Two-dimensional measurements of the solvent structural relaxation dynamics in dipolar solvation

Physical Chemistry Chemical Physics : PCCP
Sungnam ParkNorbert F Scherer

Abstract

Resonant-pump polarizability response spectroscopy (RP-PORS) is based on an optical heterodyne detected transient grating (OHD-TG) method with an additional resonant pump pulse. In RP-PORS, the resonant pump pulse excites the solute-solvent system and the subsequent relaxation of the solute-solvent system is monitored by the OHD-TG spectroscopy. RP-PORS is shown to be an excellent experimental tool to directly measure the solvent responses in solvation. In the present work, we extended our previous RP-PORS (Park et al., Phys. Chem. Chem. Phys., 2011, 13, 214-223) to measure time-dependent transient solvation polarizability (TSP) spectra with Coumarin153 (C153) in acetonitrile. The time-dependent TSP spectra showed how the different solvent intermolecular modes were involved in different stages of the solvation process. Most importantly, the inertial and diffusive components of the solvent intermolecular modes in solvation were found to be spectrally and temporally well-separated. In a dipolar solvation of C153, high-frequency inertial solvent modes were found to be driven instantaneously and decay on a subpicosecond timescale while low-frequency diffusive solvent modes were induced slowly and decayed on a picosecond timescale. ...Continue Reading

References

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Nov 15, 2006·The Journal of Chemical Physics·Hemant K KashyapRanjit Biswas
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May 27, 2010·Chemical Society Reviews·Biman Bagchi, Biman Jana
Nov 26, 2010·Physical Chemistry Chemical Physics : PCCP·Sungnam ParkNorbert F Scherer

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Citations

Jul 24, 2014·The Journal of Chemical Physics·Luigi De MarcoAndrei Tokmakoff
Oct 3, 2015·The Journal of Chemical Physics·Zhenkun GuoAndrew M Moran
Sep 23, 2014·The Journal of Chemical Physics·Brian P MoleskyAndrew M Moran
Jun 8, 2015·The Journal of Chemical Physics·Brian P MoleskyAndrew M Moran
Jul 28, 2016·The Journal of Chemical Physics·Brian P MoleskyAndrew M Moran
Feb 7, 2017·Physical Chemistry Chemical Physics : PCCP·Dariusz Grzegorz Piekarski, Sergio Díaz-Tendero
Mar 16, 2018·Physical Chemistry Chemical Physics : PCCP·Esther HeidChristian Schröder
Nov 4, 2017·Topics in Current Chemistry·Zhenkun GuoAndrew M Moran
Sep 16, 2019·The Journal of Chemical Physics·Thomas P Cheshire, Andrew M Moran
Nov 17, 2016·The Journal of Chemical Physics·Brian P MoleskyAndrew M Moran
Oct 10, 2014·The Journal of Physical Chemistry. B·Xiang SunRichard M Stratt
Feb 5, 2013·Journal of the American Chemical Society·Jae Hyuk LeeHyotcherl Ihee
Mar 10, 2020·The Journal of Physical Chemistry. a·Richard ThurstonNiranjan Shivaram
Aug 31, 2021·Journal of the American Chemical Society·Hosung KiJeongho Kim

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