Attosecond vacuum UV coherent control of molecular dynamics
Entity
UAM. Departamento de QuímicaPublisher
National Academy of SciencesDate
2014-01-21Citation
10.1073/pnas.1321999111
Proceedings of the National Academy of Sciences of the United States of America 111.3 (2014): 912-917
ISSN
1091-6490 (online); 0027-8424 (print)DOI
10.1073/pnas.1321999111Funded by
Work partially supported by the Advanced Grant of the European Research Council XCHEM 290853, the European grant MC-RG ATTOTREND, the European COST Actions CM0702 and CM1204, the European ITN CORINF, the MICINN project Nos. FIS201015127 and CSD 2007-00010 (Spain), and the ERA-Chemistry project PIM2010EEC-00751. XMT was supported by Grand-in-Aid for Scientific Researches (No. C24540421) from the Japan Society for the Promotion of Science and HA-PACS Project for advanced interdisciplinary computational sciences by exa-scale computing technologyProject
info:eu-repo/grantAgreement/EC/FP7/290853; info:eu-repo/grantAgreement/EC/FP7/268284; info:eu-repo/grantAgreement/EC/FP7/264951; Gobierno de España. FIS2010-15127; Gobierno de España. CSD2007-00010Editor's Version
http://dx.doi.org/10.1073/pnas.1321999111Subjects
Chemical dynamics; Electron dynamics; Ultrafast; QuímicaNote
Título del postprint: Attosecond VUV Coherent Control of Molecular DynamicsRights
© 2014 National Academy of Sciences of the United States of AmericaAbstract
High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realized; this is because excitation and manipulation of molecular orbitals requires precisely controlled attosecond waveforms in the deep UV, which have not yet been synthesized. Here, we present a unique approach using attosecond vacuum UV pulse-trains to coherently excite and control the outcome of a simple chemical reaction in a deuterium molecule in a non-Born-Oppenheimer regime. By controlling the interfering pathways of electron wave packets in the excited neutral and singly ionized molecule, we unambiguously show that we can switch the excited electronic state on attosecond timescales, coherently guide the nuclear wave packets to dictate the way a neutral molecule vibrates, and steer and manipulate the ionization and dissociation channels. Furthermore, through advanced theory, we succeed in rigorously modeling multiscale electron and nuclear quantum control in a molecule. The observed richness and complexity of the dynamics, even in this very simplest of molecules, is both remarkable and daunting, and presents intriguing new possibilities for bridging the gap between attosecond physics and attochemistry
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Google Scholar:Ranitovic, Predrag
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Hogle, Craig W.
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Rivière, Paula
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Palacios Cañas, Alicia
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Tong, Xiao Ming
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Toshima, Nobuyuki
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González-Castrillo, Alberto
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Martin, Leigh
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Murnane, Margaret M.
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Kapteyn, Henry
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Martín García, Fernando
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