Mañana, JUEVES, 24 DE ABRIL, el sistema se apagará debido a tareas habituales de mantenimiento a partir de las 9 de la mañana. Lamentamos las molestias.
Even harmonic generation in isotropic media of dissociating homonuclear molecules
Entity
UAM. Departamento de QuímicaPublisher
Nature Publishing GroupDate
2016-09-06Citation
10.1038/srep32653
Scientific Reports 6 (2016): 32653
ISSN
2045-2322DOI
10.1038/srep32653Funded by
We gratefully acknowledge X. B. Bian and A. D. Bandrauk for fruitful discussions and for sharing their data. This work was accomplished with an allocation of computer time from Mare Nostrum BSC and CCC-UAM and was partially supported by the European Research Council Advanced Grant No. XCHEM 290853, MINECO Project No. FIS2013-42002-R, ERA-Chemistry Project No. PIM2010EEC-00751 and DFG SM 292/3-1, European Grant No. MC-ITN CORINF, European COST Action XLIC CM1204, and the CAM project NANOFRONTMAG. R.E.F.S. acknowledges FCT - Fundacao para a Ciencia e Tecnologia, Portugal, Grant No. SFRH/BD/84053/2012. M.I. acknowledges support of the EPSRC programme Grant No. EP/I032517/1 and the Voronezh State UniversityProject
info:eu-repo/grantAgreement/EC/FP7/290853; Gobierno de España. FIS2013-42002-R; info:eu-repo/grantAgreement/EC/FP7/264951; Comunidad de Madrid. S2013/MIT-2850/NANOFRONTMAG-CMEditor's Version
http://dx.doi.org/10.1038/srep32653Subjects
Isotropic gases; IR light; Schrödinger equation; Dissociating molecule; QuímicaRights
© The Author(s) 2016Abstract
Isotropic gases irradiated by long pulses of intense IR light can generate very high harmonics of the incident field. It is generally accepted that, due to the symmetry of the generating medium, be it an atomic or an isotropic molecular gas, only odd harmonics of the driving field can be produced. Here we show how the interplay of electronic and nuclear dynamics can lead to a marked breakdown of this standard picture: a substantial part of the harmonic spectrum can consist of even rather than odd harmonics. We demonstrate the effect using ab-initio solutions of the time-dependent Schrödinger equation for H2+ and its isotopes in full dimensionality. By means of a simple analytical model, we identify its physical origin, which is the appearance of a permanent dipole moment in dissociating homonuclear molecules, caused by light-induced localization of the electric charge during dissociation. The effect arises for sufficiently long laser pulses and the region of the spectrum where even harmonics are produced is controlled by pulse duration. Our results (i) show how the interplay of femtosecond nuclear and attosecond electronic dynamics, which affects the charge flow inside the dissociating molecule, is reflected in the nonlinear response, and (ii) force one to augment standard selection rules found in nonlinear optics textbooks by considering light-induced modifications of the medium during the generation process
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Google Scholar:Silva, R. E. F.
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Rivière, Paula
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Morales, F.
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Smirnova, O.
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Ivanov, M.
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Martín García, Fernando
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