Abstract The rapid advancements of ultrafast intense laser technology have opened new avenues for investigating entanglement in laser-induced systems. However, the application of these advances in quantum technology requires a reliable and universally applicable method for enhancing and regulating entanglement. Here we demonstrate how a few-cycle intense laser field can significantly enhance the degree of entanglement compared to its multi-cycle counterpart, using the example of electron–electron entanglement of orbital angular momentum (OAM) states in recollision-excitation non-sequential double ionization of Ar atoms. By confining the ionization dynamics to a specific narrow time window, the few-cycle pulse purifies the electron trajectories, thereby ensuring high coherence between entangled OAM channels and enhancing entanglement. Furthermore, the degree of entanglement can be efficiently modulated by varying the carrier envelope phase of the few-cycle laser pulse, which is achieved by altering the population across OAM channels. Optimizing coherence through electron trajectory purification with a designed specific temporal waveform of laser field provides a general pathway for enhancing entanglement in laser-induced systems.
Abstract The rapid advancements of ultrafast intense laser technology have opened new avenues for investigating entanglement in laser-induced systems. However, the application of these advances in quantum technology requires a reliable and universally applicable method for enhancing and regulating entanglement. Here we demonstrate how a few-cycle intense laser field can significantly enhance the degree of entanglement compared to its multi-cycle counterpart, using the example of electron–electron entanglement of orbital angular momentum (OAM) states in recollision-excitation non-sequential double ionization of Ar atoms. By confining the ionization dynamics to a specific narrow time window, the few-cycle pulse purifies the electron trajectories, thereby ensuring high coherence between entangled OAM channels and enhancing entanglement. Furthermore, the degree of entanglement can be efficiently modulated by varying the carrier envelope phase of the few-cycle laser pulse, which is achieved by altering the population across OAM channels. Optimizing coherence through electron trajectory purification with a designed specific temporal waveform of laser field provides a general pathway for enhancing entanglement in laser-induced systems.
Quantum excitation is usually regarded as a transient process occurring instantaneously, leaving the underlying physics shrouded in mystery. Recent research shows that Rydberg-state excitation with ultrashort laser pulses can be investigated and manipulated with state-of-the-art few-cycle pulses. We theoretically find that the efficiency of Rydberg state excitation can be enhanced with a short laser pulse and modulated by varying the laser intensities. We also uncover new facets of the excitation dynamics, including the launching of an electron wave packet through strong-field ionization, the re-entry of the electron into the atomic potential and the crucial step where the electron makes a U-turn, resulting in twin captures into Rydberg orbitals. By tuning the laser intensity, we show that the excitation of the Rydberg state can be coherently controlled on a sub-optical-cycle timescale. Our work paves the way toward ultrafast control and coherent manipulation of Rydberg states, thus benefiting Rydberg-state-based quantum technology.
Quantitative control and measurement of quantum entanglement are essential for advancing quantum technologies. Photoionization induced by ultrashort laser pulses provides a unique platform for studying entanglement between photoelectrons and residual ions, representing one of the most intriguing quantum phenomena in attosecond physics. Although extensive studies have focused on the coherence properties within either the emitted electrons or the ions individually, the electron-ion entanglement has remained largely unexplored. In this work, we bridge this gap by investigating the resonance-enhanced multiphoton ionization of argon atoms driven by two time-delayed ultrashort ultraviolet pulses. Employing state-of-the-art first-principles multi-electron simulations, we demonstrate the ability to reconstruct and precisely manipulate the purity of electron quantum states through detailed analysis of the photoelectron angular distributions. Our results reveal distinct scattering-phase differences among various electron configurations within the same partial wave channel, providing unequivocal evidence of electron-ion correlation and entanglement. With the fast development of free-electron lasers, this study establishes an experimentally feasible framework for directly controlling quantum entanglement in ultrafast ionization processes, offering new insights and powerful methodologies for exploring complex electron dynamics in many-electron systems.
We investigate the time evolution of quantum entanglement between an electron, liberated by a strong few-cycle laser pulse, and its parent ion core. Since the standard procedure is numerically prohibitive in this case, we propose a method to quantify the quantum correlation in such a system: we use the reduced density matrices of the directional subspaces along the polarization of the laser pulse and along the transverse directions as building blocks for an approximate entanglement entropy. We present our results, based on accurate numerical simulations, in terms of several of these entropies, for selected values of the peak electric-field strength and the carrier-envelope phase difference of the laser pulse. The time evolution of the mutual entropy of the electron and the ion-core motion along the direction of the laser polarization is similar to our earlier results based on a simple one-dimensional model. However, taking into account also the dynamics perpendicular to the laser polarization reveals a surprisingly different entanglement dynamics above the laser intensity range corresponding to pure tunneling: the quantum entanglement decreases with time in the over-the-barrier ionization regime.
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.
Entanglement has a capacity to enhance imaging procedures, but this remains unexplored for attosecond imaging. Here, we elucidate that possibility, addressing orbital angular momentum (OAM) entanglement in ultrafast processes. In the correlated process non-sequential double ionization (NSDI) we demonstrate robust photoelectron entanglement. In contrast to commonly considered continuous variables, the discrete OAM allows for a simpler interpretation, computation, and measurement of entanglement. The logarithmic negativity reveals that the entanglement is robust to incoherence and an entanglement witness minimizes the number of measurements to detect the entanglement, both quantities are related to OAM coherence terms. We quantify the entanglement for a range of targets and field parameters to find the most entangled photoelectron pairs. This methodology provides a general way to use OAM to quantify and measure entanglement, well-suited to attosecond processes, and can be exploited to enhance imaging capabilities through correlated measurements, or for generation of OAM-entangled electrons.
Controlling electronic decoherence in molecules is an outstanding challenge in chemistry. Recent advances in the theory of electronic decoherence [B. Gu and I. Franco, J. Phys. Chem. Lett. 9, 773 (2018)] have demonstrated that it is possible to manipulate the rate of electronic coherence loss via control of the relative phase in the initial electronic superposition state. This control emerges when there are both relaxation and pure-dephasing channels for decoherence and applies to initially separable electron-nuclear states. In this paper, we demonstrate that (1) such an initial superposition state and the subsequent quantum control of electronic decoherence can be created via weak-field one-photon photoexcitation with few-cycle laser pulses of definite carrier envelope phase (CEP), provided the system is initially prepared in a separable electron-nuclear state. However, we also demonstrate that (2) when stationary molecular states (which are generally not separable) are considered, such one-photon laser control disappears. Remarkably, this happens even in situations in which the initially factorizable state is an excellent approximation to the stationary state with fidelity above 98.5%. The laser control that emerges for initially separable states is shown to arise because these states are superpositions of molecular eigenstates that open up CEP-controllable interference routes at the one-photon limit. Using these insights, we demonstrate that (3) the laser control of electronic decoherence from stationary states can be recovered by using a two-pulse control scheme, with the first pulse creating a vibronic superposition state and the second one inducing interference. This contribution advances a viable scheme for the laser control of electronic decoherence and exposes a surprising artifact that is introduced by widely used initially factorizable system-bath states in the field of open quantum systems.