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Now showing 1 - 10 of 13
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    Ultrafast Structural Changes in Chiral Molecules Measured with Free-Electron Lasers
    (Bristol : IOP Publ., 2020) Schmidt, P.; Music, V.; Hartmann, G.; Boll, R.; Erk, B.; Bari, S.; Allum, F.; Baumann, T.M.; Brenner, G.; Brouard, M.; Burt, M.; Coffee, R.; Dörner, S.; Galler, A.; Grychtol, P.; Heathcote, D.; Inhester, L.; Kazemi, M.; Larsson, M.; Li, Z.; Lutmann, A.; Manschwetus, B.; Marder, L.; Mason, R.; Moeller, S.; Osipov, T.; Otto, H.; Passow, C.; Rolles, D.; Rupprecht, P.; Schubert, K.; Schwob, L.; Thomas, R.; Vallance, C.; Von Korff Schmising, C.; Wagner, R.; Walter, P.; Wolf, T.J.A.; Zhaunerchyk, V.; Meyer, M.; Ehresmann, A.; Knie, A.; Demekhin, P.V.; Ilchen, M.
    (X-ray) free-electron lasers are employed to site specifically interrogate atomic fragments during ultra-fast photolysis of chiral molecules via time-resolved photoelectron circular dichroism. © 2020 Institute of Physics Publishing. All rights reserved.
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    Atomic processes in bicircular fields
    (Bristol : IOP Publ., 2016) Odžak, S.; Hasović, E.; Becker, W.; Milošević, D.B.
    We investigate laser-assisted electron-ion recombination (LAR), high-order harmonic generation (HHG) and above-threshold ionization (ATI) of argon atoms by a bicircular laser field, which consists of two coplanar counter-rotating circularly polarized fields of frequencies rω and sω. The energy of soft x rays generated in the LAR process is analyzed as a function of the incident electron angle and numerical results of direct recombination of electrons with Ar+ ions are presented. We also present the results of HHG by a bicircular field and confirm the selection rules derived earlier for inert-gas atoms in a p ground state. We show that the photoelectron spectra in the ATI process, presented in the momentum plane, as well as the LAR spectra exhibit the same discrete rotational symmetry as the applied field.
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    Photoelectron holography in strong optical and dc electric fields
    (Bristol : Institute of Physics Publishing, 2014) Stodolna, A.; Huismans, Y.; Rouzée, A.; Lépine, F.; Vrakking, M.J.J.
    The application of velocity map imaging for the detection of photoelectrons resulting from atomic or molecular ionization allows the observation of interferometric, and in some cases holographic structures that contain detailed information on the target from which the photoelecrons are extracted. In this contribution we present three recent examples of the use of photoelectron velocity map imaging in experiments where atoms are exposed to strong optical and dc electric fields. We discuss (i) observations of the nodal structure of Stark states of hydrogen measured in a dc electric field, (ii) mid-infrared strong-field ionization of metastable Xe atoms and (iii) the reconstruction of helium electronic wavepackets in an attosecond pump-probe experiment. In each case, the interference between direct and indirect electron pathways, reminiscent of the reference and signal waves in holography, is seen to play an important role.
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    Correlated electronic decay following intense near-infrared ionization of clusters
    (Bristol : IOP Publ., 2015) Schütte, Bernd; Arbeiter, Mathias; Fennel, Thomas; Jabbari, Ghazal; Kuleff, Alexander I.; Vrakking, Marc J. J.; Rouzée, Arnaud
    We report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.
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    The role of the Kramers-Henneberger atom in the higher-order Kerr effect
    (Bristol : IOP, 2013) Richter, M.; Patchkovskii, S.; Morales, F.; Smirnova, O.; Ivanov, M.
    We discuss the connection between strong-field ionization, saturation of the Kerr response and the formation of the Kramers-Henneberger (KH) atom and long-living excitations in intense infrared (IR) external fields. We present a generalized model for the intensity-dependent response of atoms in strong IR laser fields, describing deviations in the nonlinear response at the frequency of the driving field from the standard model. We show that shaping the driving laser pulse allows one to reveal signatures of the excited KH states in the Kerr response of an individual atom.
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    Photon transport in one-dimensional systems coupled to three-level quantum impurities
    (Bristol : IOP, 2013) Martens, C.; Longo, P.; Busch, K.
    We discuss the transport properties of a single photon in a one-dimensional waveguide with an embedded three-level atom and utilize both stationary plane-wave solutions and time-dependent transport calculations to investigate the interaction of a photon with driven and undriven V- and Λ-systems. Specifically, for the case of an undriven V-system, we analyze the phenomenon of long-time occupation of the upper atomic levels in conjunction with almost dark states. For the undriven Λ-system, we find non-stationary dark states and we explain how the photon's transmittance can be controlled by an initial phase difference between the energetically lower-lying atomic states. With regard to the driven three-level systems, we discuss electromagnetically induced transparency in terms of the pulse propagation of a single photon through a Λ-type atom. In addition, we demonstrate how a driven V-type atom can be utilized to control the momentum distribution of the scattered photon.
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    Non-instantaneous third-order optical response of gases in low-frequency fields
    (Washington, DC : Soc., 2022) Morales, Felipe; Richter, Maria; Ivanov, Misha; Husakou, Anton
    It is commonly assumed that for low-intensity short optical pulses far from resonance, the third-order optical nonlinear response is instantaneous. We solve the three-dimensional time-dependent Schrödinger equation for the hydrogen atom and show that this is not the case: the polarization is not simply proportional to the cube of the electric field even at low intensities. We analyze the fundamental-frequency and third-harmonic nonlinear susceptibilities of hydrogen, investigate their dependence on intensity, and find that the delays in the Kerr response rapidly approach the femtosecond time-scale at higher intensities, while the delays in the third harmonic generation remain much lower. We also propose an experimental scheme to detect and characterize the above effects.
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    Excited state distribution and spin-effects in strong-field excitation of neutral Helium
    (Bristol : IOP Publ., 2015) Zimmermann, Henri; Eilzer, Sebastian; Eichmann, Ulli
    We investigated the principal quantum number n distribution of excited states resulting from the interaction of Helium with strong, short laser pulses. We find excellent agreement with predictions of the semiclassical frustrated tunneling ionization (FTI) model [1] as well as fully quantum mechanical calculations. Furthermore, the excitation process directly populates triplet excited states due to the breakdown of the Russel-Saunders coupling scheme for high orbital angular momentum l states of Helium, which are predominantly populated in the strong laser field.
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    Intracycle interference in ionization of Ar by a laser assisted XUV pulse
    (Bristol : IOP Publ., 2017) Arbó, D.G.; López, S. D.; Kubin, M.; Hummert, J.; Vrakking, M.J.J.; Kornilov, O.
    Synopsis We present a theoretical and experimental study of the subcycle interference in laser assisted XUV ionization of Ar atoms. Averaging over the focal volume happens to blur the intracycle interference, which thus cannot be measured directly. We show that even at these conditions, the intracycle interference can be obtained through the subtraction of two different angle and energy-resolved distributions at slightly different laser intensities.
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    Symmetries and Selection Rules of the Spectra of Photoelectrons and High-Order Harmonics Generated by Field-Driven Atoms and Molecules
    (Basel : MDPI, 2021) Habibović, Dino; Becker, Wilhelm; Milošević, Dejan B.
    Using the strong-field approximation we systematically investigate the selection rules for high-order harmonic generation and the symmetry properties of the angle-resolved photoelectron spectra for various atomic and molecular targets exposed to one-component and two-component laser fields. These include bicircular fields and orthogonally polarized two-color fields. The selection rules are derived directly from the dynamical symmetries of the driving field. Alternatively, we demonstrate that they can be obtained using the conservation of the projection of the total angular momentum on the quantization axis. We discuss how the harmonic spectra of atomic targets depend on the type of the ground state or, for molecular targets, on the pertinent molecular orbital. In addition, we briefly discuss some properties of the high-order harmonic spectra generated by a few-cycle laser field. The symmetry properties of the angle-resolved photoelectron momentum distribution are also determined by the dynamical symmetry of the driving field. We consider the first two terms in a Born series expansion of the T matrix, which describe the direct and the rescattered electrons. Dynamical symmetries involving time translation generate rotational symmetries obeyed by both terms. However, those that involve time reversal generate reflection symmetries that are only observed by the direct electrons. Finally, we explain how the symmetry properties, imposed by the dynamical symmetry of the driving field, are altered for molecular targets.