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Paper detail

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

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 $f_1$ and by the molecular coherences along $f_2$. 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 which incorporates sum-frequency pathways, with linear and harmonic operators fully supports this (re)interpretation of the 2D-TTR spectra.

preprint2020arXivOpen access
Griffin MeadHaw-Wei LinIoan-Bogdan MagdăuThomas F. Miller IIIGeoffrey A. Blake
physics.chem-phphysics.optics
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Griffin MeadHaw-Wei LinIoan-Bogdan MagdăuThomas F. Miller IIIGeoffrey A. Blake

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