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Laser control of molecular excitations in stochastic dissipative media

  • In the present work, ideas for controlling photochemical reactions in dissipative environments using shaped laser pulses are presented. New time-local control algorithms for the stochastic Schrodinger equation are introduced and compared to their reduced density matrix analog. The numerical schemes rely on time-dependent targets for guiding the reaction along a preferred path. The methods are tested on the vibrational control of adsorbates at metallic surfaces and on the ultrafast electron dynamics in a strong dissipative medium. The selective excitation of the specific states is achieved with improved yield when using the new algorithms. Both methods exhibit similar convergence behavior and results compare well with those obtained using local optimal control for the reduced density matrix. The favorable scaling of the methods allows to tackle larger systems and to control photochemical reactions in dissipative media of molecules with many more degrees of freedom.

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Metadaten
Author:Jean Christophe TremblayORCiDGND
DOI:https://doi.org/10.1063/1.3587093
ISSN:0021-9606 (print)
Parent Title (English):The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr
Publisher:American Institute of Physics
Place of publication:Melville
Document Type:Article
Language:English
Year of first Publication:2011
Year of Completion:2011
Release Date:2017/03/26
Volume:134
Issue:17
Pagenumber:16
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Peer Review:Referiert