Coherent anti-stokes raman scattering spectral interferometry: determination of the real and imaginary components of nonlinear susceptibility chi(3) for vibrational microscopy.

We demonstrate coherent anti-Stokes Raman scattering (CARS) heterodyne spectral interferometry for retrieval of the real and imaginary components of the third-order nonlinear susceptibility (chi(3)) of molecular vibrations. Extraction of the imaginary component of chi(3) allows a straightforward reconstruction of the vibrationally resonant signal that is completely free of the electronic nonresonant background and resembles the spontaneous Raman spectrum. Heterodyne detection offers potential for signal amplification and enhanced sensitivity for CARS microscopy.

[1]  S. Boppart,et al.  Nonlinear optical contrast enhancement for optical coherence tomography. , 2003, Optics express.

[2]  Andreas Volkmer,et al.  Multiplex Coherent Anti-Stokes Raman Scattering Microspectroscopy and Study of Lipid Vesicles , 2002 .

[3]  Andreas Volkmer,et al.  Vibrational Imaging with High Sensitivity via Epidetected Coherent Anti-Stokes Raman Scattering Microscopy , 2001 .

[4]  B. Lax,et al.  Coherent cancellation of background in four‐wave mixing spectroscopy , 1980 .

[5]  B. Bouma,et al.  Improved signal-to-noise ratio in spectral-domain compared with time-domain optical coherence tomography. , 2003, Optics letters.

[6]  Manuel Joffre,et al.  Linear techniques of phase measurement by femtosecond spectral interferometry for applications in spectroscopy , 1995 .

[7]  X. Xie,et al.  Coherent Anti-Stokes Raman Scattering Microscopy: Instrumentation, Theory, and Applications , 2004 .

[8]  X. Xie,et al.  Polarization coherent anti-Stokes Raman scattering microscopy. , 2001, Optics letters.

[9]  X. Xie,et al.  Vibrational imaging of lipid droplets in live fibroblast cells with coherent anti-Stokes Raman scattering microscopy Published, JLR Papers in Press, August 16, 2003. DOI 10.1194/jlr.D300022-JLR200 , 2003, Journal of Lipid Research.

[10]  R. W. Hellwarth,et al.  Third-order optical susceptibilities of liquids and solids , 1977 .

[11]  Andreas Volkmer,et al.  Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay , 2002 .