Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection
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Author(s)
Type
Journal Article
Abstract
Nonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electron–nuclear dynamics at CIs, offered by the advent of nearly single-cycle, phase-stable, mid-infrared laser pulses. To illustrate the control mechanism, a two-dimensional model of the NO2 molecule is considered. The key idea of the control scheme is to match the time scale of the laser field oscillations to the characteristic time scale of the wave packet transit through the CI. The instantaneous laser field changes the shape and position of the CI as the wave packet passes through. As the CI moves in the laser field, it 'slices' through the wave packet, sculpting it in the coordinate and momentum space in a way that is sensitive to the carrier-envelope phase of the control pulse. We find that the electronic coherence imparted on the sub-laser-cycle time scale manifests during much longer nuclear dynamics that follow on the many tens of femtosecond time scale. Control efficiency as a function of molecular orientation is analyzed, showing that modest alignment is sufficient for showing the described effects.
Date Issued
2015-11-06
Date Acceptance
2015-10-06
Citation
New Journal of Physics, 2015, 17
ISSN
1367-2630
Publisher
IOP Publishing
Journal / Book Title
New Journal of Physics
Volume
17
Copyright Statement
Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence. Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.
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Sponsor
Engineering & Physical Science Research Council (EPSRC)
Commission of the European Communities
Grant Number
EP/I032517/1
264951
Subjects
Science & Technology
Physical Sciences
Physics, Multidisciplinary
Physics
sub-femtosecond laser control
molecular dynamics
conical intersection
nonadiabatic effects
POTENTIAL-ENERGY SURFACES
RESOLVED PHOTOELECTRON-SPECTROSCOPY
ABOVE-THRESHOLD DISSOCIATION
HIGH-HARMONIC SPECTROSCOPY
LONG-WAVELENGTH LIMIT
WAVE-PACKET DYNAMICS
LOWEST 2A STATES
AB-INITIO
NITROGEN-DIOXIDE
QUANTUM CONTROL
Publication Status
Published
Article Number
113023