Facile Background Discrimination in Femtosecond Stimulated Raman Spectroscopy Using a Dual-Frequency Raman Pump Technique

Bera, Kajari; Kwang, Siu Yi; Cassabaum, Alyssa A.; Rich, Christopher C.; Frontiera, Renee R.

doi:10.1021/acs.jpca.9b02473

Facile Background Discrimination in Femtosecond Stimulated Raman Spectroscopy Using a Dual-Frequency Raman Pump Technique

Journal Article · Thu Sep 05 04:00:00 EDT 2019 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.9b02473· OSTI ID:1594946

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Univ. of Minnesota, Minneapolis, MN (United States); University of Minnesota, Minneapolis, MN (United States)
Univ. of Minnesota, Minneapolis, MN (United States)

Femtosecond stimulated Raman spectroscopy (FSRS) is a useful technique for uncovering chemical reaction dynamics by acquiring high-resolution Raman spectra with ultrafast time resolution. However, in FSRS, it can be challenging to discern Raman features from signals arising from transient absorption and other four-wave mixing pathways. To overcome this difficulty, we combine the principles of shifted excitation Raman difference spectroscopy with a simple fixed frequency comb to perform dual-frequency Raman pump FSRS. Through the addition of only two mirrors and a slit to the standard FSRS setup, this method provides Raman spectra at two different excitation wavelengths that can be processed by an automated algorithm to reconstruct the Raman spectrum. In this study, we demonstrate the utility of dual-frequency Raman pump FSRS to easily identify Raman signatures by visual inspection for excited-state and ground-state spectra, both on- and off-resonance. We show that previously assigned short-lived vibrations of photoexcited β-carotene are actually not vibrational in nature. We also use crystalline betaine-30 as a challenging test case for this method, as the FSRS spectra contain a number of narrow transient vibronic and non-SRS features. By reliably reducing interference from background signals, the interpretation is substantially more quantitative and enables the future study of new systems, particularly those with small Raman cross-sections or solid-state samples with narrow vibronic features.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Minnesota, Minneapolis, MN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)

Grant/Contract Number:: SC0018203

OSTI ID:: 1594946

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 37 Vol. 123; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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