Dynamics of structural relaxation upon Rydberg excitation of an impurity in an Ar crystal

Sonia Jimenez; Alfredo Pasquarello; Roberto Car; Majed Chergui

doi:10.1016/S0301-0104(98)00154-2

Dynamics of structural relaxation upon Rydberg excitation of an impurity in an Ar crystal

Sonia Jimenez, Alfredo Pasquarello, Roberto Car, Majed Chergui

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Abstract

We study the ultrafast dynamics of structural relaxation induced by the Rydberg excitation of an NO molecule in an Ar crystal. We used classical molecular dynamics simulations and normal mode analysis to describe the dynamics of the cage of Ar atoms surrounding the NO molecule. The results show a behaviour characterized by an impulsive expansion of the cage radius at short times (≤ 250 fs), followed by multimodal oscillations over several picoseconds around a radius of ~4 Å. This corresponds to a dilatation of the ground state cage radius of ~9%. The dynamics show a high degree of nuclear vibrational coherence. The relaxation process is described by the damping of mainly five vibrational modes. Their frequencies range from 20 to 75 cm^-1 and correspond to resonant modes of the crystal. The associated lifetimes range from 0.5 to 16 ps. The mode of highest frequency being the most anharmonic.

Original language	English (US)
Pages (from-to)	343-352
Number of pages	10
Journal	Chemical Physics
Volume	233
Issue number	2-3
DOIs	https://doi.org/10.1016/S0301-0104(98)00154-2
State	Published - Aug 1 1998

All Science Journal Classification (ASJC) codes

Physics and Astronomy(all)
Physical and Theoretical Chemistry

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10.1016/S0301-0104(98)00154-2

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@article{58b993bbe1da4e088b9f4c3c89976669,

title = "Dynamics of structural relaxation upon Rydberg excitation of an impurity in an Ar crystal",

abstract = "We study the ultrafast dynamics of structural relaxation induced by the Rydberg excitation of an NO molecule in an Ar crystal. We used classical molecular dynamics simulations and normal mode analysis to describe the dynamics of the cage of Ar atoms surrounding the NO molecule. The results show a behaviour characterized by an impulsive expansion of the cage radius at short times (≤ 250 fs), followed by multimodal oscillations over several picoseconds around a radius of ~4 {\AA}. This corresponds to a dilatation of the ground state cage radius of ~9%. The dynamics show a high degree of nuclear vibrational coherence. The relaxation process is described by the damping of mainly five vibrational modes. Their frequencies range from 20 to 75 cm-1 and correspond to resonant modes of the crystal. The associated lifetimes range from 0.5 to 16 ps. The mode of highest frequency being the most anharmonic.",

author = "Sonia Jimenez and Alfredo Pasquarello and Roberto Car and Majed Chergui",

note = "Funding Information: We wish to thank Prof. J.-F. Loude for providing fitting programs and the referee for valuable suggestions. This work was supported by the Swiss National Science Foundation under grant N°21-47100.96. Most of the calculations were performed at the Swiss Center for Scientific Computing (CSCS) in Manno.",

year = "1998",

month = aug,

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doi = "10.1016/S0301-0104(98)00154-2",

language = "English (US)",

volume = "233",

pages = "343--352",

journal = "Chemical Physics",

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publisher = "Elsevier",

number = "2-3",

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TY - JOUR

T1 - Dynamics of structural relaxation upon Rydberg excitation of an impurity in an Ar crystal

AU - Jimenez, Sonia

AU - Pasquarello, Alfredo

AU - Car, Roberto

AU - Chergui, Majed

N1 - Funding Information: We wish to thank Prof. J.-F. Loude for providing fitting programs and the referee for valuable suggestions. This work was supported by the Swiss National Science Foundation under grant N°21-47100.96. Most of the calculations were performed at the Swiss Center for Scientific Computing (CSCS) in Manno.

PY - 1998/8/1

Y1 - 1998/8/1

N2 - We study the ultrafast dynamics of structural relaxation induced by the Rydberg excitation of an NO molecule in an Ar crystal. We used classical molecular dynamics simulations and normal mode analysis to describe the dynamics of the cage of Ar atoms surrounding the NO molecule. The results show a behaviour characterized by an impulsive expansion of the cage radius at short times (≤ 250 fs), followed by multimodal oscillations over several picoseconds around a radius of ~4 Å. This corresponds to a dilatation of the ground state cage radius of ~9%. The dynamics show a high degree of nuclear vibrational coherence. The relaxation process is described by the damping of mainly five vibrational modes. Their frequencies range from 20 to 75 cm-1 and correspond to resonant modes of the crystal. The associated lifetimes range from 0.5 to 16 ps. The mode of highest frequency being the most anharmonic.

AB - We study the ultrafast dynamics of structural relaxation induced by the Rydberg excitation of an NO molecule in an Ar crystal. We used classical molecular dynamics simulations and normal mode analysis to describe the dynamics of the cage of Ar atoms surrounding the NO molecule. The results show a behaviour characterized by an impulsive expansion of the cage radius at short times (≤ 250 fs), followed by multimodal oscillations over several picoseconds around a radius of ~4 Å. This corresponds to a dilatation of the ground state cage radius of ~9%. The dynamics show a high degree of nuclear vibrational coherence. The relaxation process is described by the damping of mainly five vibrational modes. Their frequencies range from 20 to 75 cm-1 and correspond to resonant modes of the crystal. The associated lifetimes range from 0.5 to 16 ps. The mode of highest frequency being the most anharmonic.

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U2 - 10.1016/S0301-0104(98)00154-2

DO - 10.1016/S0301-0104(98)00154-2

M3 - Article

AN - SCOPUS:0032381712

SN - 0301-0104

VL - 233

SP - 343

EP - 352

JO - Chemical Physics

JF - Chemical Physics

IS - 2-3

ER -

Dynamics of structural relaxation upon Rydberg excitation of an impurity in an Ar crystal

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