The influence of ultrashort low-frequency laser pulses of different intensities and pulse lengths on the dynamics of a resonantly driven atomic system is investigated theoretically. We demonstrate the periodical dependence of the total ionization rate on the appearance time of a strong few-cycle laser pulse. By depleting the excited state, the intense short pulse not only resets the Rabi oscillations, but also introduces a time shift that is proportional to the pulse length. This time shift can be employed to determine the ultrashort pulse length. In the case of ultrashort pulses with lower intensities, we observe side-bands in the two-photon ionization spectrum, whose intensities vary periodically with the appearance time of the pulse. This can be utilized to measure the period of Rabi oscillations. We have developed an S-matrix theory of two-colour ionization which can explain some of the observations of our numerical calculations. Furthermore, we have studied the high harmonic generation spectra as well as the attosecond pulses generated from the high harmonics. We show that the Rabi oscillation can be used to alter the ionization rate within laser sub-cycles and therefore select different quantum trajectories in the high harmonics generation.
The influence of ultrashort low-frequency laser pulses of different intensities and pulse lengths on the dynamics of a resonantly driven atomic system is investigated theoretically. We demonstrate the periodical dependence of the total ionization rate on the appearance time of a strong few-cycle laser pulse. By depleting the excited state, the intense short pulse not only resets the Rabi oscillations, but also introduces a time shift that is proportional to the pulse length. This time shift can be employed to determine the ultrashort pulse length. In the case of ultrashort pulses with lower intensities, we observe side-bands in the two-photon ionization spectrum, whose intensities vary periodically with the appearance time of the pulse. This can be utilized to measure the period of Rabi oscillations. We have developed an S-matrix theory of two-colour ionization which can explain some of the observations of our numerical calculations. Furthermore, we have studied the high harmonic generation spectra as well as the attosecond pulses generated from the high harmonics. We show that the Rabi oscillation can be used to alter the ionization rate within laser sub-cycles and therefore select different quantum trajectories in the high harmonics generation.
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.
We investigate the third order harmonic generation for model atoms interacting with intense short laser pulses. We focus on the cases where the ponderomotive energy is not big enough to generate high-order harmonics, and where resonant transitions between bound states are also as important as multi-photon ionization and low-order harmonic generation. We find that the third order harmonic intensity from a model hydrogen atom can decrease as the laser frequency draws near a resonance between bound states. We explain this result by looking into the ionization and Rabi oscillation from the numerical calculation of the time-dependent 1-D Schrödinger equation. In order to support our explanation we also investigate the populations of bound states that play an important role in this atomic process.
We demonstrate Rabi oscillations in nonlinear ionization of argon by an intense femtosecond extreme ultraviolet (XUV) laser field produced by high-harmonic generation. We monitor the formation of Ar2+ as a function of the time delay between the XUV pulse and an additional near-infrared (NIR) femtosecond laser pulse, and show that the population of an Ar+∗ intermediate resonance exhibits strong modulations both due to an NIR laser-induced Stark shift and XUV-induced Rabi cycling between the ground state of Ar+ and the Ar+∗ excited state. Our experiment represents a direct experimental observation of a Rabi-cycling process in the XUV regime.
Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
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.