OH-stretch vibrational relaxation of HOD in liquid to supercritical D2O

The Journal of Physical Chemistry. a
Dirk SchwarzerPeter Vöhringer

Abstract

The population relaxation of the OH-stretching vibration of HOD diluted in D2O is studied by time-resolved infrared (IR) pump-probe spectroscopy for temperatures of up to 700 K in the density range 12 <or= rho <or= 58 mol/L. For selected state points of the fluid solution, transient IR spectra were recorded following resonant excitation of the v = 0 --> 1 OH stretching transition with a 200 fs laser pulse centered at approximately 3500 cm(-1). Above 400 K these spectra show no indication of spectral diffusion after pump-probe delays of 0.3 ps. Over nearly the entire density range and for sufficiently high temperatures (T > 360 K), the vibrational relaxation rate constant, kr, is strictly proportional to the dielectric constant, epsilon, of water. Together with existing molecular dynamics simulations, this result suggests a simple linear dependence of kr on the number of hydrogen-bonded D2O molecules. It is shown that, for a given temperature, an isolated binary collision model is able to adequately describe the density dependence of vibrational energy relaxation even in hydrogen-bonded fluids. However, dynamic hydrogen bond breakage and formation is a source of spectral diffusion and affects the nature of the measured kr. For s...Continue Reading

References

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Citations

Jul 8, 2008·The Journal of Chemical Physics·Alexander KandratsenkaPeter Vöhringer
May 12, 2009·The Journal of Chemical Physics·Alexander KandratsenkaVyacheslav S Vikhrenko
Jun 15, 2011·The Journal of Chemical Physics·Martin OlschewskiPeter Vöhringer
Jan 10, 2012·The Journal of Chemical Physics·Takuma Yagasaki, Shinji Saito
Dec 2, 2009·The Journal of Chemical Physics·Adolfo BastidaBeatriz Miguel
Jun 18, 2009·The Journal of Chemical Physics·Tim SchäferDirk Schwarzer
Dec 19, 2012·Annual Review of Physical Chemistry·Takuma Yagasaki, Shinji Saito
Sep 16, 2008·Angewandte Chemie·Raluca MusatStanislas Pommeret
May 1, 2010·Physical Chemistry Chemical Physics : PCCP·Kresimir Franjic, Dwayne Miller
Aug 18, 2010·Physical Chemistry Chemical Physics : PCCP·Stephan KratzPeter Vöhringer
Mar 31, 2007·Physical Chemistry Chemical Physics : PCCP·Alexander KandratsenkaVyacheslav S Vikhrenko
Sep 24, 2009·Physical Chemistry Chemical Physics : PCCP·Jaane SeehusenPeter Vöhringer
Jan 25, 2011·Physical Chemistry Chemical Physics : PCCP·Stephan KnopPeter Vöhringer
Jul 25, 2012·Physical Chemistry Chemical Physics : PCCP·Tim SchäferDirk Schwarzer
Jan 5, 2017·The Journal of Chemical Physics·Beatriz MiguelAdolfo Bastida
Oct 2, 2008·The Journal of Physical Chemistry. B·Benjamin H Savitzky, Richard M Stratt
May 17, 2008·The Journal of Physical Chemistry. a·Tomotsumi FujisawaYoshifumi Kimura
Jan 19, 2007·The Journal of Physical Chemistry. a·Rene G RodriguezRichard Brey
Nov 17, 2010·The Journal of Physical Chemistry. a·Takuma YagasakiIwao Ohmine
Jan 26, 2012·The Journal of Physical Chemistry. B·Janus UrbanekPeter Vöhringer
Dec 1, 2010·The Journal of Physical Chemistry. B·Fivos Perakis, Peter Hamm
Jan 29, 2011·The Journal of Physical Chemistry. a·Martin OlschewskiPeter Vöhringer
Jun 30, 2019·Journal of the American Chemical Society·Karsten Heyne, Oliver Kühn
Dec 1, 2007·The Journal of Physical Chemistry. B·Dan CringusDouwe A Wiersma

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