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. 2020 Oct 8;124(40):8904-8908.
doi: 10.1021/acs.jpcb.0c07935. Epub 2020 Sep 28.

Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy

Griffin Mead  1 , Haw-Wei Lin  1 , Ioan-Bogdan Magdău  1 , Thomas F Miller 3rd  1 , Geoffrey A Blake  1   2
Affiliations

Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy

Griffin Mead et al. J Phys Chem B. .

Abstract

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 ω1 and by the molecular coherences along ω2. 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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