Time-resolved dynamics in N2O4 probed using high harmonic generation

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DOIResolve DOI: http://doi.org/10.1126/science.1163077
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TypeArticle
Journal titleScience
ISSN0036-8075
Volume322
Issue5905
Pages12071211; # of pages: 5
AbstractThe attosecond time-scale electron-recollision process that underlies high harmonic generation has uncovered extremely rapid electronic dynamics in atoms and diatomics. We showed that high harmonic generation can reveal coupled electronic and nuclear dynamics in polyatomic molecules. By exciting large amplitude vibrations in dinitrogen tetraoxide, we showed that tunnel ionization accesses the ground state of the ion at the outer turning point of the vibration but populates the first excited state at the inner turning point. This state-switching mechanism is manifested as bursts of high harmonic light that is emitted mostly at the outer turning point. Theoretical calculations attribute the large modulation to suppressed emission from the first excited state of the ion. More broadly, these results show that high harmonic generation and strong-field ionization in polyatomic molecules undergoing bonding or configurational changes involve the participation of multiple molecular orbitals.
Publication date
LanguageEnglish
AffiliationNRC Steacie Institute for Molecular Sciences; National Research Council Canada
Peer reviewedYes
NPARC number21277112
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Record identifierb51703f0-2977-4fe1-9c56-37c6dc1f3aa0
Record created2015-12-02
Record modified2016-05-09
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