Femtosecond CARS of Binary Liquid Mixtures: Dephasing via Concentration Fluctuations in the Intermediate Regime

F. Lindenberger; R. Stöckl; B. P. Asthana; A. Laubereau

doi:10.1021/jp991228f

Femtosecond CARS of Binary Liquid Mixtures: Dephasing via Concentration Fluctuations in the Intermediate Regime

F. Lindenberger, R. Stöckl, B. P. Asthana, A. Laubereau

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Publikation: Beitrag in Fachzeitschrift › Artikel › Begutachtung

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Abstract

The symmetric CH₃-stretching mode v₁ of CH₃I is investigated in a solution of CDCl₃ in the concentration range 7-100% and temperature interval 242-374 K using time-resolved coherent anti-Stokes Raman scattering (CARS) with 250 fs pulses and magic polarization geometries. Striking deviations from simple exponential relaxation dynamics are reported for mixtures with mole fractions around 0.5. Analysis of the concentration dependence allows to distinguish the dephasing contribution of concentration fluctuations with correlation time >1 ps, indicating the intermediate case for this relaxation mechanism. The results are well described by the Knapp-Fischer model for concentration fluctuations, yielding a molecular residence time in the solvation layer of 1.1-3.2 ps in the temperature range 242-374 K in accordance with theoretical estimates.

Originalsprache	Englisch
Seiten (von - bis)	5655-5660
Seitenumfang	6
Fachzeitschrift	Journal of Physical Chemistry A
Jahrgang	103
Ausgabenummer	29
DOIs	https://doi.org/10.1021/jp991228f
Publikationsstatus	Veröffentlicht - 22 Juli 1999

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title = "Femtosecond CARS of Binary Liquid Mixtures: Dephasing via Concentration Fluctuations in the Intermediate Regime",

abstract = "The symmetric CH3-stretching mode v1 of CH3I is investigated in a solution of CDCl3 in the concentration range 7-100% and temperature interval 242-374 K using time-resolved coherent anti-Stokes Raman scattering (CARS) with 250 fs pulses and magic polarization geometries. Striking deviations from simple exponential relaxation dynamics are reported for mixtures with mole fractions around 0.5. Analysis of the concentration dependence allows to distinguish the dephasing contribution of concentration fluctuations with correlation time >1 ps, indicating the intermediate case for this relaxation mechanism. The results are well described by the Knapp-Fischer model for concentration fluctuations, yielding a molecular residence time in the solvation layer of 1.1-3.2 ps in the temperature range 242-374 K in accordance with theoretical estimates.",

author = "F. Lindenberger and R. St{\"o}ckl and Asthana, {B. P.} and A. Laubereau",

year = "1999",

month = jul,

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doi = "10.1021/jp991228f",

language = "English",

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journal = "Journal of Physical Chemistry A",

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TY - JOUR

T1 - Femtosecond CARS of Binary Liquid Mixtures

T2 - Dephasing via Concentration Fluctuations in the Intermediate Regime

AU - Lindenberger, F.

AU - Stöckl, R.

AU - Asthana, B. P.

AU - Laubereau, A.

PY - 1999/7/22

Y1 - 1999/7/22

N2 - The symmetric CH3-stretching mode v1 of CH3I is investigated in a solution of CDCl3 in the concentration range 7-100% and temperature interval 242-374 K using time-resolved coherent anti-Stokes Raman scattering (CARS) with 250 fs pulses and magic polarization geometries. Striking deviations from simple exponential relaxation dynamics are reported for mixtures with mole fractions around 0.5. Analysis of the concentration dependence allows to distinguish the dephasing contribution of concentration fluctuations with correlation time >1 ps, indicating the intermediate case for this relaxation mechanism. The results are well described by the Knapp-Fischer model for concentration fluctuations, yielding a molecular residence time in the solvation layer of 1.1-3.2 ps in the temperature range 242-374 K in accordance with theoretical estimates.

AB - The symmetric CH3-stretching mode v1 of CH3I is investigated in a solution of CDCl3 in the concentration range 7-100% and temperature interval 242-374 K using time-resolved coherent anti-Stokes Raman scattering (CARS) with 250 fs pulses and magic polarization geometries. Striking deviations from simple exponential relaxation dynamics are reported for mixtures with mole fractions around 0.5. Analysis of the concentration dependence allows to distinguish the dephasing contribution of concentration fluctuations with correlation time >1 ps, indicating the intermediate case for this relaxation mechanism. The results are well described by the Knapp-Fischer model for concentration fluctuations, yielding a molecular residence time in the solvation layer of 1.1-3.2 ps in the temperature range 242-374 K in accordance with theoretical estimates.

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JO - Journal of Physical Chemistry A

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Femtosecond CARS of Binary Liquid Mixtures: Dephasing via Concentration Fluctuations in the Intermediate Regime

Abstract

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