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Nature Communications

Interatomic Coulombic decay cascades in multiply excited neon clusters

Kiyonobu Nagaya, Denys Iablonskyi, Nikolay V. Golubev, K. Matsunami, H. Fukuzawa, Koji Motomura, Toshiyuki Nishiyama, Tsukasa Sakai, Tetsuya Tachibana, Subhendu Mondal, S. Wada, Kevin Charles Prince, Carlo Callegari, Catalin Miron, Norio Saitô, Makina Yabashi, Philipp V. Demekhin, Lorenz S. Cederbaum, Alexander I. Kuleff, Mengyu Yao, Kiyoshi Ueda

Published Dec 5, 2016• 33 citations
Publisher

Abstract

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.

DOI
10.1038/ncomms13477

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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 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.
Electronic decay processes provide a fascinating window into correlated electronic rearrangements occurring on ultrafast timescales. Following these dynamics in real time has become increasingly accessible experimentally, but extracting the underlying electronic dynamics from measured spectra requires understanding how nuclear motion shapes the observable signal. Here, we extend an analytical description of time-resolved electronic decay spectra to include dissociative nuclear dynamics and apply it to Interparticle Coulombic Decay (ICD) in the neon dimer. The resulting spectra reproduce the experimentally observed spectral shape and reveal an unexpectedly important role of interference between pathways involving different vibronic resonance states. We further establish a clear connection between the temporal build-up of the spectral structure and the nuclear wavepacket dynamics in the decaying electronic state. Most strikingly, our analytical expressions reveal that the time-dependent integrated ICD signal contains contributions proportional to both exp⁡(−t/τ)\exp(-t/τ)exp(−t/τ) and exp⁡[−t/(2τ)]\exp[-t/(2τ)]exp[−t/(2τ)]. Nevertheless, a conventional mono-exponential fit can describe the temporal signal remarkably well while yielding a decay lifetime that differs substantially from the underlying value. Applying the theoretically derived fitting model to experimental data for the neon dimer yields an ICD lifetime τττ of 73 fs, rather than the previously extracted 150(50) fs, placing the experimental value within the range of previous theoretical predictions. Since the underlying temporal structure is common to electronic decay processes, our findings have implications for extracting lifetimes from time-resolved decay spectra well beyond ICD.
The authors have studied double ionization of Ba 6snl Rydberg states through resonant two-photon excitation of 8snl double-Rydberg states with n=13 and 14 and different l. The laser intensity dependence of Ba 2+ yield measured for l>or=8, when the electrons suffer long-range dipole interaction, shows a decrease from four-photon for l=8 to less than three for l=11. The four-photon dependence is due to autoionization decay populating the Ba + (7p) levels which gives an indirect signature to the Ba 2+ production. By increasing l this decay vanishes and the data show evidence of a direct double-ionization process via planetary-electron states for l>or=10. Additional intensity measurements performed for low l=6 states strongly mixed with 5fn'l' ones by short-range multipole interaction, reveal indirect Ba 2+ production and an individual case of partial stabilization due to destructive interference leading to direct double ionization.
Abstract Understanding Coulomb driven many-body dynamics in ultracold atomic systems far from equilibrium remains an open challenge, particularly when ultrafast excitation channels create competing pathways toward Rydberg gases or ultracold plasmas. Here, we investigate the many-body dynamics in a 87 Rb Bose-Einstein condensate after exposure to a single femtosecond laser pulse. By tuning the laser wavelength across the two-photon ionization threshold, we can control the initial state that is either dominated by free electrons and leads to an ultracold plasma or dominated by electrons in excited states which leads to a dense Rydberg gas. The large bandwidth enables overcoming the Rydberg blockade that limits the excitation density for narrow-linewidth lasers. We directly measure the kinetic energy of the released electrons and compare the final distribution of free, bound and plasma electrons to molecular dynamics simulations where the electrons are modeled as individual particles including collisional ionization and recombination processes. We find very good agreement between the simulated electron distribution and the experimental observation. We identify charge imbalance as main driver for the decay of a dense Rydberg gas into an ultracold plasma.