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arXiv:1912.05896 · Journal of Physics B Atomic Molecular and Optical Physics

Vibronic coupling induced by fast Rabi oscillations for kinetic energy control in free atom

Andrei V. Ivanov, Evgeniy Perlin

Published Aug 17, 2020• 1 citation
arXivHTMLPDF

Abstract

Abstract Vibronic coupling effects usually manifest themselves in molecules and crystals rather than in unbound atoms. We theoretically demonstrate the existence of vibronic states in a moving two-level atom exposed to a strong electromagnetic (EM) wave. In this case, the Rabi oscillations of the electron density give rise to periodic displacements of the atomic nucleus with the Rabi frequency. The periodic displacements mix the Stark split electron levels and lead to the establishment of a channel for energy transfer in the atomic system. Such a channel paves the way for fast control of the kinetic energy of a free atom with the use of the parameters of an EM wave. Thus, the system kinetic energy can be decreased or increased if the detuning between the laser pulse frequency and the optical transition is positive or negative, respectively. For actual values of the detuning, the pulse duration should be an order of magnitude longer than the lifetime of the excited atomic level in order to complete the energy transfer process.

DOI
10.1088/1361-6455/abb012

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•Sep 3, 2026•0 citations
Abstract Vibronic coupling effects usually manifest themselves in molecules and crystals rather than in unbound atoms. We theoretically demonstrate the existence of vibronic states in a moving two-level atom exposed to a strong electromagnetic (EM) wave. In this case, the Rabi oscillations of the electron density give rise to periodic displacements of the atomic nucleus with the Rabi frequency. The periodic displacements mix the Stark split electron levels and lead to the establishment of a channel for energy transfer in the atomic system. Such a channel paves the way for fast control of the kinetic energy of a free atom with the use of the parameters of an EM wave. Thus, the system kinetic energy can be decreased or increased if the detuning between the laser pulse frequency and the optical transition is positive or negative, respectively. For actual values of the detuning, the pulse duration should be an order of magnitude longer than the lifetime of the excited atomic level in order to complete the energy transfer process.
The resonance fluorescence from a vibronic system with displaced potential-energy surfaces is studied. Because of the equal vibrational frequencies in the two electronic quantum states, a large number of vibronic transitions can be excited by a strong laser field. Even in the case of weaker driving fields, nonperturbative effects may be observed provided that the vibrational relaxation is slow enough. If the vibronic coupling is not extremely strong, the Rabi oscillations will arise mainly from the excitation of the vibrationless transition. Furthermore, the damping of the Rabi oscillations may be accompanied by a substantial decrease in intensity.
We propose free-electron Rabi oscillation by creating an isolated two-level system in a synthetic energy space induced by laser. The π/2-pulse and π-pulse in synthetic Rabi dynamics can function as 'beam splitters' and 'mirrors' for free-electron interferometry, allowing us to detect local electromagnetic fields and plasmonic excitations. When the coupling field is quantized, we can observe quantum and vacuum Rabi oscillations of the two-level electron, which can be used to investigate the quantum statistics of optical excitations and electron-photon entanglement. Recent advances in laser control of electron microscopes and spectroscopes makes the experimental detection of synthetic Rabi oscillations possible. However, observing the quantum Rabi oscillation of electrons remains challenging. Our work has the potential to advance various fundamentals and applications of resonant light-matter interactions between low-energy electrons and quatum light.
Rabi oscillations reflect the existence of a coherent superposition of two molecular eigenstates during the interaction of molecules with a strong, resonant electromagnetic field. This phenomenon is not restricted to two-level systems. We demonstrate its occurrence in a three-level system where the radiation induces a two-photon absorption. The intermediate level is (slightly) detuned from resonance. For a theoretical description the dressed-state picture is adopted. The two-photon excitation is performed either by using one laser, yielding a one-color two-photon process, or by using two counterpropagating, spatially overlapping laser beams, yielding a two-color two-photon process. Rabi oscillations are produced by varying the fluence, i.e., by changing either the laser power or the molecule-laser interaction time. For the one-color case the two-photon transition dipole moment for an SF6{\mathrm{SF}}_{6}SF6​ transition has been determined from the relation between laser fluence and number of Rabi oscillations. For the two-color cases the detuning with the intermediate level is varied by tuning the respective laser frequencies while keeping the sum frequency constant. A dramatic change in the degree of excitation as a function of the intermediate detuning has been observed. \textcopyright{} 1996 The American Physical Society.
Motivated by experimental advances that the collective excitation of two Rydberg atoms was observed, we provide an elaborate theoretical study for the dynamical behavior of two-atom Rabi oscillations. In the large-intermediate-detuning case, the two-photon Rabi oscillation is found to be significantly affected by the strength of the interatomic van der Waals interaction. With a careful comparison of the exact numbers and values of the oscillation frequency, we propose a new way to determine the strength of excitation blockade, agreeing well with the previous universal criterion for full, partial, and no blockade regions. In the small-intermediate-detuning case, we find a blockade-like effect, but the collective enhancement factor is smaller than 2 due to the quantum interference of double optical transitions involving the intermediate state. Moreover, a fast two-photon Rabi oscillation in ns timescale is manifested by employing intense lasers with an intensity of ∼ MW/cm 2 , offering a possibility of ultrafast control of quantum dynamics with Rydberg atoms.
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.
This thesis investigates quantum dynamics induced in atoms by ultrashort pulses of light. The work is motivated by recent developments in free-electron lasers, which generate ultrashort pulses of intense, coherent light and enable coherent control of quantum dynamics. We develop theoretical models to study the processes of absorption and emission in laser-atom interactions. Additionally, we study photoionisation, which creates an ion and an electron, and the entanglement that can be generated between these particles. Finally, we have investigated how the spontaneous decay of the ion induces entanglement transfer from the ion-electron pair to the electron-photon pair.This thesis compiles seven papers. Paper I investigates the absorption of light from an attosecond pulse by an atom in a prepared coherent superposition of states. We show how the evolution of the phase of the superposition wave packet influences the attosecond transient absorption spectra. Paper II predicts the existence of Mollow-like triplets in the absorption spectra of strongly coupled atoms. We establish the conditions for the pulse envelope under which this triplet pattern can be supported.Paper III studies two-photon Rabi oscillations, establishing which systems can sustain such dynamics. We find that a two-photon Rabi oscillating system can induce giant counter-rotating oscillations in the population dynamics, enabling investigations of physical effects beyond the rotating-wave approximation.Paper IV studies ionisation from an atom strongly coupled by a dichromatic field, where interference between the two frequency components shapes the temporal symmetry of the atomic dynamics, allowing for coherent control of the photoelectron distribution.Paper V considers an experiment performed at a Free-Electron Laser facility where a helium atom is ionised and the resulting ion is subsequently strongly coupled. The photoelectron spectra are theoretically reproduced and the entanglement between the ion and photoelectron is studied. Paper VI investigates how the entanglement in the ion--electron pair, generated via photoionisation followed by strong coupling, can be coherently controlled by harnessing the time symmetry of the pulse. We find that the observable manifestation of the entanglement can be altered in such a way that the electron energy becomes associated with the ionic state, allowing the entanglement to be detected via coincidence measurements. Paper VII investigates how quantum correlations between the ion and the electron can be coherently controlled by sequential strong coupling of the ion. We find that both the build-up of entanglement and its manifestation can be controlled, and we establish a quantitative measure of the amplitude entanglement that explains the dynamics in an intuitive way. Paper VIII studies the process of entanglement transfer induced by the spontaneous decay of the ion. We find that the ion--electron entanglement generated during the ultrashort interaction with the laser field is transferred to the electron--photon system over the much longer timescale of fluorescence.