TY - JOUR
T1 - Two-Dimensional Frequency Resolved Optomolecular Gating of High-Order Harmonic Generation
AU - Ferré, A.
AU - Soifer, H.
AU - Pedatzur, O.
AU - Bourassin-Bouchet, C.
AU - Bruner, B. D.
AU - Canonge, R.
AU - Catoire, F.
AU - Descamps, D.
AU - Fabre, B.
AU - Mével, E.
AU - Petit, S.
AU - Dudovich, N.
AU - Mairesse, Y.
N1 - Publisher Copyright:
© 2016 American Physical Society.
PY - 2016/2/2
Y1 - 2016/2/2
N2 - Probing electronic wave functions of polyatomic molecules is one of the major challenges in high-harmonic spectroscopy. The extremely nonlinear nature of the laser-molecule interaction couples the multiple degrees of freedom of the probed system. We combine two-dimensional control of the electron trajectories and vibrational control of the molecules to disentangle the two main steps in high-harmonic generation - ionization and recombination. We introduce a new measurement scheme, frequency-resolved optomolecular gating, which resolves the temporal amplitude and phase of the harmonic emission from excited molecules. Focusing on the study of vibrational motion in N2O4, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.
AB - Probing electronic wave functions of polyatomic molecules is one of the major challenges in high-harmonic spectroscopy. The extremely nonlinear nature of the laser-molecule interaction couples the multiple degrees of freedom of the probed system. We combine two-dimensional control of the electron trajectories and vibrational control of the molecules to disentangle the two main steps in high-harmonic generation - ionization and recombination. We introduce a new measurement scheme, frequency-resolved optomolecular gating, which resolves the temporal amplitude and phase of the harmonic emission from excited molecules. Focusing on the study of vibrational motion in N2O4, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.
UR - http://www.scopus.com/inward/record.url?scp=84957824918&partnerID=8YFLogxK
U2 - 10.1103/PhysRevLett.116.053002
DO - 10.1103/PhysRevLett.116.053002
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AN - SCOPUS:84957824918
SN - 0031-9007
VL - 116
JO - Physical Review Letters
JF - Physical Review Letters
IS - 5
M1 - 053002
ER -