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Physical Review A

Resonant interatomic Coulombic decay in a laser field

C. Hoffmeister, Carsten Müller, Alexander B Voitkiv

Published Apr 6, 2022• 2 citations
Publisher

Abstract

We consider photoionization in a system of two atoms of different species caused by a laser field. In this process an inner-valence vacancy, created by photoexcitation in one of the atoms, decays not only due to intra- but also interatomic electron-electron correlations with the energy release in the latter case being transferred to the other atom which is ionized. We show that when the intensity of the laser field increases this photoionization process---due to Rabi oscillations and Pauli blocking---may acquire qualitatively new features in its time evolution and the electron emission spectra.

DOI
10.1103/physreva.105.042803

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New Journal of Physics•Sep 12, 2013•9 citations
We consider photoionization in a system of two atoms of different species caused by a laser field. In this process an inner-valence vacancy, created by photoexcitation in one of the atoms, decays not only due to intra- but also interatomic electron-electron correlations with the energy release in the latter case being transferred to the other atom which is ionized. We show that when the intensity of the laser field increases this photoionization process---due to Rabi oscillations and Pauli blocking---may acquire qualitatively new features in its time evolution and the electron emission spectra.
Modifications of photoionization arising from resonant electron-electron correlations between neighbouring atoms in an atomic sample are studied. The sample contains atomic species A and B, with the ionization potential of A being smaller than the energy of a dipole-allowed transition in B. The atoms are subject to an external radiation field which is near-resonant with the dipole transition in B. Photoionization of an atom A may thus proceed via a two-step mechanism: photoexcitation in the subsystem of species B, followed by interatomic Coulombic decay. As a basic atomic configuration, we investigate resonant photoionization in a three-atomic system A-B-B, consisting of an atom A and two neighbouring atoms B. It is found that, under suitable conditions, the influence of the neighbouring atoms can strongly affect the photoionization process, including its total probabilty, time development and photoelectron spectra. In particular, by comparing our results with those for photoionization of an isolated atom A and a two-atomic system A-B, respectively, we reveal the characteristic impact exerted by the third atom.
Modifications of photoionization arising from resonant electron–electron correlations between neighbouring atoms in an atomic sample are studied. The sample contains atomic species A and B , with the ionization potential of A being smaller than the energy of a dipole-allowed transition in B . The atoms are subject to an external radiation field which is near resonant with the dipole transition in B . Photoionization of an atom A may thus proceed via a two-step mechanism: photoexcitation in the subsystem of species B , followed by interatomic Coulombic decay. As a basic atomic configuration, we investigate resonant photoionization in a three-atomic system A – B – B consisting of an atom A and two neighbouring atoms B . It is found that, under suitable conditions, the presence of neighbouring atoms can strongly affect the photoionization process, including its total probability, time development and photoelectron spectra. In particular, comparing our results with those for photoionization of an isolated atom A and a two-atomic system A – B , respectively, we reveal the characteristic impact made by the third atom.
Abstract Ionization-excitation of an atom induced by the absorption of a single photon in the presence of a neighboring atom is studied. The latter is, first, resonantly photoexcited and, afterwards, transfers the excitation energy radiationlessly to the other atom, leading to its ionization with simultaneous excitation. The process relies on the combined effects of interatomic and intraatomic electron correlations. Under suitable conditions, it can dominate by several orders of magnitude over direct photoionization-excitation and even over direct photoionization. In addition, we briefly discuss another kind of two-center resonant photoionization with excitation where the ionization and residual excitation in the final state are located at different atomic sites.
In high-intensity laser light, matter can be ionized by direct multiphoton absorption even at photon energies below the ionization threshold. However on tuning the laser to the lowest resonant transition, the system becomes multiply excited, and more efficient, indirect ionization pathways become operative. These mechanisms are known as interatomic Coulombic decay (ICD), where one of the species de-excites to its ground state, transferring its energy to ionize another excited species. Here we show that on tuning to a higher resonant transition, a previously unknown type of interatomic Coulombic decay, intra-Rydberg ICD occurs. In it, de-excitation of an atom to a close-lying Rydberg state leads to electron emission from another neighbouring Rydberg atom. Moreover, systems multiply excited to higher Rydberg states will decay by a cascade of such processes, producing even more ions. The intra-Rydberg ICD and cascades are expected to be ubiquitous in weakly-bound systems exposed to high-intensity resonant radiation.
We analyze theoretically the high intensity photoionization dynamics of a system with two atomic states resonantly coupled by coherent extreme ultraviolet laser radiation that also gives rise to the ionization. The ground state occupation of such a system is shown to exhibit damped Rabi oscillations. The corresponding ionization, which is responsible for the damping, scales almost linearly with the field intensity when the pulse length exceeds the Rabi period. For shorter pulses a quadratic scaling is found. The Rabi frequency is shifted compared to its value for an isolated two-level system. The shift increases with excitation intensity and can acquire a high percentage of the unrenormalized frequency at high intensities. Analytical results obtained within a simplified solvable model demonstrate that the damping and the shift both result from the coupling of the discrete states to the ionization continuum and are therefore closely related. Numerical simulations for a two-electron system reveal at high intensities the importance of off-resonant ionization channels.