Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy
Chemical Physics
2020-07-20 v1 Optics
Abstract
We demonstrate that halogenated methane 2D-Terahertz Terahertz Raman (2D-TTR) spectra are determined by the complicated structure of the instrument response function (IRF) along and by the molecular coherences along . 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 which incorporates sum-frequency pathways, with linear and harmonic operators fully supports this (re)interpretation of the 2D-TTR spectra.
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Cite
@article{arxiv.2007.08694,
title = {Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy},
author = {Griffin Mead and Haw-Wei Lin and Ioan-Bogdan Magdău and Thomas F. Miller and Geoffrey A. Blake},
journal= {arXiv preprint arXiv:2007.08694},
year = {2020}
}
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