Electron localization following attosecond molecular photoionization

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Title Electron localization following attosecond molecular photoionization
Author Sansone, G.; Kelkensberg, F; Perez-Torres, J. F.; Morales, F.; Kling, M. F.; Siu, W.; Ghafur, Omair; Johnsson, P.; Swoboda, M.; Benedetti, E.; Ferrari, F.; Lépine, F.; Sanz-Vicario, J. L.; Zherebtsov, S.; Znakovskaya, I.; L'Huiller, A.; Ivanov, M. Yu.; Nisoli, M.; Martin, F.; Vrakking, M. J. J.
Journal Name Nature
Year Published 2010
Place of publication United Kingdom
Publisher Nature Publishing Group
Abstract For the past several decades, we have been able to directly probe the motion of atoms that is associated with chemical transformations and which occurs on the femtosecond (10(-15)-s) timescale. However, studying the inner workings of atoms and molecules on the electronic timescale(1-4) has become possible only with the recent development of isolated attosecond (10(-18)-s) laser pulses(5). Such pulses have been used to investigate atomic photoexcitation and photoionization(6,7) and electron dynamics in solids(8), and in molecules could help explore the prompt charge redistribution and localization that accompany photoexcitation processes. In recent work, the dissociative ionization of H(2) and D(2) was monitored on femtosecond timescales(9) and controlled using few-cycle near-infrared laser pulses(10). Here we report a molecular attosecond pump-probe experiment based on that work: H(2) and D(2) are dissociatively ionized by a sequence comprising an isolated attosecond ultraviolet pulse and an intense few-cycle infrared pulse, and a localization of the electronic charge distribution within the molecule is measured that depends-with attosecond time resolution-on the delay between the pump and probe pulses. The localization occurs by means of two mechanisms, where the infrared laser influences the photoionization or the dissociation of the molecular ion. In the first case, charge localization arises from quantum mechanical interference involving autoionizing states and the laser-altered wavefunction of the departing electron. In the second case, charge localization arises owing to laser-driven population transfer between different electronic states of the molecular ion. These results establish attosecond pump-probe strategies as a powerful tool for investigating the complex molecular dynamics that result from the coupling between electronic and nuclear motions beyond the usual Born-Oppenheimer approximation.
Peer Reviewed Yes
Published Yes
Alternative URI http://dx.doi.org/10.1038/nature09084
Volume 465
Issue Number 7299
Page from 763
Page to 766
ISSN 0028-0836
Date Accessioned 2012-01-12; 2012-02-16T05:28:28Z
Date Available 2012-02-16T05:28:28Z
Research Centre Centre for Quantum Dynamics
Faculty Faculty of Science, Environment, Engineering and Technology
Subject Atomic and Molecular Physics
URI http://hdl.handle.net/10072/42757
Publication Type Journal Articles (Refereed Article)
Publication Type Code c1x

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