Nuclear Dynamics in Polyatomic Molecules and High-Order Harmonic Generation

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DOIResolve DOI: http://doi.org/10.1103/PhysRevLett.102.253602
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TypeArticle
Journal titlePhysical Review Letters
Volume102
Issue25
SubjectNuclear Dynamics; polyatomic molecules; high-order harmonic generation; nuclear vibrational wave function; emission intensity
AbstractHigh-order harmonic generation in molecular gases is accompanied by short-time evolution of the nuclear vibrational wave function. Using normal coordinate representation, I derive a simple analytical theory of short-time autocorrelation functions and apply it to a test set of 15 small molecules. The results explain large isotope effects observed in CH4. At the harmonic cutoff in 800 nm driving field, nuclear dynamics reduces the emission intensity from NO and NO2 molecules by more than 50%. Autocorrelation functions are sensitive to the initial vibrational state, with the nodal structure of the initial vibrational wave packet reflected in the frequency spectrum of the harmonics.
Publication date
LanguageEnglish
AffiliationNational Research Council Canada; NRC Steacie Institute for Molecular Sciences
Peer reviewedNo
NPARC number16751237
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Record identifier6464d9b2-6690-46d1-a9c3-6892ce360112
Record created2011-02-09
Record modified2016-05-09
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