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

Autor:	Mead, Griffin, Lin, Haw-Wei, Magdău, Ioan-Bogdan, Miller III, Thomas F., Blake, Geoffrey A.
Rok vydání:	2020
Předmět:	Physics - Chemical Physics Physics - Optics
Druh dokumentu:	Working Paper
Popis:	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. Comment: Supplemental information available after main text
Databáze:	arXiv
Externí odkaz:	http://arxiv.org/abs/2007.08694 Zobrazit plný text záznamu View this record from Arxiv