Compact and versatile laser system for polarization-sensitive stimulated Raman spectroscopy.

We demonstrate a compact and versatile laser system for stimulated Raman spectroscopy (SRS). The system is based on a tunable continuous wave (CW) probe laser combined with a home-built semi-monolithic nanosecond pulsed pump Nd:YVO4 laser at 1064 nm. The CW operation of the probe laser offers narrow linewidth, low noise and the advantage that temporal synchronization with the pump is not required. The laser system enables polarization-sensitive stimulated Raman spectroscopy (PS-SRS) with fast high resolution measurement of the depolarization ratio by simultaneous detection of Raman scattered light in orthogonal polarizations, thus providing information about the symmetry of the Raman-active vibrational modes. Measurements of the depolarization ratios of the carbon-hydrogen (CH) stretching modes in two different polymer samples in the spectral range of 2825-3025 cm-1 were performed. Raman spectra are obtained at a sweep rate of 20 nm/s (84 cm-1/s) with a resolution of 0.65 cm-1. A normalization method is introduced for the direct comparison of the simultaneously acquired orthogonal polarized Raman spectra.

[1]  W. Kiefer Recent advances in linear and non‐linear Raman spectroscopy. Part III , 2009 .

[2]  H. Rigneault,et al.  Molecular orientational order probed by coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS) microscopy: a spectral comparative study. , 2015, The journal of physical chemistry. B.

[3]  Wolfgang Wieser,et al.  A Time-Encoded Technique for fibre-based hyperspectral broadband stimulated Raman microscopy , 2014, Nature Communications.

[4]  Vincent Couderc,et al.  Observation of Raman optical activity by heterodyne-detected polarization-resolved coherent anti-Stokes Raman scattering. , 2012, Physical review letters.

[5]  W. Zinth,et al.  Femtosecond stimulated Raman microscopy , 2007 .

[6]  I. R. Lewis,et al.  Handbook of Raman Spectroscopy: From the Research Laboratory to the Process Line , 2001 .

[7]  T. Ishibashi,et al.  Polarization‐resolved coherent anti‐Stokes Raman scattering (CARS) spectroscopy: a new probe of molecular symmetry through accurate determination of the Raman depolarization ratio , 2000 .

[8]  M. Tanaka,et al.  Review Polarised Raman spectroscopy for the study of molecular orientation distributions in polymers , 2006 .

[9]  J. Koenig,et al.  Carbon–hydrogen stretching and bending vibrations in the Raman spectra of poly (methylmethacrylate) , 1980 .

[10]  Jan C Petersen,et al.  Differential high-resolution stimulated CW Raman spectroscopy of hydrogen in a hollow-core fiber. , 2015, Optics express.

[11]  H. Rigneault,et al.  Polarization resolved stimulated raman scattering: probing depolarization ratios of liquids , 2012 .

[12]  P. Hendra,et al.  The laser-Raman and infra-red spectra of poly(methyl methacrylate) , 1969 .

[13]  Wei Min,et al.  Highly specific label-free molecular imaging with spectrally tailored excitation stimulated Raman scattering (STE-SRS) microscopy. , 2011, Nature photonics.

[14]  X. Xie,et al.  Video-Rate Molecular Imaging in Vivo with Stimulated Raman Scattering , 2010, Science.

[15]  Theodor W. Hänsch,et al.  Coherent Raman spectro-imaging with laser frequency combs , 2013, Nature.

[16]  A. Smith,et al.  Vibrational Spectra of Me2SiCl2, Me3SiCl, Me3SiOSiMe3, (Me2SiO)3, (Me2SiO)4, (Me2SiO)x, and Their Deuterated Analogs , 1984 .

[17]  L. Jayes,et al.  Vibrational spectroscopic analysis of silicones: a Fourier transform-Raman and inelastic neutron scattering investigation. , 2003, Analytical chemistry.

[18]  Charles H. Camp,et al.  High-Speed Coherent Raman Fingerprint Imaging of Biological Tissues , 2014, Nature Photonics.

[19]  V. A. Apkarian,et al.  Seeing a single molecule vibrate through time-resolved coherent anti-Stokes Raman scattering , 2014, Nature Photonics.

[20]  W. Hug,et al.  A novel high-throughput Raman spectrometer for polarization difference measurements , 1999 .

[21]  R. Das,et al.  Raman spectroscopy: Recent advancements, techniques and applications , 2011 .

[22]  S. Mukamel,et al.  Theory of Coherent Raman Scattering , 2016 .

[23]  Laurence D. Barron,et al.  Vibrational optical activity , 2010 .

[24]  Kazuyoshi Itoh,et al.  High-speed molecular spectral imaging of tissue with stimulated Raman scattering , 2012, Nature Photonics.

[25]  Laurence D. Barron,et al.  Rayleigh and Raman scattering from optically active molecules , 1971 .

[26]  Delong Zhang,et al.  Coherent Raman Scattering Microscopy in Biology and Medicine. , 2015, Annual review of biomedical engineering.

[27]  Mortazavi,et al.  Supporting Online Material Materials and Methods Figs. S1 to S13 Tables S1 to S3 References Label-free Biomedical Imaging with High Sensitivity by Stimulated Raman Scattering Microscopy , 2022 .

[28]  Hervé Rigneault,et al.  Direct imaging of molecular symmetry by coherent anti-stokes Raman scattering , 2015, Nature Communications.