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Appl. Sci. 2015, 5(2), 48-61; doi:10.3390/app5020048

Sum-Frequency-Generation-Based Laser Sidebands for Tunable Femtosecond Raman Spectroscopy in the Ultraviolet

1
Department of Chemistry and the Center for Sustainable Materials Chemistry, Oregon State University, 153 Gilbert Hall, Corvallis, OR 97331, USA
2
Department of Physics, Oregon State University, 301 Weniger Hall, Corvallis, OR 97331, USA
*
Author to whom correspondence should be addressed.
Academic Editor: Totaro Imasaka
Received: 11 March 2015 / Revised: 8 April 2015 / Accepted: 13 April 2015 / Published: 16 April 2015
View Full-Text   |   Download PDF [3368 KB, uploaded 16 April 2015]   |  

Abstract

Femtosecond stimulated Raman spectroscopy (FSRS) is an emerging molecular structural dynamics technique for functional materials characterization typically in the visible to near-IR range. To expand its applications we have developed a versatile FSRS setup in the ultraviolet region. We use the combination of a narrowband, ~400 nm Raman pump from a home-built second harmonic bandwidth compressor and a tunable broadband probe pulse from sum-frequency-generation-based cascaded four-wave mixing (SFG-CFWM) laser sidebands in a thin BBO crystal. The ground state Raman spectrum of a laser dye Quinolon 390 in methanol that strongly absorbs at ~355 nm is systematically studied as a standard sample to provide previously unavailable spectroscopic characterization in the vibrational domain. Both the Stokes and anti-Stokes Raman spectra can be collected by selecting different orders of SFG-CFWM sidebands as the probe pulse. The stimulated Raman gain with the 402 nm Raman pump is >21 times larger than that with the 550 nm Raman pump when measured at the 1317 cm−1 peak for the aromatic ring deformation and ring-H rocking mode of the dye molecule, demonstrating that pre-resonance enhancement is effectively achieved in the unique UV-FSRS setup. This added tunability in the versatile and compact optical setup enables FSRS to better capture transient conformational snapshots of photosensitive molecules that absorb in the UV range. View Full-Text
Keywords: femtosecond spectroscopy; four-wave mixing; tunable laser sidebands; stimulated Raman scattering; resonance enhancement; molecular vibrations femtosecond spectroscopy; four-wave mixing; tunable laser sidebands; stimulated Raman scattering; resonance enhancement; molecular vibrations
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (CC BY 4.0).

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MDPI and ACS Style

Zhu, L.; Liu, W.; Wang, Y.; Fang, C. Sum-Frequency-Generation-Based Laser Sidebands for Tunable Femtosecond Raman Spectroscopy in the Ultraviolet. Appl. Sci. 2015, 5, 48-61.

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