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Journal of Physics B Atomic Molecular and Optical Physics

Spin-dependent rescattering in strong-field ionization of helium

Danilo Zille, D. Seipt, Max Möller, S. Fritzsche, Stefanie Gräfe, Carsten Müller, G. G. Paulus

Published Feb 2, 2017• 8 citations
Publisher

Abstract

Abstract We investigate the influence of singlet and triplet spin states on rescattered photoelectrons in strong-field ionization of excited helium. Choosing either a symmetric or antisymmetric spatial wave function as the initial state results in different scattering cross sections for the 1 s 2 s 1 S and 3 S states. These cross sections are used in the semi-classical model of strong-field ionization. Our investigations show that the photoelectron momentum distributions of rescattered electrons exhibit a significant dependence on the relative spin state of the projectile and the bound electron which should be observable in experiments. The proposed experimental approach can be understood as a testbed for probing the spin dynamics of electrons during strong-field ionization and the presented results as a baseline for their identification.

DOI
10.1088/1361-6455/aa5db1

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Abstract We investigate the influence of singlet and triplet spin states on rescattered photoelectrons in strong-field ionization of excited helium. Choosing either a symmetric or antisymmetric spatial wave function as the initial state results in different scattering cross sections for the 1 s 2 s 1 S and 3 S states. These cross sections are used in the semi-classical model of strong-field ionization. Our investigations show that the photoelectron momentum distributions of rescattered electrons exhibit a significant dependence on the relative spin state of the projectile and the bound electron which should be observable in experiments. The proposed experimental approach can be understood as a testbed for probing the spin dynamics of electrons during strong-field ionization and the presented results as a baseline for their identification.
The strong-field-approximation theory of high-order above-threshold ionization of atoms is generalized to include the electron spin. The obtained rescattering amplitude consists of a direct and exchange part. On the examples of excited He atoms as well as Li+{\mathrm{Li}}^{+}Li+ and Be++{\mathrm{Be}}^{++}Be++ ions, it is shown that the interference of these two amplitudes leads to an observable difference between the photoelectron momentum distributions corresponding to different initial spin states: Pronounced minima appear for singlet states, which are absent for triplet states.
Abstract Spin-dependent effects in atomic processes can be caused by the spin–orbit interaction or/and by the requirement that the wave function of identical electrons is antisymmetric. Such effects are usually neglected in strong-field physics. We show two examples, supported by theoretical results and numerical calculations, in which these effects are important. The first one is based on strong-field ionization of Xe atoms by a bicircular field. The corresponding momentum distribution of spin-polarized electrons emitted in the above-threshold ionization process exhibits wavelength-dependent fast oscillations. For longer wavelengths and small electron emission angle there is a wide photoelectron kinetic energy region in which the spin asymmetry parameter changes continuously from large positive to large negative values. In addition, the emission time of such electrons in high-order above-threshold ionization is determined on the attosecond time scale. The second process considered is high-order above-threshold ionization of excited Li + ions. We have found that in this case, even in the absence of spin–orbit coupling, the photoelectron momentum distribution strongly depends on the initial spin state. In the singlet state we have characteristic minima, which are caused by the destructive interference of the direct and exchange rescattering amplitudes. Such minima are absent in the triplet state.
Abstract In atomic strong field ionization, a photoelectron’s motion is largely determined by the laser pulse’s expected electric field, as well as the atomic potential. However, when the ionization is performed by squeezed light, the photon’s quantum statistics can modify these dynamics. In this work, we generalize the classical trajectory Monte–Carlo technique to study strong field ionization by squeezed states of light. We find that electrons driven by phase-squeezed pulses exhibit increases in longitudinal momentum consistent with what is expected from the field statistics. Meanwhile, the transverse momentum distribution shows varying influence of ‘hard’ and ‘soft’ rescattering off the Coulomb potential, and the proportion of electrons recaptured as Rydberg states decreases monotonically with the amount of squeezed light applied. This work demonstrates the added experimental control over ultrafast electron dynamics achievable by tuning light’s quantum statistics, as well as the essential role of the atomic potential in strong field ionization.
Using field ionization combined with the direct detection of excited neutral atoms we measured the distribution of principal quantum number n of excited He Rydberg states after strong-field excitation at laser intensities well in the tunneling regime. Our results confirm theoretical predictions from semiclassical and quantum mechanical calculations and simultaneously underpin the validity of the semiclassical frustrated tunneling ionization model. Moreover, since our experimental detection scheme is spin sensitive in the case of He atoms, we show that strong-field excitation leads to strong population of triplet states. The origin of it lies in the fact that high angular momentum states are accessible in strong-field excitation. Thus, singlet-triplet transitions become possible due to the increased importance of spin-orbit interaction rather than due to direct laser induced spin-flip processes.
The ionization of the prealigned nitric oxide molecule by strong circularly polarized laser fields is studied via theoretical simulations of the spin-resolved photoelectron momentum distributions by solving numerically the three-dimensional time-dependent Schr\"odinger equation. Due to the spin-orbit entanglement in the ground state of nitric oxide and the sensitivity of the tunnel ionization of its doubly degenerate valence $2{\ensuremath{\pi}}_{\ifmmode\pm\else\textpm\fi{}}$ orbitals carrying opposite electron ring currents to the sense of the laser-field rotation, the momentum-resolved spin-polarized photoelectrons are produced. We show that the spin polarization exhibits strong dependence on the kinetic energy as well as the emitting angle of the photoelectron. In addition to the laser control, the momentum gate in strong-field experiments would enable full control of the spin polarization.
Abstract Ionization of laser-dressed atomic helium is investigated with focus on photoelectron angular distributions stemming from two-color multi-photon excited states. The experiment combines extreme ultraviolet (XUV) with infrared (IR) radiation, while the relative polarization and the temporal delay between the pulses can be varied. By means of an XUV photon energy scan over several electronvolts, we get access to excited states in the dressed atom exhibiting various binding energies, angular momenta, and magnetic quantum numbers. Furthermore, varying the relative polarization is employed as a handle to switch on and off the population of certain states that are only accessible by two-photon excitation. In this way, photoemission can be suppressed for specific XUV photon energies. Additionally, we investigate the dependence of the photoelectron angular distributions on the IR laser intensity. At our higher IR intensities, we start leaving the simple multi-photon ionization regime. The interpretation of the experimental results is supported by numerically solving the time-dependent Schrödinger equation in a single-active-electron approximation. Graphic abstract