Journal
JOURNAL OF PHYSICAL CHEMISTRY B
Volume 124, Issue 40, Pages 8904-8908Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.0c07935
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We demonstrate that halogenated methane (HM) two-dimensional (2D)-terahertz-terahertz-Raman (2D-TTR) spectra are determined by the complicated structure of the instrument response function (IRF) along omega(1) and by the molecular coherences along omega(2). Experimental improvements have helped increase the resolution and dynamic range of the measurements, including accurate THz pulse shape characterization. Sum-frequency excitations convolved with the IRF are found to quantitatively reproduce the 2D-TTR signal. A new reduced density matrix model that incorporates sum-frequency pathways, with linear and harmonic operators, fully supports this (re)interpretation of the 2D-TTR spectra.
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