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Title:Polarization Control Of Rotationally Resolved 2dir Spectroscopy
Author(s):Kowzan, Grzegorz
Contributor(s):Allison, Thomas K; Lewis, Neomi; Silfies, Myles C
Subject(s):Instrument/Technique Demonstration
Abstract:\begin{wrapfigure}{r}{0pt} \includegraphics[scale=0.85]{polctrl.eps} \end{wrapfigure} Detection of trace amounts of molecules in multi-species mixtures is important for many purposes, ranging from chemical dynamics in complex environments to breath analysis. 2DIR spectroscopy is a powerful tool for studying both molecular structure and dynamics. It can provide better selectivity than linear spectroscopy due to the extra degrees of freedom for distinguishing the components of a complex mixture, but its application to trace-gas detection has been hindered by insufficient sensitivity and resolution of the technique. Cavity-enhancement methods for ultrafast nonlinear spectroscopy using frequency combs have the potential to overcome this problem\footnote{T. K. Allison. J. Phys. B 50, 044004 (2017).}. In 2DIR spectroscopy of coupled vibrational modes, it is common to use specific beam polarization angles to suppress parts of the molecular response and simplify structure determination\footnote{M. T. Zanni, N. Ge, Y. S. Kim, R. M. Hochstrasser. Proc. Nat. Acad. Sci. 98, 11265 (2001).}. Here we show how to suppress parts of the rotational response of a single vibrational mode. We provide specific polarization angles that suppress diagonal or antidiagonal peaks, or the pathways with interstate coherences after the second excitation. We present simulations for carbon monoxide that demonstrate the effect of eliminating specific pathways on 2DIR rotationally-resolved spectra. \phantom{\footnote{Supported by U.S. National Science Foundation award 1708743, U.S. Air Force Office of Scientific\\ Research grant FA9550-20-1-0259. M. C. Silfies supported by the GAANN program of U.S. Dept. of Education.\\ G. Kowzan supported by National Science Center, Poland scholarship 2017/24/T/ST2/00242.}}
Issue Date:2021-06-23
Publisher:International Symposium on Molecular Spectroscopy
Genre:Conference Paper / Presentation
Date Available in IDEALS:2021-09-24

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