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Circular dichroism in ion yields employing femtosecond laser ionization-the role of laser pulse duration

  • The circular dichroism (CD) induced by femtosecond laser pulse excitation of 3-methylcyclopentanone has been investigated by means of experiment and theory as a function of the laser pulse duration. In the experiment the CD in ion yields is measured by femtosecond laser ionization via a one-photon resonant excited state. In the theoretical part the CD is calculated by solving laser driven quantum electron dynamics for the same resonant excitation based on ab initio electronic structure calculations employing a complete description of the electric field-electric dipole and magnetic field-magnetic dipole interactions. Both the experimentally measured CD in ion yields and the calculated CD in excited state populations exhibit a marked increase of the CD for pulse duration increasing from 50 fs to about 200 fs. Beyond 200 fs pulse duration the CD levels off. The combination of experimental and theoretical evidences indicates that the CD decreases with increasing laser intensity connected to the increased coupling between the excitedThe circular dichroism (CD) induced by femtosecond laser pulse excitation of 3-methylcyclopentanone has been investigated by means of experiment and theory as a function of the laser pulse duration. In the experiment the CD in ion yields is measured by femtosecond laser ionization via a one-photon resonant excited state. In the theoretical part the CD is calculated by solving laser driven quantum electron dynamics for the same resonant excitation based on ab initio electronic structure calculations employing a complete description of the electric field-electric dipole and magnetic field-magnetic dipole interactions. Both the experimentally measured CD in ion yields and the calculated CD in excited state populations exhibit a marked increase of the CD for pulse duration increasing from 50 fs to about 200 fs. Beyond 200 fs pulse duration the CD levels off. The combination of experimental and theoretical evidences indicates that the CD decreases with increasing laser intensity connected to the increased coupling between the excited states.show moreshow less

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Metadaten
Author:Philipp Horsch, Gunter Urbasch, Karl-Michael Weitzel, Dominik Kroener
DOI:https://doi.org/10.1039/c0cp01903h
ISSN:1463-9076 (print)
Parent Title (English):Physical chemistry, chemical physics : a journal of European Chemical Societies
Publisher:Royal Society of Chemistry
Place of publication:Cambridge
Document Type:Article
Language:English
Year of first Publication:2011
Year of Completion:2011
Release Date:2017/03/26
Volume:13
Issue:6
Pagenumber:9
First Page:2378
Last Page:2386
Funder:German Research Foundation (DFG) [WE B30/9, DK 2942]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Peer Review:Referiert