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Title: Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses

Abstract

We studied the nuclear dynamics in diatomic molecules (N{sub 2}, O{sub 2}, and CO) following their interaction with intense near-IR few-cycle laser pulses. Using Coulomb-explosion imaging in combination with the pump-probe approach, we mapped dissociation pathways of those molecules and their molecular ions. We identified all symmetric and asymmetric breakup channels for molecular ions up to N{sub 2}{sup 5+}, O{sub 2}{sup 4+}, and CO{sup 4+}. For each of those channels we measured the kinetic energy release (KER) spectra as a function of delay between the pump and probe pulses. For both N{sub 2} and O{sub 2} the asymmetric (3,1) channel is only observed for short (<20 fs) delays and completely disappears after that. We interpret this observation as a signature of electron localization taking place in dissociating molecular tri-cations when their internuclear separation reaches about 2.5 times the equilibrium bond length. This is a direct confirmation that electron localization plays an essential role in the universal mechanism of enhanced ionization in homonuclear diatomic molecules. Using classical and quantum mechanical simulations of the time-dependent KER spectra, we identify the pathways and intermediate states involved in the laser-induced dissociation of those molecules.

Authors:
; ; ;  [1];  [2];  [3];  [1]
  1. J. R. Macdonald Laboratory, Kansas State University, Kansas 66506 (United States)
  2. Department of Physics, American University of Sharjah, Sharjah (United Arab Emirates)
  3. Departamento de Quimica, C-IX, Universidad Autonoma de Madrid, ES-28049 Madrid (Spain)
Publication Date:
OSTI Identifier:
21537012
Resource Type:
Journal Article
Journal Name:
Physical Review. A
Additional Journal Information:
Journal Volume: 83; Journal Issue: 1; Other Information: DOI: 10.1103/PhysRevA.83.013417; (c) 2011 American Institute of Physics; Journal ID: ISSN 1050-2947
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; ASYMMETRY; BOND LENGTHS; CARBON MONOXIDE; CATIONS; COULOMB ENERGY; DISSOCIATION; IONIZATION; KINETIC ENERGY; LASER RADIATION; MEASURING METHODS; MOLECULAR IONS; MOLECULES; OXYGEN; QUANTUM MECHANICS; TIME DEPENDENCE; TIME RESOLUTION; WAVE PACKETS; CARBON COMPOUNDS; CARBON OXIDES; CHALCOGENIDES; CHARGED PARTICLES; DIMENSIONS; ELECTROMAGNETIC RADIATION; ELEMENTS; ENERGY; IONS; LENGTH; MECHANICS; NONMETALS; OXIDES; OXYGEN COMPOUNDS; RADIATIONS; RESOLUTION; TIMING PROPERTIES

Citation Formats

Bocharova, I A, Thumm, U, Ray, D, Cocke, C L, Alnaser, A S, Niederhausen, T, Litvinyuk, I V, and Centre for Quantum Dynamics, Griffith University, Nathan, Queensland 4111. Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses. United States: N. p., 2011. Web. doi:10.1103/PHYSREVA.83.013417.
Bocharova, I A, Thumm, U, Ray, D, Cocke, C L, Alnaser, A S, Niederhausen, T, Litvinyuk, I V, & Centre for Quantum Dynamics, Griffith University, Nathan, Queensland 4111. Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses. United States. doi:10.1103/PHYSREVA.83.013417.
Bocharova, I A, Thumm, U, Ray, D, Cocke, C L, Alnaser, A S, Niederhausen, T, Litvinyuk, I V, and Centre for Quantum Dynamics, Griffith University, Nathan, Queensland 4111. Sat . "Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses". United States. doi:10.1103/PHYSREVA.83.013417.
@article{osti_21537012,
title = {Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses},
author = {Bocharova, I A and Thumm, U and Ray, D and Cocke, C L and Alnaser, A S and Niederhausen, T and Litvinyuk, I V and Centre for Quantum Dynamics, Griffith University, Nathan, Queensland 4111},
abstractNote = {We studied the nuclear dynamics in diatomic molecules (N{sub 2}, O{sub 2}, and CO) following their interaction with intense near-IR few-cycle laser pulses. Using Coulomb-explosion imaging in combination with the pump-probe approach, we mapped dissociation pathways of those molecules and their molecular ions. We identified all symmetric and asymmetric breakup channels for molecular ions up to N{sub 2}{sup 5+}, O{sub 2}{sup 4+}, and CO{sup 4+}. For each of those channels we measured the kinetic energy release (KER) spectra as a function of delay between the pump and probe pulses. For both N{sub 2} and O{sub 2} the asymmetric (3,1) channel is only observed for short (<20 fs) delays and completely disappears after that. We interpret this observation as a signature of electron localization taking place in dissociating molecular tri-cations when their internuclear separation reaches about 2.5 times the equilibrium bond length. This is a direct confirmation that electron localization plays an essential role in the universal mechanism of enhanced ionization in homonuclear diatomic molecules. Using classical and quantum mechanical simulations of the time-dependent KER spectra, we identify the pathways and intermediate states involved in the laser-induced dissociation of those molecules.},
doi = {10.1103/PHYSREVA.83.013417},
journal = {Physical Review. A},
issn = {1050-2947},
number = 1,
volume = 83,
place = {United States},
year = {2011},
month = {1}
}