Cristin-resultat-ID: 2052201
Sist endret: 24. november 2022, 11:07
NVI-rapporteringsår: 2022
Resultat
Vitenskapelig artikkel
2022

Laser-induced dynamic alignment of the HD molecule without the Born-Oppenheimer approximation

Bidragsytere:
  • Ludwik Adamowicz
  • Simen Kvaal
  • Caroline Lasser og
  • Thomas Bondo Pedersen

Tidsskrift

Journal of Chemical Physics
ISSN 0021-9606
e-ISSN 1089-7690
NVI-nivå 1

Om resultatet

Vitenskapelig artikkel
Under utgivelse/in press
Publiseringsår: 2022
Publisert online: 2022
Trykket: 2022
Volum: 157
Hefte: 14
Artikkelnummer: 144302
Open Access

Importkilder

Scopus-ID: 2-s2.0-85139888209

Beskrivelse Beskrivelse

Tittel

Laser-induced dynamic alignment of the HD molecule without the Born-Oppenheimer approximation

Sammendrag

Laser-induced molecular alignment is well understood within the framework of the Born-Oppenheimer (BO) approximation. Without the BO approximation, however, the concept of molecular structure is lost, making alignment hard to define precisely. In this work, we demonstrate the emergence of alignment from the first-ever non-BO quantum dynamics simulations, using the HD molecule exposed to ultrashort laser pulses as a few-body test case. We extract the degree of alignment from the non-BO wave function by means of an operator expressed in terms of pseudo-proton coordinates that mimics the BO-based definition of alignment. The only essential approximation, in addition to the semiclassical electric-dipole approximation for the matter-field interaction, is the choice of time-independent explicitly correlated Gaussian basis functions. We use a variational, electric-field-dependent basis-set construction procedure, which allows us to keep the basis-set dimension low whilst capturing the main effects of electric polarization on the nuclear and electronic degrees of freedom. The basis-set construction procedure is validated by comparing with virtually exact grid-based simulations for two one-dimensional model systems: laser-driven electron dynamics in a soft attractive Coulomb potential and nuclear rovibrational dynamics in a Morse potential.

Bidragsytere

Ludwik Adamowicz

  • Tilknyttet:
    Forfatter
    ved University of Arizona

Simen Kvaal

  • Tilknyttet:
    Forfatter
    ved Teoretisk kjemi ved Universitetet i Oslo

Caroline Lasser

  • Tilknyttet:
    Forfatter
    ved Technische Universität München

Thomas Bondo Pedersen

  • Tilknyttet:
    Forfatter
    ved Teoretisk kjemi ved Universitetet i Oslo
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