Ultrafast dephasing in hydrogen-bonded pyridine–water mixtures release_utzqzv7ldfggbbmq3aawmgofum

by Gombojav O. Ariunbold, Bryan Semon, Supriya Nagpal, Yuri Rostovtsev

Published in Open Physics by Walter de Gruyter GmbH.

2021   Volume 19, p234-240

Abstract

<jats:title>Abstract</jats:title> Hydrogen-bonded mixtures with varying concentration are a complicated networked system that demands a detection technique with both time and frequency resolutions. Hydrogen-bonded pyridine–water mixtures are studied by a time-frequency resolved coherent Raman spectroscopic technique. Femtosecond broadband dual-pulse excitation and delayed picosecond probing provide sub-picosecond time resolution in the mixtures temporal evolution. For different pyridine concentrations in water, asymmetric blue versus red shifts (relative to pure pyridine spectral peaks) were observed by simultaneously recording both the coherent anti-Stokes and Stokes Raman spectra. Macroscopic coherence dephasing times for the perturbed pyridine ring modes were observed in ranges of 0.9–2.6 ps for both 18 and <jats:inline-formula> <jats:alternatives> <jats:inline-graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="graphic/j_phys-2021-0027_eq_001.png" /> <m:math xmlns:m="http://www.w3.org/1998/Math/MathML"> <m:mn>10</m:mn> <m:mspace width="0.33em" /> <m:msup> <m:mrow> <m:mi mathvariant="normal">cm</m:mi> </m:mrow> <m:mrow> <m:mo>−</m:mo> <m:mn>1</m:mn> </m:mrow> </m:msup> </m:math> <jats:tex-math>10\hspace{0.33em}{{\rm{cm}}}^{-1}</jats:tex-math> </jats:alternatives> </jats:inline-formula> broad probe pulses. For high pyridine concentrations in water, an additional spectral broadening (or escalated dephasing) for a triangular ring vibrational mode was observed. This can be understood as a result of ultrafast collective emissions from coherently excited ensemble of pairs of pyridine molecules bound to water molecules.
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