-12,087(2007).
[CrossRef]

T. Hellerer, C. Axang, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, “Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy,” Proc. Natl. Acad. Sci. U.S.A. 104, 14,658-14,663(2007).
[CrossRef]

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

2006 (9)

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, “Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy,” J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, “High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses,” Opt. Lett. 31, 1543-1545 (2006).
[CrossRef] [PubMed]

E. O. Potma, C. L. Evans, and X. S. Xie, “Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging,” Opt. Lett. 31, 241-243 (2006).
[CrossRef] [PubMed]

J. P. Ogilvie, E. Beaurepaire, A. Alexandrou, and M. Joffre, “Fourier-transform coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 31, 480-482 (2006).
[CrossRef] [PubMed]

S. Nath, D. C. Urbanek, S. J. Kern, and M. A. Berg, “High-resolution Raman spectra with femtosecond pulses: An example of combined time- and frequency-domain spectroscopy,” Phys. Rev. Lett. 97, 267401 (2006).
[CrossRef]

E. R. Andresen, S. R. Keiding, and E. O. Potma, “Picosecond anti-Stokes generation in a photonic-crystal fiber for interferometric CARS microscopy,” Opt. Express 14, 7246-7251(2006).
[CrossRef] [PubMed]

M. Cui, M. Joffre, J. Skodack, and J. P. Ogilvie, “Interferometric Fourier transform coherent anti-Stokes Raman scattering,” Opt. Express 14, 8448-8458 (2006).
[CrossRef] [PubMed]

B. von Vacano, T. Buckup, and M. Motzkus, “Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering,” Opt. Lett. 31, 2495-2497 (2006).
[CrossRef] [PubMed]

T. W. Kee, H. X. Zhao, and M. T. Cicerone, “One-laser interferometric broadband coherent anti-Stokes Raman scattering,” Opt. Express 14, 3631-3640 (2006).
[CrossRef] [PubMed]

2005 (9)

D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
[CrossRef]

H. Kano and H. Hamaguchi, “Vibrationally resonant imaging of a single living cell by supercontinuum-based multiplex coherent anti-Stokes Raman scattering microspectroscopy,” Opt. Express 13, 1322-1327 (2005).
[CrossRef] [PubMed]

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, “High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

R. Porter, F. Shan, and T. Guo, “Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses,” Rev. Sci. Instrum. 76, 043108 (2005).
[CrossRef]

B. Yellampalle, R. D. Averitt, A. Efimov, and A. J. Taylor, “Spectral interferometric coherent Raman imaging,” Opt. Express 13, 7672-7682 (2005).
[CrossRef] [PubMed]

S.-H. Lim, A. G. Caster, and S. R. Leone, “Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy,” Phys. Rev. A 72, 041803 (2005).
[CrossRef]

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, “Coherent anti-stokes Raman scattering imaging of axonal myelin in live spinal tissues,” Biophys. J. 89, 581-591 (2005).
[CrossRef] [PubMed]

A. Volkmer, “Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy,” J. Phys. D: Appl. Phys. 38, R59-R81 (2005).
[CrossRef]

M. C. Fischer, T. Ye, G. Yurtsever, A. Miller, M. Ciocca, W. Wagner, and W. S. Warren, “Two-photon absorption and self-phase modulation measurements with shaped femtosecond laser pulses,” Opt. Lett. 30, 1551-1553(2005).
[CrossRef] [PubMed]

2004 (5)

K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, “High spectral resolution multiplex CARS spectroscopy using chirped pulses,” Chem. Phys. Lett. 387, 436-441 (2004).
[CrossRef]

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

T. W. Kee and M. T. Cicerone, “Simple approach to one-laser, broadband coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 29, 2701-2703 (2004).
[CrossRef] [PubMed]

C. L. Evans, E. O. Potma, and X. S. Xie, “Coherent anti-Stokes Raman scattering spectral interferometry: Determination of the real and imaginary components of nonlinear susceptibility (3) for vibrational microscopy,” Opt. Lett. 29, 2923-2925(2004).
[CrossRef]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, “Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes,” Appl. Phys. Lett. 85, 5787-5789(2004).
[CrossRef]

2003 (2)

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region,” J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

H. N. Paulsen, K. M. Hilligsoe, J. Thogersen, S. R. Keiding, and J. J. Larsen, “Coherent anti-Stokes Raman scattering microscopy with a photonic crystal fiber based light source,” Opt. Lett. 28, 1123-1125 (2003).
[CrossRef] [PubMed]

2002 (5)

J. X. Chen, A. Volkmer, L. D. Book, and X. S. Xie, “Multiplex coherent anti-Stokes Raman scattering microspectroscopy and study of lipid vesicles,” J. Phys. Chem. B 106, 8493-8498(2002).
[CrossRef]

M. Muller and J. M. Schins, “Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy,” J. Phys. Chem. B 106, 3715-3723 (2002).
[CrossRef]

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89, 273,001 (2002).
[CrossRef]

A. Volkmer, L. D. Book, and X. S. Xie, “Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay,” Appl. Phys. Lett. 80, 1505-1507(2002).
[CrossRef]

2001 (1)

1999 (2)

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

H. J. Koester, D. Baur, R. Uhl, and S. W. Hell, “Ca2+ fluorescence imaging with pico- and femtosecond two-photon excitation: Signal and photodamage,” Biophys. J. 77, 2226-2236(1999).
[CrossRef] [PubMed]

1997 (1)

R. Merlin, “Generating coherent THz phonons with light pulses,” Solid State Commun. 102, 207-220 (1997).
[CrossRef]

1995 (1)

1987 (1)

Y. X. Yan and K. A. Nelson, “Impulsive stimulated light-scattering. 2. Comparison to frequency-domain light-scattering spectroscopy,” J. Chem. Phys. 87, 6257-6265(1987).
[CrossRef]

1982 (1)

Akimov, D. A.

D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
[CrossRef]

Alexandrou, A.

Andresen, E. R.

Averitt, R. D.

Axang, C.

T. Hellerer, C. Axang, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, “Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy,” Proc. Natl. Acad. Sci. U.S.A. 104, 14,658-14,663(2007).
[CrossRef]

Baum, P.

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, “High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Baur, D.

H. J. Koester, D. Baur, R. Uhl, and S. W. Hell, “Ca2+ fluorescence imaging with pico- and femtosecond two-photon excitation: Signal and photodamage,” Biophys. J. 77, 2226-2236(1999).
[CrossRef] [PubMed]

Beaurepaire, E.

Berg, M. A.

S. Nath, D. C. Urbanek, S. J. Kern, and M. A. Berg, “High-resolution Raman spectra with femtosecond pulses: An example of combined time- and frequency-domain spectroscopy,” Phys. Rev. Lett. 97, 267401 (2006).
[CrossRef]

Bodermann, B.

M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, “High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. B 81, 875-879 (2005).
[CrossRef]

Bonn, 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,” Chem. Phys. Chem. 8, 279-287 (2007).
[CrossRef]

Book, L. D.

A. Volkmer, L. D. Book, and X. S. Xie, “Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay,” Appl. Phys. Lett. 80, 1505-1507(2002).
[CrossRef]

J. X. Chen, A. Volkmer, L. D. Book, and X. S. Xie, “Multiplex coherent anti-Stokes Raman scattering microspectroscopy and study of lipid vesicles,” J. Phys. Chem. B 106, 8493-8498(2002).
[CrossRef]

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

Boppart, S. A.

G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, “High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses,” Opt. Lett. 31, 1543-1545 (2006).
[CrossRef] [PubMed]

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, “Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes,” Appl. Phys. Lett. 85, 5787-5789(2004).
[CrossRef]

Brackmann, C.

T. Hellerer, C. Axang, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, “Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy,” Proc. Natl. Acad. Sci. U.S.A. 104, 14,658-14,663(2007).
[CrossRef]

Bredfeldt, J. S.

D. L. Marks, C. Vinegoni, J. S. Bredfeldt, and S. A. Boppart, “Interferometric differentiation between resonant and coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes,” Appl. Phys. Lett. 85, 5787-5789(2004).
[CrossRef]

Buckup, T.

Caster, A. G.

S. H. Lim, A. G. Caster, O. Nicolet, and S. R. Leone, “Chemical imaging by single pulse interferometric coherent anti-Stokes Raman scattering microscopy,” J. Phys. Chem. B 110, 5196-5204 (2006).
[CrossRef] [PubMed]

S.-H. Lim, A. G. Caster, and S. R. Leone, “Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy,” Phys. Rev. A 72, 041803 (2005).
[CrossRef]

Chen, B. C.

B. C. Chen and S. H. Lim, “Optimal laser pulse shaping for interferometric multiplex coherent anti-stokes Raman scattering microscopy,” J. Phys. Chem. B 112, 3653-3661 (2008).
[CrossRef] [PubMed]

Chen, J. X.

J. X. Chen, A. Volkmer, L. D. Book, and X. S. Xie, “Multiplex coherent anti-Stokes Raman scattering microspectroscopy and study of lipid vesicles,” J. Phys. Chem. B 106, 8493-8498(2002).
[CrossRef]

Cheng, J. X.

H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, “Coherent anti-stokes Raman scattering imaging of axonal myelin in live spinal tissues,” Biophys. J. 89, 581-591 (2005).
[CrossRef] [PubMed]

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

Cheriaux, G.

Cicerone, M. T.

Ciocca, M.

Cui, M.

Dudovich, N.

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region,” J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89, 273,001 (2002).
[CrossRef]

Duncan, M. D.

Efimov, A.

Enejder, A.

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K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, “High spectral resolution multiplex CARS spectroscopy using chirped pulses,” Chem. Phys. Lett. 387, 436-441 (2004).
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T. Hellerer, C. Axang, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, “Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy,” Proc. Natl. Acad. Sci. U.S.A. 104, 14,658-14,663(2007).
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R. Porter, F. Shan, and T. Guo, “Coherent anti-Stokes Raman scattering microscopy with spectrally tailored ultrafast pulses,” Rev. Sci. Instrum. 76, 043108 (2005).
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H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: The main lipid phase transition,” Chem. Phys. Chem. 8, 279-287 (2007).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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K. P. Knutsen, J. C. Johnson, A. E. Miller, P. B. Petersen, and R. J. Saykally, “High spectral resolution multiplex CARS spectroscopy using chirped pulses,” Chem. Phys. Lett. 387, 436-441 (2004).
[CrossRef]

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M. Muller and J. M. Schins, “Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy,” J. Phys. Chem. B 106, 3715-3723 (2002).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, “Coherent anti-stokes Raman scattering imaging of axonal myelin in live spinal tissues,” Biophys. J. 89, 581-591 (2005).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region,” J. Chem. Phys. 118, 9208-9215 (2003).
[CrossRef]

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, and Y. Silberberg, “Single-pulse phase-contrast nonlinear Raman spectroscopy,” Phys. Rev. Lett. 89, 273,001 (2002).
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D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14,976-14,981(2005).
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M. Greve, B. Bodermann, H. R. Telle, P. Baum, and E. Riedle, “High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. B 81, 875-879 (2005).
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H. J. Koester, D. Baur, R. Uhl, and S. W. Hell, “Ca2+ fluorescence imaging with pico- and femtosecond two-photon excitation: Signal and photodamage,” Biophys. J. 77, 2226-2236(1999).
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S. Nath, D. C. Urbanek, S. J. Kern, and M. A. Berg, “High-resolution Raman spectra with femtosecond pulses: An example of combined time- and frequency-domain spectroscopy,” Phys. Rev. Lett. 97, 267401 (2006).
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H. A. Rinia, M. Bonn, M. Muller, and E. M. Vartiainen, “Quantitative CARS spectroscopy using the maximum entropy method: The main lipid phase transition,” Chem. Phys. Chem. 8, 279-287 (2007).
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G. W. Jones, D. L. Marks, C. Vinegoni, and S. A. Boppart, “High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses,” Opt. Lett. 31, 1543-1545 (2006).
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H. F. Wang, Y. Fu, P. Zickmund, R. Y. Shi, and J. X. Cheng, “Coherent anti-stokes Raman scattering imaging of axonal myelin in live spinal tissues,” Biophys. J. 89, 581-591 (2005).
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C. L. Evans, X. Y. Xu, S. Kesari, X. S. Xie, S. T. C. Wong, and G. S. Young, “Chemically-selective imaging of brain structures with CARS microscopy,” Opt. Express 15, 12,076-12,087(2007).
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C. L. Evans, X. Y. Xu, S. Kesari, X. S. Xie, S. T. C. Wong, and G. S. Young, “Chemically-selective imaging of brain structures with CARS microscopy,” Opt. Express 15, 12,076-12,087(2007).
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Figures (8)

Fig. 1
Fig. 1

Energy diagram of (a) single mode (picosecond) CARS; (b) multiplex CARS; (c) FTCARS signal generation: an initial broadband pulse excites Raman coherences that are probed a delay τ later by a second broadband pulse. P: pump, S: Stokes, A: anti-Stokes.

Fig. 2
Fig. 2

(a) Experimental setup of standard FTCARS. The laser is a 12 fs Ti:sapphire oscillator centered at 790 nm . BS: beam splitter, LP: long-pass filter, SP: short-pass filter, Obj: objective lens. A He–Ne fringe tracking system (not shown) provides accurate monitoring of the time delay. For IFTCARS, the optical arrangement shown in (b) is added after the interferometer, and the long-pass filter (LP) is moved to filter the pump arm only. RM: return mirror, CM: curved mirror, gr: grating, ND: linear ND filter, EM: end mirror (Fourier plane), cg: compensation glass.

Fig. 3
Fig. 3

Time-domain data of 2-propanol using standard FTCARS spectroscopy. Incident pulse energies were 300 pJ and acquisition time was 1 s . The ratio of resonant to NR signal field is 1:20, as measured from the Fourier transform of the time-domain data.

Fig. 4
Fig. 4

(a) Nonresonant background image of 15 μm polystyrene beads in water ( 4 mW in each beam, 512 × 512 pixels, 10 μs exposure time per pixel); (b) FTCARS image of a single polystyrene bead from the sample shown in (a) ( 4 mW in each beam, 36 × 36 pixels, 7 ms exposure time per pixel, spectral resolution of 16 cm 1 ); (c) FTCARS spectrum from a single pixel within the bead in image (b).

Fig. 5
Fig. 5

FTCARS images of 15 μm polystyrene beads embedded in PMMA. The image is acquired with 4 mW power in each beam with a data acquisition time of 7 ms / pixel . The spectral resolution is 16 cm 1 . The top row of images show a maximum contribution from the PMMA near 820 cm 1 , while the lower row corresponds to the dominant polystyrene peak near 1000 cm 1 in agreement with the Raman reported spectra. The upper row has been multiplied by a factor of 4 to show the weaker PMMA signal on the same scale as the polystyrene.

Fig. 6
Fig. 6

(a) Line scan through a 4 μm polystyrene bead taken with IFTCARS. The image is acquired with 1 mW power in each beam with a data acquisition time of 4 s and spectral resolution of 16 cm 1 . (b) Corresponding standard FTCARS line scan (added LO is blocked). (c) Comparison of FTCARS spectra at pixel 75 in the two images.

Fig. 7
Fig. 7

Total noise versus LO power. Two regimes are clearly seen: a background noise regime ( LO < 1 pW ) and the shot noise regime ( LO < 100 pW ). The actual LO used in the interferometric FTCARS images shown in Fig. 6 is 38 pW as indicated. At very low excitation power where the NR background is small, standard FTCARS results in operation within the background noise regime, degrading the SNR.

Fig. 8
Fig. 8

(a) Dependence of the FTCARS resonant signal amplitude on the frequency of the CARS mode for different choices of the long-pass filter wavelength. (b) Dependence of the FTCARS resonant signal amplitude on the frequency of the CARS mode to be excited. Several different relative power ratios between pulses 1 and 2 ( P 1 / P 2 ) are shown.

Equations (2)

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I ( τ ) = I 1 + I local + I r 12 + 2 c I local I r 12 cos ( ϕ r 12 ( τ ) ϕ local ) ,
SNR = 2 c I local I r 12 a + b I < 2 c I r 12 b ,

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