Ultrafast vibrational relaxation and energy dissipation of hydrated excess protons in polar solvents

Achintya Kundu; Fabian Dahms; Benjamin P. Fingerhut; Erik T.J. Nibbering; Ehud Pines; Thomas Elsaesser

doi:10.1016/j.cplett.2018.10.030

Ultrafast vibrational relaxation and energy dissipation of hydrated excess protons in polar solvents

Achintya Kundu, Fabian Dahms, Benjamin P. Fingerhut, Erik T.J. Nibbering, Ehud Pines, Thomas Elsaesser

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

6 Scopus citations

Abstract

Vibrational relaxation and energy redistribution of Zundel cations H₅O₂ ⁺ in acetonitrile and neat water are studied by femtosecond infrared pump-probe spectroscopy with resonant excitation of the 1200 cm⁻¹ proton transfer mode. Transient spectra in a range from 1000 to 2200 cm⁻¹ reveal intermode anharmonic couplings and a sub-100 fs decay of the proton transfer mode, followed by femtosecond vibrational redistribution within the cations’ vibrational manifold and picosecond energy transfer to the solvent. Energy transfer to an aqueous environment occurs on the same time scale as within neat water, demonstrating the strong coupling of cations and water solvation shell.

Original language	English
Pages (from-to)	111-116
Number of pages	6
Journal	Chemical Physics Letters
Volume	713
DOIs	https://doi.org/10.1016/j.cplett.2018.10.030
State	Published - 1 Dec 2018

Keywords

Femtosecond infrared spectroscopy
Hydrated excess proton
Solvation
Vibrational relaxation

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1016/j.cplett.2018.10.030

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title = "Ultrafast vibrational relaxation and energy dissipation of hydrated excess protons in polar solvents",

abstract = "Vibrational relaxation and energy redistribution of Zundel cations H5O2 + in acetonitrile and neat water are studied by femtosecond infrared pump-probe spectroscopy with resonant excitation of the 1200 cm−1 proton transfer mode. Transient spectra in a range from 1000 to 2200 cm−1 reveal intermode anharmonic couplings and a sub-100 fs decay of the proton transfer mode, followed by femtosecond vibrational redistribution within the cations{\textquoteright} vibrational manifold and picosecond energy transfer to the solvent. Energy transfer to an aqueous environment occurs on the same time scale as within neat water, demonstrating the strong coupling of cations and water solvation shell.",

keywords = "Femtosecond infrared spectroscopy, Hydrated excess proton, Solvation, Vibrational relaxation",

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T1 - Ultrafast vibrational relaxation and energy dissipation of hydrated excess protons in polar solvents

AU - Kundu, Achintya

AU - Dahms, Fabian

AU - Fingerhut, Benjamin P.

AU - Nibbering, Erik T.J.

AU - Pines, Ehud

AU - Elsaesser, Thomas

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Vibrational relaxation and energy redistribution of Zundel cations H5O2 + in acetonitrile and neat water are studied by femtosecond infrared pump-probe spectroscopy with resonant excitation of the 1200 cm−1 proton transfer mode. Transient spectra in a range from 1000 to 2200 cm−1 reveal intermode anharmonic couplings and a sub-100 fs decay of the proton transfer mode, followed by femtosecond vibrational redistribution within the cations’ vibrational manifold and picosecond energy transfer to the solvent. Energy transfer to an aqueous environment occurs on the same time scale as within neat water, demonstrating the strong coupling of cations and water solvation shell.

AB - Vibrational relaxation and energy redistribution of Zundel cations H5O2 + in acetonitrile and neat water are studied by femtosecond infrared pump-probe spectroscopy with resonant excitation of the 1200 cm−1 proton transfer mode. Transient spectra in a range from 1000 to 2200 cm−1 reveal intermode anharmonic couplings and a sub-100 fs decay of the proton transfer mode, followed by femtosecond vibrational redistribution within the cations’ vibrational manifold and picosecond energy transfer to the solvent. Energy transfer to an aqueous environment occurs on the same time scale as within neat water, demonstrating the strong coupling of cations and water solvation shell.

KW - Femtosecond infrared spectroscopy

KW - Hydrated excess proton

KW - Solvation

KW - Vibrational relaxation

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DO - 10.1016/j.cplett.2018.10.030

M3 - Article

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SP - 111

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JO - Chemical Physics Letters

JF - Chemical Physics Letters

ER -

Ultrafast vibrational relaxation and energy dissipation of hydrated excess protons in polar solvents

Abstract

Keywords

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