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Title: Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse

Authors:
; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1356868
Grant/Contract Number:
SC0012628
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 95; Journal Issue: 5; Related Information: CHORUS Timestamp: 2017-05-12 22:08:53; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English

Citation Formats

Nikodem, Astrid, Levine, R. D., and Remacle, F. Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse. United States: N. p., 2017. Web. doi:10.1103/PhysRevA.95.053404.
Nikodem, Astrid, Levine, R. D., & Remacle, F. Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse. United States. doi:10.1103/PhysRevA.95.053404.
Nikodem, Astrid, Levine, R. D., and Remacle, F. 2017. "Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse". United States. doi:10.1103/PhysRevA.95.053404.
@article{osti_1356868,
title = {Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse},
author = {Nikodem, Astrid and Levine, R. D. and Remacle, F.},
abstractNote = {},
doi = {10.1103/PhysRevA.95.053404},
journal = {Physical Review A},
number = 5,
volume = 95,
place = {United States},
year = 2017,
month = 5
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 12, 2018
Publisher's Accepted Manuscript

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  • We demonstrate an experimental control of electron localization in deuterium molecular ions created and dissociated by the combined action of an attosecond pulse train and a many-cycle infrared (IR) pulse. The attosecond pulse train is synthesized using both even and odd high order harmonics of the driving IR frequency so that it can strobe the IR field once per IR cycle. An asymmetric ejection of the deuterium ions oscillates with the full IR period when the APT-IR time-delay is scanned. The observed control is due to the creation of a coherent superposition of 1s {sigma}{sub g} and 2p {sigma}{sub u}more » states via interference between one-photon and two-photon dissociation channels.« less
  • We present ab initio quantum and classical investigations on the production and control of a single attosecond pulse by using few-cycle intense laser pulses as the driving field. The high-harmonic-generation power spectrum is calculated by accurately and efficiently solving the time-dependent Schroedinger equation using the time-dependent generalized pseudospectral method. The time-frequency characteristics of the attosecond xuv pulse are analyzed in detail by means of the wavelet transform of the time-dependent induced dipole. To better understand the physical processes, we also perform classical trajectory simulation of the strong-field electron dynamics and electron returning energy map. We found that the quantum andmore » classical results provide complementary and consistent information regarding the underlying mechanisms responsible for the production of the coherent attosecond pulse. For few-cycle (5 fs) driving pulses, it is shown that the emission of the consecutive harmonics in the supercontinuum cutoff regime can be synchronized and locked in phase resulting in the production of a coherent attosecond pulse. Moreover, the time profile of the attosecond pulses can be controlled by tuning the carrier envelope phase.« less
  • The infrared photochemical decomposition of bicyclopropyl-d/sub 4/, specifically deuterated on one ring, has been examined. The molecule incorporates two reactive moieties that are differentiated only by isotopic substitution, hydrogenated and deuterated cyclopropane rings. Since statistical theories predict essentially equivalent rates of decomposition of each ring at any internal energy, the branching ratio constitutes a direct probe for nonstatistical effects. From a determination of the deuterium distribution in the single-ring cleaved product, allylcyclopropane, a branching ratio, k/sub H//k/sub D/ = 1.03 +- 0.08, is calculated. This is in good agreement with the statistical prediction and provides direct chemical evidence for themore » lack of significant nonrandom chemistry in the multiphoton infrared photochemistry of bicyclopropyl under the conditions of these experiments. 6 figures, 1 table.« less
  • Recent experimental observations of time-resolved multidimensional signals in the light-harvesting antennae Fenna-Mathews-Olson [G. S. Engel et al., Nature (London) 446, 782 (2007)] show large oscillations of exciton populations coupled to the long-lived coherences. These effects may not be reproduced by the standard Redfield theory which assumes weak coupling to a bath. A more general relaxation superoperator which holds for all system-bath coupling parameter regimes is constructed by taking into account the statistics (covariances) of Lindblad equation parameters. Simulations for a model dimer reproduce all observed strong coupling effects.