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Physical Review A

Spin-dependent quantum theory of high-order above-threshold ionization

Danilo Zille, D. Seipt, Max Möller, S. Fritzsche, G. G. Paulus, Dejan B. Milošević

Published Jun 12, 2017• 8 citations
Publisher

Abstract

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 ${\mathrm{Li}}^{+}$ and ${\mathrm{Be}}^{++}$ 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.

DOI
10.1103/physreva.95.063408

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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 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.
Quantum theory of high-order above-threshold ionization (HATI) of atoms, prepared in a coherent superposition of bound states, by a strong laser field is formulated. Numerical results are obtained using the solutions of the time-dependent Schr\"odinger equation and the improved strong-field approximation. As an example, coherent superposition of the excited 2s2s2s and 2p2p2p states of the He atom is used. Applying a two-level model, it is shown how the relative amplitude and phase of the states in this coherent superposition can be controlled with a weak resonant laser pulse. Numerical results presented for HATI by a strong nonresonant probe laser pulse confirm that the photoelectron spectra and the momentum distributions strongly depend on the relative phase of the states in the prepared coherent superposition. For the case of HATI by a strong resonant laser pulse, we modify our strong-field-approximation theory by applying the two-level model to describe the time evolution of the atomic bound state before the instant of ionization. Contrary to the HATI from a single state by a long laser pulse, the corresponding photoelectron spectra of HATI from the coherent superposition of states depend on the carrier-envelope phase of the resonant ionizing pulse. Therefore, the strong-field ionization from a coherent superposition of states by a resonant laser pulse can be used to determine the carrier-envelope phase for long pulses for which the standard methods such as stereo--above-threshold ionization technique fail. The results strongly depend on the relative amplitude and phase of states in the coherent superposition of states, which can be controlled with a weak resonant laser pulse.
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.
We consider an analytic approach to the elucidation of the role played by Coulomb interaction in the formation of the spectrum and angular distributions of the electrons produced by above threshold ionization of the atoms. Our approach is based on allowance for the multiple scattering of a photoelectron by the Coulomb potential of the residual ion, with pickup of a field photon in each scattering act. The amplitude of a process with direct ionization of the atom and subsequent scattering of the photoelectron in the continuum by the Coulomb potential of the residual ion are found.
Squeezed coherent quantum light is described by the complex squeeze parameter ζ = s e i ϑ and the coherent-state displacement parameter β = | β | e i ϕ β . Our study of strong-field ionization [D. Habibović and D. B. Milošević, ], which focused on bright squeezed vacuum quantum light with β = 0 and s ≫ 1 , is extended to ionization by squeezed coherent light. It is shown that the amplitudes s and | β | strongly influence the ionization process, whereas phases ϑ and ϕ β play a less significant role. The present work provides a unified treatment of coherent, squeezed vacuum, and squeezed coherent light within a single theoretical framework. The quantum nature of the driving field is incorporated by averaging the strong-field ionization probability over the Husimi-Kano phase-space distribution. Using neon as a representative target, we analyze how the parameters characterizing squeezed coherent light modify photoelectron spectra and intensity-dependent enhancements. We show that nonclassical photon statistics can lead to a pronounced steepening of the rescattering plateau and, at low mean intensities, to an effective suppression of the nominal high-energy cutoff. These effects originate from the reduced weight of high-intensity field components inherent to squeezed states and have no analog in strong-field ionization driven by a coherent light. Our results highlight the potential for quantum-statistical control of strong-field ionization and provide a foundation for exploring laser-matter interactions driven by quantum light.