Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy
Griffin Mead, Haw-Wei Lin, Ioan-Bogdan Magd\u{a}u, Thomas F. Miller, III, Geoffrey A. Blake
TL;DR
This paper advances understanding of 2D-Terahertz-Terahertz-Raman spectroscopy by analyzing the instrument response and molecular coherences, demonstrating that sum-frequency excitations explain the observed spectra.
Contribution
It introduces a new Reduced Density Matrix model incorporating sum-frequency pathways to interpret 2D-TTR spectra.
Findings
Sum-frequency excitations convolved with IRF reproduce 2D-TTR signals
Experimental improvements enhanced resolution and dynamic range
The new model supports the sum-frequency interpretation
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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