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dc.contributor.authorAdamowicz, L.
dc.contributor.authorKvaal, S.
dc.contributor.authorLasser, C.
dc.contributor.authorPedersen, T.B.
dc.date.accessioned2022-11-23T18:21:16Z
dc.date.available2022-11-23T18:21:16Z
dc.date.issued2022
dc.identifier.citationAdamowicz, L., Kvaal, S., Lasser, C., & Pedersen, T. B. (2022). Laser-induced dynamic alignment of the HD molecule without the Born-Oppenheimer approximation. Journal of Chemical Physics, 157(14).
dc.identifier.issn0021-9606
dc.identifier.pmid36243530
dc.identifier.doi10.1063/5.0101352
dc.identifier.urihttp://hdl.handle.net/10150/666895
dc.description.abstractLaser-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 it hard to precisely define alignment. 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 while 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. © 2022 Author(s).
dc.language.isoen
dc.publisherAmerican Institute of Physics Inc.
dc.rightsCopyright © 2022 Author(s). Published under an exclusive license by AIP Publishing.
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/
dc.titleLaser-induced dynamic alignment of the HD molecule without the Born-Oppenheimer approximation
dc.typeArticle
dc.typetext
dc.contributor.departmentDepartment of Chemistry and Biochemistry, University of Arizona
dc.identifier.journalJournal of Chemical Physics
dc.description.note12 month embargo; published online: 10 October 2022
dc.description.collectioninformationThis item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at repository@u.library.arizona.edu.
dc.eprint.versionFinal published version
dc.source.journaltitleJournal of Chemical Physics


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