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

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https://ir.library.oregonstate.edu/concern/articles/h415pc590

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  • 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.
  • This is the publisher’s final pdf. The published article is copyrighted by the author(s) and published by MDPI. The published article can be found at: http://www.mdpi.com/journal/applsci
  • Keywords: stimulated Raman scattering, tunable laser sidebands, four-wave mixing, resonance enhancement, molecular vibrations, femtosecond spectroscopy
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  • Zhu, L., Liu, W., Wang, Y., & Fang, C. (2015). Sum-Frequency-Generation-Based Laser Sidebands for Tunable Femtosecond Raman Spectroscopy in the Ultraviolet. Applied Sciences, 5(2), 48-61. doi:10.3390/app5020048
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  • 5
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  • 2
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  • This project is supported by the Oregon State University Faculty Startup Research Grant and Research Equipment Reserve Fund (to C.F.) and the National Science Foundation (NSF) CAREER award (grant number CHE-1455353, to C.F. since Feb. 2015). We also acknowledge graduate research assistantship (to L.Z.) from the NSF Center for Sustainable Materials Chemistry (grant number CHE-1102637)
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