Mapping molecular orbital symmetry on high-order harmonic generation spectrum using two-color laser fields

Hiromichi Niikura, Nirit Dudovich, D. M. Villeneuve, P. B. Corkum

Research output: Contribution to journalArticle

48 Citations (Scopus)

Abstract

We have measured high-order harmonic generation spectra of D2, N2, and CO2 by mixing orthogonally polarized 800 and 400 nm laser fields. The intensity of the high-harmonic spectrum is modulated as we change the relative phase of the two pulses. For randomly orientated molecules, the phase of the intensity modulation depends on the symmetry of the molecular orbitals from which the high harmonics are emitted. This allows us to identify the symmetry of any orbital that contributes to high-harmonic generation, even without aligning the molecule. Our approach can be a route to imaging dynamical changes in three-dimensional molecular orbitals on a time scale as short as a few hundred attoseconds.

Original languageEnglish
Article number053003
JournalPhysical Review Letters
Volume105
Issue number5
DOIs
Publication statusPublished - 2010 Jul 28
Externally publishedYes

Fingerprint

harmonic generations
molecular orbitals
harmonics
color
symmetry
lasers
molecules
routes
modulation
orbitals
pulses

ASJC Scopus subject areas

  • Physics and Astronomy(all)

Cite this

Mapping molecular orbital symmetry on high-order harmonic generation spectrum using two-color laser fields. / Niikura, Hiromichi; Dudovich, Nirit; Villeneuve, D. M.; Corkum, P. B.

In: Physical Review Letters, Vol. 105, No. 5, 053003, 28.07.2010.

Research output: Contribution to journalArticle

@article{348c533297be47a485373eccf35fbf52,
title = "Mapping molecular orbital symmetry on high-order harmonic generation spectrum using two-color laser fields",
abstract = "We have measured high-order harmonic generation spectra of D2, N2, and CO2 by mixing orthogonally polarized 800 and 400 nm laser fields. The intensity of the high-harmonic spectrum is modulated as we change the relative phase of the two pulses. For randomly orientated molecules, the phase of the intensity modulation depends on the symmetry of the molecular orbitals from which the high harmonics are emitted. This allows us to identify the symmetry of any orbital that contributes to high-harmonic generation, even without aligning the molecule. Our approach can be a route to imaging dynamical changes in three-dimensional molecular orbitals on a time scale as short as a few hundred attoseconds.",
author = "Hiromichi Niikura and Nirit Dudovich and Villeneuve, {D. M.} and Corkum, {P. B.}",
year = "2010",
month = "7",
day = "28",
doi = "10.1103/PhysRevLett.105.053003",
language = "English",
volume = "105",
journal = "Physical Review Letters",
issn = "0031-9007",
publisher = "American Physical Society",
number = "5",

}

TY - JOUR

T1 - Mapping molecular orbital symmetry on high-order harmonic generation spectrum using two-color laser fields

AU - Niikura, Hiromichi

AU - Dudovich, Nirit

AU - Villeneuve, D. M.

AU - Corkum, P. B.

PY - 2010/7/28

Y1 - 2010/7/28

N2 - We have measured high-order harmonic generation spectra of D2, N2, and CO2 by mixing orthogonally polarized 800 and 400 nm laser fields. The intensity of the high-harmonic spectrum is modulated as we change the relative phase of the two pulses. For randomly orientated molecules, the phase of the intensity modulation depends on the symmetry of the molecular orbitals from which the high harmonics are emitted. This allows us to identify the symmetry of any orbital that contributes to high-harmonic generation, even without aligning the molecule. Our approach can be a route to imaging dynamical changes in three-dimensional molecular orbitals on a time scale as short as a few hundred attoseconds.

AB - We have measured high-order harmonic generation spectra of D2, N2, and CO2 by mixing orthogonally polarized 800 and 400 nm laser fields. The intensity of the high-harmonic spectrum is modulated as we change the relative phase of the two pulses. For randomly orientated molecules, the phase of the intensity modulation depends on the symmetry of the molecular orbitals from which the high harmonics are emitted. This allows us to identify the symmetry of any orbital that contributes to high-harmonic generation, even without aligning the molecule. Our approach can be a route to imaging dynamical changes in three-dimensional molecular orbitals on a time scale as short as a few hundred attoseconds.

UR - http://www.scopus.com/inward/record.url?scp=77955119295&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=77955119295&partnerID=8YFLogxK

U2 - 10.1103/PhysRevLett.105.053003

DO - 10.1103/PhysRevLett.105.053003

M3 - Article

AN - SCOPUS:77955119295

VL - 105

JO - Physical Review Letters

JF - Physical Review Letters

SN - 0031-9007

IS - 5

M1 - 053003

ER -