Stimulated Raman phase shift spectroscopy: a pathway to hyperfine fingerprint spectra
The principle and experimental realization of a novel Raman spectroscopic technique entitled stimulated Raman phase shift (SRPS) spectroscopy was demonstrated. This technique depends on the measurement of the stimulated Raman scattering (SRS) induced phase shift of Stokes light field ($\Delta$ $\phi...
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Main Authors | , , , , |
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Format | Journal Article |
Language | English |
Published |
05.03.2024
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Subjects | |
Online Access | Get full text |
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Summary: | The principle and experimental realization of a novel Raman spectroscopic
technique entitled stimulated Raman phase shift (SRPS) spectroscopy was
demonstrated. This technique depends on the measurement of the stimulated Raman
scattering (SRS) induced phase shift of Stokes light field ($\Delta$ $\phi$)
that is related to the real part of the third order nonlinear susceptibility of
SRS. In principle, the spectral lineshape of 1/|$\Delta$ $\phi$| is a delta
function waveform, which is insensitive to the fluctuation of Stokes light
intensity, the decoherence of phonon in materials, as well as the inhomogeneous
fluorescence background. In order to measure 1/|$\Delta$ $\phi$|, a SRPS
including a Mach-Zender interferometer and a signal processing device was
developed. Using the developed spectrometer, the SRPS and stimulated Raman gain
(SRG) spectra of neat dimethyl sulfoxide were detected simultaneously. Seven
Raman peaks corresponding to specific molecule vibrational and rotational modes
were observed in the SRPS spectra, while only two peaks could be identified in
the SRG spectra without a priori knowledge. The linewidth of the Raman peak
centered at 2913.283 cm$^{-1}$ indicating the v$_s$(CH$_3$)stretching mode of
the methyl groups was less than 0.00036 cm$^{-1}$ in the measured SRPS spectra,
which was almost four orders of magnitude narrower than that in the measured
SRG spectra. Meanwhile, the detection signal-to-noise ratio of the Raman peak
centered at 2913.283 cm$^{-1}$ was 25.3 dB, representing an increase of 14.3 dB
compared to the SRG spectra. The reliability of SRPS technique was verified by
10 independent measurements, and the standard deviation of the Raman peak
frequency was less than $\pm$0.338 cm$^{-1}$ . The SRPS technique paves the way
for characterizing the hyperfine fingerprint of materials. |
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DOI: | 10.48550/arxiv.2403.03417 |