We study the dynamics of quantum matter interacting with time-energy entangled photons. We consider the stimulation of a collective mode of a two-dimensional material by means of one of the two partners of a time-energy entangled pair of photons. Using an exactly solvable model, we analyze the out-of-equilibrium properties of both light and matter degrees of freedom, and show how entanglement in the incident photons deeply modifies relevant time scales of the light-matter interaction process. We find that entanglement strongly suppresses the delay between the transmission and absorption events, which become synchronous in the limit of strongly entangled wave packets. By comparing numerical simulations with analytic modeling, we trace back this behavior to the representation of entangled wave packets in terms of a superposition of multiple train pulses containing an increasing number of ultrashort non-entangled packets. As a result, we show that the entangled driving allows the creation of a matter excitation on a time scale shorter than the temporal width of the pulse. Eventually, by analyzing temporal correlations of the excited matter degrees of freedom, we show that driving with entangled photons imprints characteristic temporal correlations of time-energy entangled modes in the matter degree of freedom.
We study the dynamics of quantum matter interacting with time-energy entangled photons. We consider the stimulation of a collective mode of a two-dimensional material by means of one of the two partners of a time-energy entangled pair of photons. Using an exactly solvable model, we analyze the out-of-equilibrium properties of both light and matter degrees of freedom, and show how entanglement in the incident photons deeply modifies relevant time scales of the light-matter interaction process. We find that entanglement strongly suppresses the delay between the transmission and absorption events, which become synchronous in the limit of strongly entangled wave packets. By comparing numerical simulations with analytic modeling, we trace back this behavior to the representation of entangled wave packets in terms of a superposition of multiple train pulses containing an increasing number of ultrashort non-entangled packets. As a result, we show that the entangled driving allows the creation of a matter excitation on a time scale shorter than the temporal width of the pulse. Eventually, by analyzing temporal correlations of the excited matter degrees of freedom, we show that driving with entangled photons imprints characteristic temporal correlations of time-energy entangled modes in the matter degree of freedom.
Energy-time entangled photons are critical in many quantum optical phenomena and have emerged as important elements in quantum information protocols. Entanglement in this degree of freedom often manifests itself on ultrafast time scales, making it very difficult to detect, whether one employs direct or interferometric techniques, as photon-counting detectors have insufficient time resolution. Here, we implement ultrafast photon counters based on nonlinear interactions and strong femtosecond laser pulses to probe energy-time entanglement in this important regime. Using this technique and single-photon spectrometers, we characterize all the spectral and temporal correlations of two entangled photons with femtosecond resolution. This enables the witnessing of energy-time entanglement using uncertainty relations and the direct observation of nonlocal dispersion cancellation on ultrafast time scales. These techniques are essential to understand and control the energy-time degree of freedom of light for ultrafast quantum optics.
Abstract The ability to modify light−matter coupling in time (e.g. using external pulses) opens up the exciting possibility of generating and probing new aspects of quantum correlations in many-body light–matter systems. Here we study the impact of such a pulsed coupling on the light–matter entanglement in the Dicke model as well as the respective subsystem quantum dynamics. Our dynamical many-body analysis exploits the natural partition between the radiation and matter degrees of freedom, allowing us to explore time-dependent intra-subsystem quantum correlations by means of squeezing parameters, and the inter-subsystem Schmidt gap for different pulse duration (i.e. ramping velocity) regimes—from the near adiabatic to the sudden quench limits. Our results reveal that both types of quantities indicate the emergence of the superradiant phase when crossing the quantum critical point. In addition, at the end of the pulse light and matter remain entangled even though they become uncoupled, which could be exploited to generate entangled states in non-interacting systems.
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.
We propose an extension of coherent control using laser-synthesized free-electron matter waves. In contrast to coherent control schemes exploiting optical coherences to steer the dynamics of matter waves, we analyze the opposite and investigate the control of quantum light emission driven by laser-sculpted coherent free-electron matter waves. We apply this concept to the control of entangled photon-pair emission in electron-atom collisions, in which the incident electron wave packet, colliding with a target atom B, is engineered by interferometric resonantly enhanced multiphoton ionization of a parent atom A. Each ionization pathway leads to electron wave packets that coherently interfere during temporal evolution in the continuum. Their mutual coherence can be controlled by adjusting the relative phases or time delays of the frequency components of the ionizing field contributing to the interfering pathways. We report coherent control of entangled photon-pair generation in radiative photocascade emission upon decay of the target atom after inelastic excitation triggered by the collision with the synthesized electron wave packet.
Quantum light is increasingly recognized as a promising resource for developing optical measurement techniques. Particular attention has been paid to enhancing the precision of the measurements beyond classical techniques by using nonclassical correlations between quantum entangled photons. Recent advances in the quantum optics technology have made it possible to manipulate spectral and temporal properties of entangled photons, and photon correlations can facilitate the extraction of matter information with relatively simple optical systems compared to conventional schemes. In these respects, the applications of entangled photons to time-resolved spectroscopy can open new avenues for unambiguously extracting information on dynamical processes in complex molecular and materials systems. Here, we propose time-resolved spectroscopy in which specific signal contributions are selectively enhanced by harnessing nonclassical correlations of entangled photons. The entanglement time characterizes the mutual delay between an entangled twin and determines the spectral distribution of photon correlations. The entanglement time plays a dual role as the knob for controlling the accessible time region of dynamical processes and the degrees of spectral selectivity. In this sense, the role of the entanglement time is substantially equivalent to the temporal width of the classical laser pulse. The results demonstrate that the application of quantum entangled photons to time-resolved spectroscopy leads to monitoring dynamical processes in complex molecular and materials systems by selectively extracting desired signal contributions from congested spectra. We anticipate that more elaborately engineered photon states would broaden the availability of quantum light spectroscopy.
For decades, ultrafast light-matter interactions have provided a powerful means to observe electrons in motion across a wide range of physical systems. This dissertation builds new theoretical frameworks to make sense of the emergent phenomena that arise when light drives matter into the strong-field regime, spanning atomic, molecular, and condensed-matter systems. The resulting dynamics leave their fingerprints on a variety of observables, such as photoionization spectra, high-harmonic generation, and nonlinear spectroscopic signals, each of which provides a different window onto the underlying electronic motion. The work is organized into two parts.The first part focuses on the electric-field observables of nonlinear optical signals. Because both the amplitude and phase of the emitted field are experimentally accessible through techniques such as spectral interferometry and electro-optic sampling, the full field itself serves as a rich observable for characterizing nonlinear responses in atomic, molecular, and condensed-matter systems. Leveraging this, the simulations presented here uncover novel and largely unexplored physical phenomena encoded in these field observables. The second part turns to optical spectroscopy with quantum light. Although nonlinear optical processes are conventionally modeled within a semiclassical framework, treating the matter quantum mechanically while the driving ultrafast fields remain classical, the resulting signals can nonetheless exhibit intrinsically non-classical properties. Building on this insight, a framework for interpreting experimental data is introduced and used to show that four-wave mixing driven by ultrafast femtosecond laser pulses generates bright squeezed light. Beyond squeezed light, strong field-matter interactions can also produce attosecond entangled photons, a distinct form of quantum light. Several strategies are proposed to enhance the efficiency of their generation, with the developed theory predicting rates of energy-time entangled biphoton production orders of magnitude beyond those achievable with conventional spontaneous parametric down-conversion (SPDC) sources. The studies presented here are initial steps toward investigating quantum properties of these systems through quantum phynonlinear spectroscopy, which is not achievable with classical light.