Laser Phase Control of Electron-Nuclear Dynamics in Dissociative Ionization with Intense Femtosecond Pulses: Exact (non-Born-Oppenheimer) Numerical Simulations for H+2

被引:4
作者
Bandrauk, André D. [1 ]
Chelkowski, Szczepan [1 ]
Zamojski, Michel [1 ]
机构
[1] Laboratoire de Chimie Theorique, Faculte des Sciences, Universitéa de Sherbrooke, Sherbrooke, Que
来源
Zeitschrift fur Physikalische Chemie | 2000年 / 214卷 / 10期
关键词
Charge-resonance-enhanced ionizations - Coherent control - Dissociative ionization - Electron-nuclear dynamics - Exact numerical solutions - Intense laser - Laser control - Ultrashort Laser;
D O I
10.1524/zpch.2000.214.10.1393
中图分类号
学科分类号
摘要
Exact numerical solutions of the time-dependent Schroedinger equation, TDSE of a 1-D H+ molecule are obtained for intense (I > 1014 W/cm2) ultrashort (≈<50 fs) laser pulses in order to examine laser control of the exact non-BornOppenheimer electron-nuclear dynamics in this simplest system. Such a non-perturbative treatment of the exact electron-nuclear dynamics allows us to examine the usefulness of simple two-colour (ÖM + 2 ÖM) coherent superpositions of laser pulses to control and manipulate electron and nuclear motion simultaneously. Three processes occur at these high intensities: molecular dissociation, electron ionization and Coulomb explosion. Varying the relative phase of the ÖM and 2 ÖM laser fields allows for the simplest control of the complete electron-nuclear dynamics of these three processes as shown by the present simulation. A major finding is that electron dynamics in the presence of intense ultrashort laser pulses is “counterintuitive”, which can be explained in terms of a quasistatic tunnelling model. Control of the dissociative H+p channel can be explained in terms of “bond softening” occurring from laser-induced avoided crossings of dressed molecular potentials. Control of Coulomb explosion depends on a new nonperturbative phenomenon-Charge Resonance Enhanced Ionization, CREI, which occurs at large critical internuclear distances and can be explained in terms of “frontier” orbitals. © 2000, Oldenbourg Wissenschaftsverlag GmbH. All rights reserved.
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页码:1393 / 1422
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