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Chinese Physics B

Electron localization of linear symmetric molecular ion ${{\rm{H}}}_{3}^{2+}$

Zhengmao Jia, Zhinan Zeng, Ruxin Li

Published Jan 1, 2017• 1 citation
Publisher

Abstract

Electron localization in the dissociation of the symmetric linear molecular ion H-3(2+) is investigated. The numerical simulation shows that the electron localization distribution is dependent on the central frequency and peak electric field amplitude of the external ultrashort ultraviolet laser pulse. When the electrons of the ground state are excited onto the 2p sigma(2)Sigma(+)(u) by a one-photonprocess, most electrons of the dissociation states are localized at the protons on both sides symmetrically. Almost no electron is stabilized at the middle proton due to the odd symmetry of the wave function. With the increase of the frequency of the external ultraviolet laser pulse, the electron localization ratio of the middle proton increases, for more electrons of the ground state are excited onto the higher 3p sigma(2)Sigma(+)(u) state. 50.9% electrons of all the dissociation events can be captured by the middle Coulomb potential well through optimizing the central frequency and peak electric field amplitude of the ultraviolet laser pulse. Besides, a direct current (DC) electric field can be utilized to control the electron motions of the dissociation states after the excitation of an ultraviolet laser pulse, and 68.8% electrons of the dissociation states can be controlled into the middle proton.

DOI
10.1088/1674-1056/26/1/013203

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Electron localization of H2+{{\rm{H}}}_{2}^{+}H2+​ in a dc electric field
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Laser Induced Dissociation Control of H2+H_2^+H2+​ and H32+H_3^{2+}H32+​
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Abstract We theoretically investigate the frequency dependence in the laser-induced electron localization control of H 2 + . A direct current electric field is used to steer electron motion after the excitation by an ultrashort ultraviolet laser pulse. The electron localization probabilities of the two protons can be modulated by varying the frequency of the exciting laser pulse, due to the different electron movement directions of the lowest three excited states. The strong direct current electric field can act as an effective long-wavelength terahertz pulse in the dissociation control only when most of the electrons of the excited states move in a same direction.
Quantum Dynamics of H2+H_2^+H2+​ in Orthogonal Two-Color Fields
We present full-dimensional quantum simulations of H2+H_2^+H2+​ dissociative ionization driven by strong orthogonal laser fields. We consider equal-frequency orthogonal components, which generate elliptical or circular polarization depending on their relative phase and amplitude, as well as orthogonal 800800800- and 400400400-nm two-color fields. These two-dimensional fields strongly modify the fragmentation dynamics. Most notably, we identify a high-energy peak in the proton kinetic-energy-release (KER) spectrum at approximately 4−54-54−5 eV that is absent from the corresponding single-color, linearly polarized calculations. The yield of this peak can be coherently controlled by varying the relative carrier-envelope phase of the perpendicular field component. The perpendicular field also disrupts the clear electron-proton energy-sharing pattern observed in the main 3−3.53-3.53−3.5 eV dissociation channel, indicating more complex multichannel dynamics. Time-dependent state projections and calculations initiated from individual excited states attribute the additional peak to laser-induced vibrational excitation of H2+H_2^+H2+​. Furthermore, the perpendicular field rotates the fragment angular distributions, causing the most probable proton and electron emission directions to deviate substantially from the principal zzz axis. These findings demonstrate that the spatial and temporal geometry of orthogonal laser fields provides an additional degree of freedom for controlling ultrafast electron-nuclear dynamics.
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Orthogonally polarized two-color sequential laser pulses are used to control the electron localization in the dissociation of H2+{}_{2}{}^{+}2​+. The first single attosecond pulse, whose polarization axis is perpendicular to the molecular axis, excites H2+{}_{2}{}^{+}2​+ from $1s{\ensuremath{\sigma}}_{g}$ to $2p{\ensuremath{\pi}}_{u}$, and the time-delayed infrared pulse, whose polarization axis is parallel to the molecular axis, steers the electron between two nuclei. The simulation of the time-dependent Schr\"odinger equation predicts the control degree of the electron localization can be up to 90% with the current laser technology. In this article, we reveal that the mechanism for this asymmetric localization is due to the mixture of $2p{\ensuremath{\pi}}_{g}$ and $2p{\ensuremath{\pi}}_{u}$, instead of $1s{\ensuremath{\sigma}}_{g}$and $2p{\ensuremath{\sigma}}_{u}$ in the previous studies.