Laser tunnel ionization from multiple orbitals in HCl

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DOIResolve DOI: http://doi.org/10.1126/science.1175253
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TypeArticle
Journal titleScience
Volume325
Issue5946
Pages13641367; # of pages: 11
AbstractTunneling, one of the most striking manifestations of quantum mechanics, influences the electronic structure of many molecules and solids and is responsible for radioactive decay. Much of the interaction of intense light pulses with matter commences with electrons tunneling from atoms or molecules to the continuum. Until recently, this starting point was assumed to be the highest occupied orbital of a given system. We have now observed tunneling from a lower-lying state in hydrogen chloride (HCl). Analyzing two independent experimental observables allowed us to isolate (via fragment ions), identify (via molecular frame photoelectron angular distributions), and, with the help of ab initio simulations, quantify the contribution of lower-lying orbitals to the total and angle-dependent tunneling current of the molecule. Our results bolster the emerging tenet that the coherent interaction between different orbitals—which can amplify the impact of lower orbitals—must be considered in tunneling processes.
Publication date
LanguageEnglish
AffiliationNRC Steacie Institute for Molecular Sciences; National Research Council Canada
Peer reviewedYes
NPARC number14829317
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Record identifier452fb4b9-fbc9-4635-ab52-753a4424c804
Record created2010-03-26
Record modified2016-05-09
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