Observation of laser-induced electronic structure in oriented polyatomic molecules

P. M. Kraus, O. I. Tolstikhin, D. Baykusheva, A. Rupenyan, J. Schneider, C. Z. Bisgaard, T. Morishita, F. Jensen, L. B. Madsen and H. J. Wörner ()
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P. M. Kraus: Laboratorium für Physikalische Chemie, ETH Zürich
O. I. Tolstikhin: Moscow Institute of Physics and Technology
D. Baykusheva: Laboratorium für Physikalische Chemie, ETH Zürich
A. Rupenyan: Laboratorium für Physikalische Chemie, ETH Zürich
J. Schneider: Laboratorium für Physikalische Chemie, ETH Zürich
C. Z. Bisgaard: FOSS Analytical A/S, FOSS Allé 1
T. Morishita: The University of Electro-Communications
F. Jensen: Aarhus University
L. B. Madsen: Aarhus University
H. J. Wörner: Laboratorium für Physikalische Chemie, ETH Zürich

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract 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.

Date: 2015
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DOI: 10.1038/ncomms8039

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