Volume 100, Issue 6 pp. 834-844

Attosecond localization of electrons in molecules

André D. Bandrauk

Corresponding Author

André D. Bandrauk

Laboratoire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, Québec, J1K 2R1, Canada

Canada Research Chair in Computational Chemistry and Photonics

Laboratoire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, Québec, J1K 2R1, CanadaSearch for more papers by this author
Stephane Chelkowski

Stephane Chelkowski

Laboratoire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, Québec, J1K 2R1, Canada

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Hong Shon Nguyen

Hong Shon Nguyen

Laboratoire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, Québec, J1K 2R1, Canada

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First published: 10 September 2004
Citations: 138

Abstract

Numerical solutions of the time-dependent Schrödinger equation for a 1D model non-Born–Oppenheimer Hurn:x-wiley:00207608:media:QUA20252:tex2gif-stack-1 are used to illustrate the nonlinear nonperturbative response of molecules to intense (I ≥ 1013 W/cm2), ultrashort (t < 10 fs) laser pulses. Molecular high-order harmonic generation (MHOHG) is shown to be an example of such response and the resulting nonlinear photon emission spectrum is shown to lead to the synthesis of single attosecond (10−18 s) pulses. Application of such ultrashort pulses to the Hurn:x-wiley:00207608:media:QUA20252:tex2gif-stack-2 system results in localized electron wavepackets whose motion can be detected by asymmetry in the photoelectron spectrum generated by a subsequent probe attosecond pulse, thus leading to measurement of electron motion in molecules on the attosecond time scale. © 2004 Wiley Periodicals, Inc. Int J Quantum Chem, 2004

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