Dispersion‐compensated supercontinuum generation for ultrabroadband multiplex coherent anti‐Stokes Raman scattering spectroscopy

We have generated a dispersion-compensated picosecond ultrabroadband supercontinuum light source at the sample position without using any additional compensator such as a prism pair or a grating pair. The dispersion-compensated supercontinuum, which is obtained just by optimizing the length of a photonic crystal fiber, has been used as a Stokes laser source for ultrabroadband multiplex coherent anti-Stokes Raman scattering (CARS) spectroscopy. Owing to an optimized temporal overlap between the narrowband pump and the Stokes supercontinuum pulses, a CARS signal has been obtained efficiently with a spectral coverage of more than 2800 cm−1. Furthermore, a vibrationally resonant CARS signal is observed not only when the pump pulse and the Stokes supercontinuum are temporally overlapped but also when the pump pulse follows the supercontinuum. It can be explained by an impulsive excitation of the vibrational coherence by the supercontinuum and a subsequent probe by a narrowband pump pulse. Using the dispersion-compensated supercontinuum, we can perform not only the frequency-domain multiplex CARS but also the time-domain impulsive CARS measurement by controlling the delay time between the narrowband laser and the supercontinuum. Both these techniques can be applied to microspectroscopy in order to obtain the wide spectral range of vibrational resonances and the suppression of the nonresonant background. Copyright © 2006 John Wiley & Sons, Ltd.

[1]  H. Hamaguchi,et al.  Near-infrared coherent anti-Stokes Raman scattering microscopy using supercontinuum generated from a photonic crystal fiber , 2005 .

[2]  J. Greve,et al.  Vibrational bands of luminescent zinc(II)-octaethylporphyrin using a polarization-sensitive microscopic multiplex CARS technique , 2001 .

[3]  W. R. Wiley,et al.  Three-Dimensional Vibrational Imaging by Coherent Anti-Stokes Raman Scattering , 1999 .

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

[5]  S. Kawata,et al.  Molecular vibration imaging in the fingerprint region by use of coherent anti-Stokes Raman scattering microscopy with a collinear configuration. , 2000, Optics letters.

[6]  H. Hamaguchi,et al.  Vibrationally resonant imaging of a single living cell by supercontinuum-based multiplex coherent anti-Stokes Raman scattering microspectroscopy. , 2005, Optics express.

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

[8]  Hiro-o Hamaguchi,et al.  Femtosecond coherent anti-Stokes Raman scattering spectroscopy using supercontinuum generated from a photonic crystal fiber , 2004 .

[9]  A. Zheltikov.  Limiting temporal and spectral resolution in spectroscopy and microscopy of coherent Raman scattering with chirped ultrashort laser pulses , 2005 .

[10]  U. I. Urbana-Champaign,et al.  Non-linear interferometric vibrational imaging , 2003, Conference on Lasers and Electro-Optics, 2003. CLEO '03..

[11]  H. Hamaguchi,et al.  Ultrabroadband (>2500cm−1) multiplex coherent anti-Stokes Raman scattering microspectroscopy using a supercontinuum generated from a photonic crystal fiber , 2005 .

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

[13]  Michiel Müller,et al.  Chemical specificity in three-dimensional imaging with multiplex coherent anti-Stokes Raman scattering microscopy. , 2002, Optics letters.

[14]  Gengfeng Zheng,et al.  Laser-scanning coherent anti-Stokes Raman scattering microscopy and applications to cell biology. , 2002, Biophysical journal.

[15]  Hiro-o Hamaguchi,et al.  Characterization of a supercontinuum generated from a photonic crystal fiber and its application to coherent Raman spectroscopy. , 2003, Optics letters.

[16]  Vladislav Yakovlev,et al.  Enhancing red-shifted white-light continuum generation in optical fibers for applications in nonlinear Raman microscopy. , 2005, Optics express.

[17]  J. Thøgersen,et al.  Coherent anti-Stokes Raman scattering microscopy with a photonic crystal fiber based light source , 2003, Conference on Lasers and Electro-Optics, 2003. CLEO '03..

[18]  Tak W. Kee,et al.  Simple approach to one-laser, broadband coherent anti-Stokes Raman scattering microscopy. , 2004, Optics letters.

[19]  All-optical processing in coherent nonlinear spectroscopy , 2004 .

[20]  Yaron Silberberg,et al.  Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy. , 2003, Physical review letters.

[21]  Juleon M. Schins,et al.  Direct measurement of chain order in single phospholipid mono- and bilayers with multiplex CARS , 2004 .

[22]  Aleksei M. Zheltikov,et al.  Microstructure fibers as frequency-tunable sources of ultrashort chirped pulses for coherent nonlinear spectroscopy , 2004 .

[23]  Rick Trebino,et al.  Cross-correlation frequency resolved optical gating analysis of broadband continuum generation in photonic crystal fiber: simulations and experiments. , 2002, Optics express.

[24]  Yaron Silberberg,et al.  Single-pulse phase-contrast nonlinear Raman spectroscopy. , 2002, Physical review letters.