The effect of light-induced conical intersections on the alignment of diatomic molecules

G. Halász, A. Vibók, Milan Šindelka, Lorenz S. Cederbaum, Nimrod Moiseyev

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

It has already been shown that dressing of diatomic molecules by standing or by running linearly polarized laser waves gives rise to conical intersections (CIs). Due to the presence of such light-induced CIs (LICI), the rovibronic molecular motions are strongly coupled. Here we investigate an impact of LICI on molecular alignment. We show that the degree of alignment of a diatomic molecule as a function of time as obtained from the rigid rotor calculations (where the LICI is ignored) is very different from the exact calculations (where the LICI is taken into consideration). This claim is valid under an assumption that the initially prepared wavepacket has a significant amplitude at the nuclear geometry where the LICI is located. Moreover, our results clearly show that the LICI increases the electronic excitation of the diatom. In particular for weak laser fields this effect is very significant. Our prediction of the LICI's effect on the alignment of diatomic molecules can be confirmed by a two-laser experiment. Here, the first laser should have weak intensity and its duration should be sufficiently long as to align the molecules. The wavelength should be tuned in such a way as to ensure that the initial nuclear wavepacket has a significant amplitude at the internuclear distance corresponding to the LICI. The second laser pulse should be strong to produce measurable high-order harmonics. The high-order harmonic generation spectra should be measured as a function of the time delay between the two laser pulses, and are predicted to give an experimental evidence for the LICI effect on the alignment.

Original languageEnglish
Pages (from-to)146-150
Number of pages5
JournalChemical Physics
Volume399
DOIs
Publication statusPublished - May 3 2012

Fingerprint

diatomic molecules
intersections
alignment
Molecules
lasers
Lasers
Laser pulses
Rigid rotors
rigid rotors
Molecular orientation
algae
Harmonic generation
pulses
Time delay
harmonic generations
time lag
harmonics
Wavelength
Geometry
geometry

Keywords

  • Alignment of diatomic molecules
  • Conical intersection
  • Light-matter interaction

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Physics and Astronomy(all)

Cite this

The effect of light-induced conical intersections on the alignment of diatomic molecules. / Halász, G.; Vibók, A.; Šindelka, Milan; Cederbaum, Lorenz S.; Moiseyev, Nimrod.

In: Chemical Physics, Vol. 399, 03.05.2012, p. 146-150.

Research output: Contribution to journalArticle

Halász, G. ; Vibók, A. ; Šindelka, Milan ; Cederbaum, Lorenz S. ; Moiseyev, Nimrod. / The effect of light-induced conical intersections on the alignment of diatomic molecules. In: Chemical Physics. 2012 ; Vol. 399. pp. 146-150.
@article{284b7c34fc294b62b4e7c2ac0801edcf,
title = "The effect of light-induced conical intersections on the alignment of diatomic molecules",
abstract = "It has already been shown that dressing of diatomic molecules by standing or by running linearly polarized laser waves gives rise to conical intersections (CIs). Due to the presence of such light-induced CIs (LICI), the rovibronic molecular motions are strongly coupled. Here we investigate an impact of LICI on molecular alignment. We show that the degree of alignment of a diatomic molecule as a function of time as obtained from the rigid rotor calculations (where the LICI is ignored) is very different from the exact calculations (where the LICI is taken into consideration). This claim is valid under an assumption that the initially prepared wavepacket has a significant amplitude at the nuclear geometry where the LICI is located. Moreover, our results clearly show that the LICI increases the electronic excitation of the diatom. In particular for weak laser fields this effect is very significant. Our prediction of the LICI's effect on the alignment of diatomic molecules can be confirmed by a two-laser experiment. Here, the first laser should have weak intensity and its duration should be sufficiently long as to align the molecules. The wavelength should be tuned in such a way as to ensure that the initial nuclear wavepacket has a significant amplitude at the internuclear distance corresponding to the LICI. The second laser pulse should be strong to produce measurable high-order harmonics. The high-order harmonic generation spectra should be measured as a function of the time delay between the two laser pulses, and are predicted to give an experimental evidence for the LICI effect on the alignment.",
keywords = "Alignment of diatomic molecules, Conical intersection, Light-matter interaction",
author = "G. Hal{\'a}sz and A. Vib{\'o}k and Milan Šindelka and Cederbaum, {Lorenz S.} and Nimrod Moiseyev",
year = "2012",
month = "5",
day = "3",
doi = "10.1016/j.chemphys.2011.06.038",
language = "English",
volume = "399",
pages = "146--150",
journal = "Chemical Physics",
issn = "0301-0104",
publisher = "Elsevier",

}

TY - JOUR

T1 - The effect of light-induced conical intersections on the alignment of diatomic molecules

AU - Halász, G.

AU - Vibók, A.

AU - Šindelka, Milan

AU - Cederbaum, Lorenz S.

AU - Moiseyev, Nimrod

PY - 2012/5/3

Y1 - 2012/5/3

N2 - It has already been shown that dressing of diatomic molecules by standing or by running linearly polarized laser waves gives rise to conical intersections (CIs). Due to the presence of such light-induced CIs (LICI), the rovibronic molecular motions are strongly coupled. Here we investigate an impact of LICI on molecular alignment. We show that the degree of alignment of a diatomic molecule as a function of time as obtained from the rigid rotor calculations (where the LICI is ignored) is very different from the exact calculations (where the LICI is taken into consideration). This claim is valid under an assumption that the initially prepared wavepacket has a significant amplitude at the nuclear geometry where the LICI is located. Moreover, our results clearly show that the LICI increases the electronic excitation of the diatom. In particular for weak laser fields this effect is very significant. Our prediction of the LICI's effect on the alignment of diatomic molecules can be confirmed by a two-laser experiment. Here, the first laser should have weak intensity and its duration should be sufficiently long as to align the molecules. The wavelength should be tuned in such a way as to ensure that the initial nuclear wavepacket has a significant amplitude at the internuclear distance corresponding to the LICI. The second laser pulse should be strong to produce measurable high-order harmonics. The high-order harmonic generation spectra should be measured as a function of the time delay between the two laser pulses, and are predicted to give an experimental evidence for the LICI effect on the alignment.

AB - It has already been shown that dressing of diatomic molecules by standing or by running linearly polarized laser waves gives rise to conical intersections (CIs). Due to the presence of such light-induced CIs (LICI), the rovibronic molecular motions are strongly coupled. Here we investigate an impact of LICI on molecular alignment. We show that the degree of alignment of a diatomic molecule as a function of time as obtained from the rigid rotor calculations (where the LICI is ignored) is very different from the exact calculations (where the LICI is taken into consideration). This claim is valid under an assumption that the initially prepared wavepacket has a significant amplitude at the nuclear geometry where the LICI is located. Moreover, our results clearly show that the LICI increases the electronic excitation of the diatom. In particular for weak laser fields this effect is very significant. Our prediction of the LICI's effect on the alignment of diatomic molecules can be confirmed by a two-laser experiment. Here, the first laser should have weak intensity and its duration should be sufficiently long as to align the molecules. The wavelength should be tuned in such a way as to ensure that the initial nuclear wavepacket has a significant amplitude at the internuclear distance corresponding to the LICI. The second laser pulse should be strong to produce measurable high-order harmonics. The high-order harmonic generation spectra should be measured as a function of the time delay between the two laser pulses, and are predicted to give an experimental evidence for the LICI effect on the alignment.

KW - Alignment of diatomic molecules

KW - Conical intersection

KW - Light-matter interaction

UR - http://www.scopus.com/inward/record.url?scp=84861344462&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84861344462&partnerID=8YFLogxK

U2 - 10.1016/j.chemphys.2011.06.038

DO - 10.1016/j.chemphys.2011.06.038

M3 - Article

VL - 399

SP - 146

EP - 150

JO - Chemical Physics

JF - Chemical Physics

SN - 0301-0104

ER -