Observation of laser-induced electronic structure in oriented polyatomic molecules

All attosecond time-resolved measurements have so far relied on the use of intense near-infrared laser pulses. In particular, attosecond streaking, laser-induced electron diffraction and high-harmonic generation all make use of non-perturbative light-matter interactions. Remarkably, the effect of th...

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Bibliographic Details
Published in:Nature communications 2015-05, Vol.6 (1), p.7039-7039, Article 7039
Main Authors: Kraus, P M, Tolstikhin, O I, Baykusheva, D, Rupenyan, A, Schneider, J, Bisgaard, C Z, Morishita, T, Jensen, F, Madsen, L B, Wörner, H J
Format: Article
Language:English
Subjects:
Electron diffraction
Electronic structure
Electrons
Harmonic generations
Infrared lasers
Lasers
Light diffraction
Molecular structure
Polyatomic molecules
Spectroscopy
Spectrum analysis
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Summary:All attosecond time-resolved measurements have so far relied on the use of intense near-infrared laser pulses. In particular, attosecond streaking, laser-induced electron diffraction and high-harmonic generation all make use of non-perturbative light-matter interactions. Remarkably, the effect of the strong laser field on the studied sample has often been neglected in previous studies. Here we use high-harmonic spectroscopy to measure laser-induced modifications of the electronic structure of molecules. We study high-harmonic spectra of spatially oriented CH3F and CH3Br as generic examples of polar polyatomic molecules. We accurately measure intensity ratios of even and odd-harmonic orders, and of the emission from aligned and unaligned molecules. We show that these robust observables reveal a substantial modification of the molecular electronic structure by the external laser field. Our insights offer new challenges and opportunities for a range of emerging strong-field attosecond spectroscopies.
ISSN:2041-1723
2041-1723
DOI:10.1038/ncomms8039