Abstract

In this article we show that heterodyne CARS, based on a controlled and stable phase-preserving chain, can be used to measure amplitude and phase information of molecular vibration modes. The technique is validated by a comparison of the imaginary part of the heterodyne CARS spectrum to the spontaneous Raman spectrum of polyethylene. The detection of the phase allows for rejection of the non-resonant background from the data. The resulting improvement of the signal to noise ratio is shown by measurements on a sample containing lipid.

© 2008 Optical Society of America

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  1. X. Nan, E. Potma, and X. S. Xie, "Nonperturbabtive chemical imaging of organelle transport in living cells with CARS microscopy," Biophys. J. 91, 728-735 (2006).
    [CrossRef] [PubMed]
  2. T. B. Huff and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
    [CrossRef] [PubMed]
  3. T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
    [CrossRef] [PubMed]
  4. M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
    [CrossRef]
  5. C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
    [CrossRef] [PubMed]
  6. J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 19, 1363-1375 (2002).
    [CrossRef]
  7. 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]
  8. S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).
  9. A. Volkmer, J. X. Cheng, and X. S. Xie, "Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy," Phys. Rev. Lett. 87, 023901 (2001).
    [CrossRef]
  10. 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, 1872-1874 (2006).
    [CrossRef] [PubMed]
  11. Y. S. Yoo, D. H. Lee, and H. Cho, "Differential two-signal picosecond-pulse coherent anti-Stokes Raman scattering imaging microscopy by using a dual-mode optical parametric oscillator," Opt. Lett. 32, 3254-3256 (2007).
    [CrossRef] [PubMed]
  12. 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 (2002).
    [CrossRef]
  13. W. P. de Boeij, H. S. Kanger, G. W. Lucassen, C. Otto, and J. Greve, "Waveguide CARS Spectroscopy: A New Method for Background Suppression, Using Dielectric Layers as a Model," Appl. Spectrosc. 47, 723-730 (1993).
    [CrossRef]
  14. V. V. Krishnamachari and E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering: A numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007).
    [CrossRef]
  15. M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
    [CrossRef] [PubMed]
  16. M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
    [CrossRef]

2008 (1)

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

2007 (5)

V. V. Krishnamachari and E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering: A numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007).
[CrossRef]

Y. S. Yoo, D. H. Lee, and H. Cho, "Differential two-signal picosecond-pulse coherent anti-Stokes Raman scattering imaging microscopy by using a dual-mode optical parametric oscillator," Opt. Lett. 32, 3254-3256 (2007).
[CrossRef] [PubMed]

T. B. Huff and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
[CrossRef] [PubMed]

2006 (4)

X. Nan, E. Potma, and X. S. Xie, "Nonperturbabtive chemical imaging of organelle transport in living cells with CARS microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
[CrossRef]

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]

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, 1872-1874 (2006).
[CrossRef] [PubMed]

2005 (1)

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

2002 (2)

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 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 19, 1363-1375 (2002).
[CrossRef]

2001 (1)

A. Volkmer, J. X. Cheng, and X. S. Xie, "Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy," Phys. Rev. Lett. 87, 023901 (2001).
[CrossRef]

1993 (1)

1978 (1)

S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).

Akhmanov, S. A.

S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).

Axäng, C.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

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 (2002).
[CrossRef]

Brackmann, C.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

Bunkin, A. F.

S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).

Cheng, J. X.

T. B. Huff and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 19, 1363-1375 (2002).
[CrossRef]

A. Volkmer, J. X. Cheng, and X. S. Xie, "Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy," Phys. Rev. Lett. 87, 023901 (2001).
[CrossRef]

Cho, H.

Cote, D.

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

de Boeij, W. P.

Enejder, A.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

Evans, C. L.

Ganikhanov, F.

Greve, J.

Hellerer, T.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

Hillertz, P.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

Huff, T. B.

T. B. Huff and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

Ivanov, S. G.

S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).

Jurna, M.

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
[CrossRef]

Kanger, H. S.

Koroteev, N. I.

S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).

Korterik, J. P.

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
[CrossRef]

Krishnamachari, V. V.

Lee, D. H.

Lin, C. P.

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Lucassen, G. W.

Nan, X.

X. Nan, E. Potma, and X. S. Xie, "Nonperturbabtive chemical imaging of organelle transport in living cells with CARS microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

Offerhaus, H. L.

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
[CrossRef]

Otto, C.

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
[CrossRef] [PubMed]

M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
[CrossRef]

W. P. de Boeij, H. S. Kanger, G. W. Lucassen, C. Otto, and J. Greve, "Waveguide CARS Spectroscopy: A New Method for Background Suppression, Using Dielectric Layers as a Model," Appl. Spectrosc. 47, 723-730 (1993).
[CrossRef]

Pilon, M.

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

Potma, E.

X. Nan, E. Potma, and X. S. Xie, "Nonperturbabtive chemical imaging of organelle transport in living cells with CARS microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

Potma, E. O.

V. V. Krishnamachari and E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering: A numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007).
[CrossRef]

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]

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Puoris'haag, M.

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Rimke, I.

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

Saar, B. G.

Volkmer, A.

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 (2002).
[CrossRef]

J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 19, 1363-1375 (2002).
[CrossRef]

A. Volkmer, J. X. Cheng, and X. S. Xie, "Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy," Phys. Rev. Lett. 87, 023901 (2001).
[CrossRef]

Xie, X. S.

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, 1872-1874 (2006).
[CrossRef] [PubMed]

X. Nan, E. Potma, and X. S. Xie, "Nonperturbabtive chemical imaging of organelle transport in living cells with CARS microscopy," Biophys. J. 91, 728-735 (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]

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 19, 1363-1375 (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 (2002).
[CrossRef]

A. Volkmer, J. X. Cheng, and X. S. Xie, "Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy," Phys. Rev. Lett. 87, 023901 (2001).
[CrossRef]

Yoo, Y. S.

Appl. Phys. Lett. (2)

M. Jurna, J. P. Korterik, H. L. Offerhaus, and C. Otto, "Noncritical phase-matched lithium triborate optical parametric oscillator for high resolution coherent anti-Stokes Raman scattering spectroscopy and microscopy," Appl. Phys. Lett. 89, 251116 (2006).
[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 (2002).
[CrossRef]

Appl. Spectrosc. (1)

Biophys. J. (1)

X. Nan, E. Potma, and X. S. Xie, "Nonperturbabtive chemical imaging of organelle transport in living cells with CARS microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

J. Microsc. (1)

T. B. Huff and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

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

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

Opt. Express. (1)

M. Jurna, J. P. Korterik, C. Otto, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Opt. Express. 15, 15207-15213 (2007).
[CrossRef] [PubMed]

Opt. Lett. (3)

Phys. Rev. Lett. (1)

A. Volkmer, J. X. Cheng, and X. S. Xie, "Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy," Phys. Rev. Lett. 87, 023901 (2001).
[CrossRef]

PNAS (1)

T. Hellerer, C. Axäng, C. Brackmann, P. Hillertz, M. Pilon, and A. Enejder, "Monitoring of lipid storage in Caenorhabditis elegans using coherent anti-Stokes Raman scattering (CARS) microscopy," PNAS 104, 14658-14663 (2007).
[CrossRef] [PubMed]

Proc. Natl. Acad. Sci. USA (1)

C. L. Evans, E. O. Potma, M. Puoris'haag, D. Cote, C. P. Lin, and X. S. Xie, "Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. USA 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Proc. SPIE (1)

M. Jurna, E. Büttner, J. P. Korterik, C. Otto, I. Rimke, and H. L. Offerhaus, "Shot noise limited heterodyne detection of CARS signals," Proc. SPIE 6860, 68600R (2008).
[CrossRef]

Sov.Phys. JETP (1)

S. A. Akhmanov, A. F. Bunkin, S. G. Ivanov, and N. I. Koroteev, "Polarization active Raman spectroscopy and coherent Raman ellipsometry," Sov.Phys. JETP 47, 667 (1978).

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Figures (4)

Fig. 1.
Fig. 1.

Energy diagram showing the optical chain for the phase-preserved generation of the wavelengths for the CARS process and Local Oscillator.

Fig. 2.
Fig. 2.

Schematic of sample used for spectroscopic measurement of amplitude and phase.

Fig. 3.
Fig. 3.

(a) The CARS amplitude spectrum of the resonant PE (blue circles) and the associated phase of the spectrum (green squares). The symbols are data and the solid curves are fits based on multiple Lorenzian bands as in Eq. (1). (b) The red dotted line is the spontaneous Raman spectrum of PE and in the blue the Imχ (3) R (ω) of the data in panel A is shown.

Fig. 4.
Fig. 4.

The sample (35×35µm) contains lipid suspended in agarose gel imaged at 2845 cm-1. (a) Forward intensity CARS image obtained with 1064nm (pump and probe) and idler (Stokes). (b) Amplitude image obtained with heterodyne CARS. (c) Phase image obtained with heterodyne CARS. (d) Im χ (3) R , the non-resonant free image of the sample. (e-h) Cross sections of the image above at the thin line at the bottom.

Equations (4)

Equations on this page are rendered with MathJax. Learn more.

χ R ( 3 ) ( ω ) Ω k ( a k Ω k ω i Γ k ) ,
I Raman ( ω ) I m χ R ( 3 ) ( ω ) .
I CARS ( ω ) χ R ( 3 ) ( ω ) + χ NR ( 3 ) 2 .
I detector = I LO + I AS + 2 I LO I AS { [ χ NR ( 3 ) + Re ( χ R ( 3 ) ) ] cos ϕ + [ Im ( χ R ( 3 ) ) ] sin ϕ } ,

Metrics