Electrons in atoms and molecules are versatile physical systems covering a vast range of light-matter interactions, enabling the physics of Rydberg states, photon-photon bound states, simulation of condensed matter Hamiltonians, and quantum sources of light. A limitation on the versatility of such electronic systems for optical interactions would appear to arise from the discrete nature of the electronic transitions and from the limited ionization energy, constraining the energy scale through which the rich physics of bound electrons can be accessed. In this work, we propose the concept of shaping spatially confined electron wavepackets as superpositions of extended states in the ionization continuum. These wavepackets enable customizable optical emission spectra transitions in the eV-keV range. We find that the specific shaping lengthens the diffraction lifetime of the wavepackets in exchange for increasing their spatial spreads. Finally, we study the spontaneous radiative transitions of these excited states, examining the influence of the wavepacket shape and size on the radiation rate of the excited state. We observe that the rate of radiative capture is primarily limited by the diffraction lifetime of the wavepacket. The approach proposed in this work could have applications towards developing designer emitters at tunable energy and length scales, potentially bringing the physics of Rydberg states to new energy scales and extending the range and versatility of emitters that can be developed using shaped electrons.
Electrons in atoms and molecules are versatile physical systems covering a vast range of light-matter interactions, enabling the physics of Rydberg states, photon-photon bound states, simulation of condensed matter Hamiltonians, and quantum sources of light. A limitation on the versatility of such electronic systems for optical interactions would appear to arise from the discrete nature of the electronic transitions and from the limited ionization energy, constraining the energy scale through which the rich physics of bound electrons can be accessed. In this work, we propose the concept of shaping spatially confined electron wavepackets as superpositions of extended states in the ionization continuum. These wavepackets enable customizable optical emission spectra transitions in the eV-keV range. We find that the specific shaping lengthens the diffraction lifetime of the wavepackets in exchange for increasing their spatial spreads. Finally, we study the spontaneous radiative transitions of these excited states, examining the influence of the wavepacket shape and size on the radiation rate of the excited state. We observe that the rate of radiative capture is primarily limited by the diffraction lifetime of the wavepacket. The approach proposed in this work could have applications towards developing designer emitters at tunable energy and length scales, potentially bringing the physics of Rydberg states to new energy scales and extending the range and versatility of emitters that can be developed using shaped electrons.
Electrons in atoms and molecules are versatile physical systems allowing a vast range of light–matter interactions. Spontaneous emission, which appears in a wide variety of applications, depends crucially on the bound electron energy levels. The discrete nature of these electron energy levels and the ionization threshold constrain the energy scale of all light–matter interactions involving bound electrons. To bypass these constraints, we take ideas from optical and electronic beam shaping and propose creating new electron states as superpositions of extended states above the ionization threshold. We show that such superpositions enable the control of spontaneous emission with tunable spectra in the eV–keV range. We find that the specific shaping lengthens the diffraction and radiative lifetimes of the wavepackets in exchange for increasing their spatial spreads. Our approach could have applications toward developing novel kinds of light emitters at hard-to-access spectral ranges.
Optically trapped Rydberg atoms are a suitable platform to explore quantum many-body physics mediated by long-range atom-atom interactions that can be engineered through externally applied light fields. However, this approach is limited to dipole-allowed transitions and a spatial resolution of the order of the optical wavelength. Here, we theoretically investigate the interaction between free electrons and individual Rydberg atoms as an approach to induce nondipolar transitions with subnanometer spatial precision and a substantial degree of control over the final atomic states. We observe unity-order excitation probabilities produced by a single electron for suitably chosen combinations of electron energies and electron-beam distance to the atom. We further discuss free-electron-atom entanglement and atom-atom entanglement in combination with lateral shaping of the electron followed by postselection. Our results support free electrons as powerful tools to manipulate Rydberg atoms in previously inaccessible ways.
This thesis is a theoretical study of the behavior of electrons in atoms and molecules subjected to external electromagnetic fields. Three electronic systems have been central in this work, the atomic and quasimolecular Rydberg states and the carbon allotrope graphene. The exaggerated properties of the highly excited Rydberg atoms, such as long lifetime, large spatial extension and low binding energy make them excellent candidates for both theoretical and experimental considerations. The analytical solutions of the hydrogen atom in quantum mechanics provide a good description for most Rydberg atoms. This is exploited in the work presented in this thesis and the accompanying papers, where we show results of numerical computations on interacting Rydberg atoms, with and without the presence of radiating fields, as well as dynamic Rydberg wave packets influenced by a train of femtosecond laser pulses. In the final part of the thesis the optical process of high-order harmonic generation in an extended molecular structure, represented by graphene, is considered. Rydberg atoms have a large dipole moment due to the large average electronic radius in the atom, which leads to a very strong dipole-dipole coupling between interacting particles in a gas of cold Rydberg atoms. This interaction, which is dependent on the internuclear separation between the atoms, induces a shift in the energy levels, which again prohibits the excitation of more than one atom in the gas, an effect commonly known as the Rydberg blockade. A correlated behavior is observed for the intrashell transitions in mutually excited Rydberg atoms. The microwave field driven dynamics is significantly supressed for internuclear distances below a given conditional radius which scales linearly with the principal quantum number n. Such an entangled electronic behavior may open for the realization of quantum gates applied in quantum informatics. The long-range interaction of Rydberg atoms is dominated by the dipole-dipole terms. Nevertheless, the investigation of two interacting Rydberg atoms, without the influence of electromagnetic radiation, has shown that the lower order multipolar terms play a vital role in the energy shifts as well as for the electronic probability distributions. We found that the energy curves, when including all multipole orders, correspond to both repulsive and attractive states with a stronger repulsion than attraction. We also propose a laser assisted approach for stabilization of Rydberg gases by controlled transitions between such attractive and repulsive energy states. Single-electron ionization of a dynamic Rydberg wave packet confined within a single energy level has been investigated. The ionization probability of an intrashell Rydberg wave packet depends strongly on the degree of polarization. For a wave packet driven repeatedly between the circular (least polarized) state and the linear (most polarized) state by a rotating microwave field and subjected to a train of femtosecond laser pulses, the ionization probability will depend crucially on the laser repetition rate and number of pulses. The angular-resolved ionization probability and energy distribution in the continuum are also influenced by these parameters. The last part of the thesis is devoted to the study of high-order harmonic generation (HHG) in graphene. In the simple man’s model HHG can be described by an electron that is ionized and driven in an external field, after which it returns to the parent atom and recombines, emitting a high-energy photon with frequency that is a multiple of the incident laser frequency. We show that the harmonic spectra obtained from the interaction with linearly as well as circularly polarized femtosecond lasers yield harmonics up the classical limit for extended molecules. In contrast to diatomic molecules, the stable grid structure of graphene ensures that the harmonic generation cutoff remains constant with increasing signal power as the graphene diameter extends beyond the classical limit. Additionally, for circularly polarized lasers harmonics exceeding the classical predictions have been observed.
Spontaneous light emission is central to a vast range of physical systems and is a founding pillar for the theory of light–matter interactions. In the presence of complex photonic media, the description of spontaneous light emission usually requires advanced theoretical quantum optics tools such as macroscopic quantum electrodynamics, involving quantized electromagnetic fields. Although rigorous and comprehensive, the complexity of such models can obscure the intuitive understanding of many quantum-optical phenomena. Here, we review a method for calculating spontaneous emission and other quantum-optical processes without making explicit use of quantized electromagnetic fields. Instead, we introduce the concept of transition currents, comprising charges in matter that undergo transitions between initial and final quantum states. We show how predictions that usually demand advanced methods in quantum electrodynamics or quantum optics can be reproduced by feeding these transition currents as sources to the classical Maxwell equations. One then obtains the relevant quantum observables from the resulting classical field amplitudes, without washing out quantum optical effects. We show that this procedure allows for a straightforward description of quantum phenomena, even when going beyond the dipole approximation and single emitters. As illustrative examples, we calculate emission patterns and Purcell-enhanced emission rates in both bound-electron and free-electron systems. For the latter, we derive cathodoluminescence emission and energy-loss probabilities of free electrons interacting with nanostructured samples. In addition, we calculate quantum-beat phenomena in bound-electron systems and wave function-dependent optical coherence in free-electron systems. Remarkably, the transition-current formalism captures more complex phenomena, such as many-body interference effects and super-radiance of both bound- and free-electron systems, second-order processes such as two-photon emission, and quantum recoil corrections to free-electron radiation. We review a variety of light–matter interactions in fields ranging from electron microscopy to nanophotonics and quantum optics, for which the transition-current theoretical formalism facilitates practical simulations and a deeper understanding of novel applications.
Coherent optical modulation of free-electron wavepackets offers a route to ultrafast beam steering, energy exchange, temporal compression, and quantum-state shaping. Recent advances in photon-induced near-field electron microscopy (PINEM), ultrafast Kapitza-Dirac effect (KDE) and dielectric laser acceleration (DLA) have demonstrated strong light-electron coupling, but longitudinal energy modulation, transverse momentum transfer, and wavepacket-dependent diffraction are still commonly described with separate models. Here, we develop a unified Light-Electron Modulation (LEM) framework that treats optical near fields as programmable phase modulators for free-electron wavepackets. Within this framework, we identify longitudinal and transverse modulation channels, analogous to electro-optic phase modulation and acousto-optic diffraction of light, respectively, and show how their operation depends on wavepacket extent, recoil, phase matching, and optical-field geometry. This formulation organizes PINEM, Raman-Nath and Bragg diffraction, DLA-like acceleration, and anomalous PINEM as limiting regimes of a common modulation picture. The resulting framework provides design principles for free-electron modulators that can control energy spectra, temporal density, transverse wavefronts, and electron-photon quantum interfaces, establishing LEM as a device-level platform for programmable femtosecond-to-attosecond matter-wave control.
Summary form only given. Condensed-matter systems are interesting and important to understand, for fundamental science as well as towards more applied objectives in the development of new materials for instance. Unfortunately, these many-body quantum systems are difficult to study: both the theoretical approach and the numerical simulation are proving impossible to carry out to relevant system sizes. Quantum simulation proposes to mimic those out-of-reach systems with more controllable and accessible quantum systems. Rydberg atoms gained renewed interest in the last decades thanks to their very high polarizability, allowing for strong and tunable short-range interactions. They constitute an interesting candidate for a quantum simulation platform. However, low angular momentum Rydberg states have limited, despite relatively long, lifetimes which limit the scope of such a quantum simulator. Moreover, low-l Rydberg states cannot be efficiently laser-trapped. In order to overcome these limitations, we propose to use circular Rydberg states, i.e., of maximum angular momentum. Circular Rydberg states exhibit much longer lifetimes, and can be trapped using laser light. By placing the circular Rydberg atoms inside a spontaneous emission-inhibiting capacitor, we hope to achieve the deterministic preparation of a 1D-chain of 40 atoms, with a collective lifetime of over 2 seconds. With expected exchange energies in the 10-100 kHz range, this would provide a platform capable of simulating quantum many-body physics up to 105exchange times. The first step towards the experimental realization of such a quantum simulator is the demonstration of the laser-trapping of circular Rydberg atoms. To this end, we use a Laguerre-Gauss hollow beam at 1064 nm, imposing a ponderomotive potential on the nearly-free electron of the Rydberg atoms. I will present our latest experimental results of light-trapping of circular Rydberg atoms.