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Title: Electronic and Nuclear Responses of Fixed-in-Space H{sub 2}S to Ultrashort Intense Laser Fields

Abstract

The Coulomb explosion dynamics of H{sub 2}S, H{sub 2}S{sup 3+}{yields}H{sup +}+S{sup +}+H{sup +}, in ultrashort intense laser fields (12 fs, {approx}2x10{sup 14} W/cm{sup 2}) is studied by the coincidence momentum imaging of the three fragment ions. Different electronic and nuclear responses are identified depending on the direction of laser polarization {epsilon} in the molecular frame. The dependence can be interpreted in terms of the electronic and bonding characters of charge transfer states of H{sub 2}S coupled to the electronic ground state.

Authors:
 [1];  [2];  [3];  [1];  [2];  [1]
  1. Institute for Molecular Science, National Institutes of Natural Sciences, Myodaiji, Okazaki, Aichi 444-8585 (Japan)
  2. (SOKENDAI), Myodaiji, Okazaki, Aichi 444-8585 (Japan)
  3. (Japan)
Publication Date:
OSTI Identifier:
20861477
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review Letters; Journal Volume: 97; Journal Issue: 24; Other Information: DOI: 10.1103/PhysRevLett.97.243002; (c) 2006 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; CHARGE TRANSPORT; CHEMICAL BONDS; COULOMB FIELD; EXPLOSIONS; GROUND STATES; HYDROGEN IONS 1 PLUS; HYDROGEN SULFIDES; LASER RADIATION; POLARIZATION; SULFUR IONS

Citation Formats

Hishikawa, Akiyoshi, Graduate University for Advanced Studies, PRESTO, Japan Science and Technology Agency, Kawaguchi, Saitama 332-0012, Takahashi, Eiji J., Graduate University for Advanced Studies, and Matsuda, Akitaka. Electronic and Nuclear Responses of Fixed-in-Space H{sub 2}S to Ultrashort Intense Laser Fields. United States: N. p., 2006. Web. doi:10.1103/PHYSREVLETT.97.243002.
Hishikawa, Akiyoshi, Graduate University for Advanced Studies, PRESTO, Japan Science and Technology Agency, Kawaguchi, Saitama 332-0012, Takahashi, Eiji J., Graduate University for Advanced Studies, & Matsuda, Akitaka. Electronic and Nuclear Responses of Fixed-in-Space H{sub 2}S to Ultrashort Intense Laser Fields. United States. doi:10.1103/PHYSREVLETT.97.243002.
Hishikawa, Akiyoshi, Graduate University for Advanced Studies, PRESTO, Japan Science and Technology Agency, Kawaguchi, Saitama 332-0012, Takahashi, Eiji J., Graduate University for Advanced Studies, and Matsuda, Akitaka. Fri . "Electronic and Nuclear Responses of Fixed-in-Space H{sub 2}S to Ultrashort Intense Laser Fields". United States. doi:10.1103/PHYSREVLETT.97.243002.
@article{osti_20861477,
title = {Electronic and Nuclear Responses of Fixed-in-Space H{sub 2}S to Ultrashort Intense Laser Fields},
author = {Hishikawa, Akiyoshi and Graduate University for Advanced Studies and PRESTO, Japan Science and Technology Agency, Kawaguchi, Saitama 332-0012 and Takahashi, Eiji J. and Graduate University for Advanced Studies and Matsuda, Akitaka},
abstractNote = {The Coulomb explosion dynamics of H{sub 2}S, H{sub 2}S{sup 3+}{yields}H{sup +}+S{sup +}+H{sup +}, in ultrashort intense laser fields (12 fs, {approx}2x10{sup 14} W/cm{sup 2}) is studied by the coincidence momentum imaging of the three fragment ions. Different electronic and nuclear responses are identified depending on the direction of laser polarization {epsilon} in the molecular frame. The dependence can be interpreted in terms of the electronic and bonding characters of charge transfer states of H{sub 2}S coupled to the electronic ground state.},
doi = {10.1103/PHYSREVLETT.97.243002},
journal = {Physical Review Letters},
number = 24,
volume = 97,
place = {United States},
year = {Fri Dec 15 00:00:00 EST 2006},
month = {Fri Dec 15 00:00:00 EST 2006}
}
  • We propose a new approach to obtain molecular frame photoelectron angular distributions from molecules ionized by intense laser pulses. With our method we study the angular tunnel ionization probability of H{sub 2} at a wavelength of 800 nm over an intensity range of 2-4.5x10{sup 14} W/cm{sup 2}. We find an anisotropy that is stronger than predicted by any existing model. To explain the observed anisotropy and its strong intensity dependence we develop an analytical model in the framework of the strong-field approximation. It expresses molecular ionization as a product of atomic ionization rate and a Fourier transform of the highestmore » occupied molecular orbital filtered by the strong-field ionization process.« less
  • No abstract prepared.
  • Double ionization channels of H{sub 2} are separated in the time domain using ultrashort 10-fs laser pulses in the 10{sup 13}-10{sup 15} W cm{sup -2} intensity range. Charge resonance enhanced ionization does not contribute anymore to double ionization because the H{sub 2}{sup +} ion does not have enough time to stretch up to the critical internuclear distance. Using a pump-probe excitation scheme, this process is shown to be very sensitive for the detection of pre- and post-pulses situated at a few tens of femtoseconds from the maximum pulse envelope.
  • We report correlated two-electron ab initio calculations for the hydrogen molecule H{sub 2} in interaction with intense ultrashort laser pulses, via a solution of the full three-dimensional time-dependent Schroedinger equation. Our results for ionization and excitation probabilities (at 800 and 400 nm) as a function of internuclear distance R show strong evidence of enhanced ionization, in both single and double ionization, as well as enhanced excitation, in single and double excitation, as the internuclear distance R increases from the equilibrium value R{sub e}. The enhancement of all these molecular processes exhibits a maximum at a critical distance R{sub c}, whichmore » can be predicted from simple electrostatic and recollision models.« less
  • We study the radiative distortion of the lowest two potential surfaces of H[sub 2][sup +] and H[sub 3][sup 2+] molecular ions in a superintense ([ital I][gt]10[sup 16] W/cm[sup 2]), high-frequency, linearly polarized laser field, using the space-translation or acceleration representation of laser-matter interaction. The electron clouds undergo field-induced redistribution in the molecular ions due to the presence of field-induced dichotomous'' dressed Coulomb potentials. Such super-field-dressed systems have a greater tendency to transfer electronic charge into the region between the nuclei and hence become more stable'' than the field-free ones. For example, at the equilibrium nuclear separation the dissociation energy ofmore » the superdressed H[sub 2][sup +] is found to increase by about 20% compared with the field-free H[sub 2][sup +]. More dramatically, the lowest two surfaces of H[sub 3][sup 2+] that are repulsive in zero field become attractive (bonding) in the presence of an intense, high-frequency field. The possibility of molecules becoming stabilized against both ionization and dissociation in superintense fields is discussed.« less