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search.filters.applied.f.access: openAccess × End date: 2023 × Start date: 2022 × End date: 2024 × Start date: 2020 × DDC: 500 × Subject: spectroscopy × WGL Institute: MBI ×

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    Population difference gratings created on vibrational transitions by nonoverlapping subcycle THz pulses
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Arkhipov, Rostislav; Pakhomov, Anton; Arkhipov, Mikhail; Babushkin, Ihar; Demircan, Ayhan; Morgner, Uwe; Rosanov, Nikolay
    We study theoretically a possibility of creation and ultrafast control (erasing, spatial frequency multiplication) of population density gratings in a multi-level resonant medium having a resonance transition frequency in the THz range. These gratings are produced by subcycle THz pulses coherently interacting with a nonlinear medium, without any need for pulses to overlap, thereby utilizing an indirect pulse interaction via an induced coherent polarization grating. High values of dipole moments of the transitions in the THz range facilitate low field strength of the needed THz excitation. Our results clearly show this possibility in multi-level resonant media. Our theoretical approach is based on an approximate analytical solution of time-dependent Schrödinger equation (TDSE) using perturbation theory. Remarkably, as we show here, quasi-unipolar subcycle pulses allow more efficient excitation of higher quantum levels, leading to gratings with a stronger modulation depth. Numerical simulations, performed for THz resonances of the H20 molecule using Bloch equations for density matrix elements, are in agreement with analytical results in the perturbative regime. In the strong-field non-perturbative regime, the spatial shape of the gratings becomes non-harmonic. A possibility of THz radiation control using such gratings is discussed. The predicted phenomena open novel avenues in THz spectroscopy of molecules with unipolar and quasi-unipolar THz light bursts and allow for better control of ultra-short THz pulses.
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    Probing multiphoton light-induced molecular potentials
    ([London] : Nature Publishing Group UK, 2020) Kübel, M.; Spanner, M.; Dube, Z.; Naumov, A.Yu.; Chelkowski, S.; Bandrauk, A.D.; Vrakking, M.J.J.; Corkum, P.B.; Villeneuve, D.M.; Staudte, A.
    The strong coupling between intense laser fields and valence electrons in molecules causes distortions of the potential energy hypersurfaces which determine the motion of the nuclei and influence possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, leading to the emergence of light-induced conical intersections. Here, we demonstrate that multiphoton couplings can give rise to complex light-induced potential energy surfaces that govern molecular behavior. In the laser-induced dissociation of H2+, the simplest of molecules, we measure a strongly modulated angular distribution of protons which has escaped prior observation. Using two-color Floquet theory, we show that the modulations result from ultrafast dynamics on light-induced molecular potentials. These potentials are shaped by the amplitude, duration and phase of the dressing fields, allowing for manipulating the dissociation dynamics of small molecules.