Femtosecond photoexcitation dynamics inside a quantum solvent

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Abstract

The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here, we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.

Original languageEnglish
Article number4006
JournalNature Communications
Volume9
Issue number1
DOIs
Publication statusPublished - 1 Dec 2018

Fingerprint

Helium
Photoexcitation
photoexcitation
Solvation
solvation
helium
Superfluid helium
Indium
helium atoms
electronics
Excited states
Density functional theory
indium
Chemical reactions
Laser pulses
Spectrum Analysis
chemical reactions
Lasers
actuators
Doping (additives)

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

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title = "Femtosecond photoexcitation dynamics inside a quantum solvent",
abstract = "The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here, we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.",
author = "Bernhard Thaler and Sascha Ranftl and Pascal Heim and Stefan Cesnik and Leonhard Treiber and Ralf Meyer and Hauser, {Andreas W.} and Ernst, {Wolfgang E.} and Markus Koch",
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T1 - Femtosecond photoexcitation dynamics inside a quantum solvent

AU - Thaler, Bernhard

AU - Ranftl, Sascha

AU - Heim, Pascal

AU - Cesnik, Stefan

AU - Treiber, Leonhard

AU - Meyer, Ralf

AU - Hauser, Andreas W.

AU - Ernst, Wolfgang E.

AU - Koch, Markus

PY - 2018/12/1

Y1 - 2018/12/1

N2 - The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here, we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.

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