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Physical Review A

High-order above-threshold ionization from a coherent superposition of states

Dejan B. Milošević, Benjamin Fetić, Predrag Ranitovic

Published Jul 15, 2022• 9 citations
Publisher

Abstract

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 $2s$ and $2p$ 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.

DOI
10.1103/physreva.106.013109

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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.
We investigate high-order above-threshold ionization (HATI) from intense quantum light-atom interaction, by numerically solving the fully quantum time-dependent Schr\"odinger equation based on quantum electrodynamics theory. Our simulations show that, in comparison with coherent-state (classical) light, the HATI spectra from intense quantum lights may have a higher cutoff energy and, moreover, for a given ponderomotive energy of the laser field, the cutoff energy is dependent on the laser wavelength and the ionization potential of the atom. The influence of quantum light on the HATI is revealed by examining the interplay between a quasiprobability distribution of the electric field of the quantum light and the Ammosov-Delone-Krainov ionization rate of the atom. Furthermore, analytical formulas of the cutoff energy of the HATI spectra for different quantum lights are derived.
It is shown that the rate and degree of ionization of an atom can be controlled by preparing a specific superposition of Rydberg states. This effect is due to the Raman interaction of Rydberg levels via resonant lower-lying levels of the atom. Depending on the initial population of an atom interacting with a strong laser field, the atom either ionizes completely or exhibits an extremely high degree of stability (in this case the probability of the atom remaining in a bound state when the laser pulse is switched off is close to 1). It is shown that states which are stable against ionization decay or, conversely, decay rapidly into the continuum can be prepared using double laser pulses with a controllable time delay.
The quantum dynamics of a two-level system illuminated by a few-cycle pulse with an adjustable carrier-envelope (C-E) phase is investigated theoretically. We consider the weak-field regime where tunneling processes and multiphoton ionization are negligible. It is shown that the upper state population exhibits a strong dependence on the C-E phase and on the time of arrival of the few-cycle pulse if the system is initially prepared in a coherent superposition state. We demonstrate that this effect can be employed to probe the coherence properties of the superposition state and allows one to determine the phase of the laser that prepares this state.
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.
We present a theoretical study of the main characteristics of two-color photoionization spectra obtained when atoms are subjected to an intense radiation pulse containing the fundamental of an infrared laser and one of its higher harmonics. The frequency of the latter is chosen to be high enough that the atom can be ionized by a single photon. The calculation is performed by numerical integration of the time-dependent Schrödinger equation for a (three-dimensional) hydrogen atom. We present the general properties of the spectra and angular distributions as well as the possible occurrence of interferences between the laser-assisted process and above-threshold ionization. Our results indicate that such interference effects, which can lead to partial coherent control of the photoionization process, can be observed at moderate laser intensities within the reach of currently operated laser and harmonic sources.
A model which describes the time evolution of strong-field photoionization of atoms is presented. Based on the numerical solution of the non-stationary Schrodinger equation, the model allows one to predict and to interpret the results of experiments on double photoionization of atoms by a combined action of a very short (attosecond) XUV pulse and a few-cycle IR pulse of a powerful laser at various delay times between the two pulses. Depending on the binding energy of the ionized electron, two types of processes are considered. If the electron is tightly bound (Ne case), the XUV pulse ionizes the atom and shakes up another (outer) electron to an excited state, which is subsequently ionized by the strong IR field. For an atom with a weakly bound outer electron (Li case), the IR field ionizes the latter, while the XUV pulse, ionizing the inner shell, terminates (or suppresses) the strong-field ionization. In both cases the yield of doubly ionized ions strongly depends on the delay time between the two pulses, revealing 'steps', oscillations and other features which characterize the time evolution of the ionization process. The presented model describes qualitatively the results of recent experiments on Ne.