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Optica

Shaping long-lived electron wavepackets for customizable optical spectra

Rumen Dangovski, Nicholas Rivera, Marin Soljacic A, Ido E. Kaminer

Published Aug 19, 2019• 0 citations
Publisher

Abstract

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.

DOI
10.1364/optica.6.001089

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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.
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.
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.
This work presents a general framework for quantum interference between processes that can involve different fundamental particles or quasi-particles. This framework shows that shaping input wavefunctions is a versatile and powerful tool for producing and controlling quantum interference between distinguishable pathways, beyond previously explored quantum interference between indistinguishable pathways. Two examples of quantum interference enabled by shaping in interactions between free electrons, bound electrons, and photons are presented: i) the vanishing of the zero-loss peak by destructive quantum interference when a shaped electron wavepacket couples to light, under conditions where the electron's zero-loss peak otherwise dominates; ii) quantum interference between free electron and atomic (bound electron) spontaneous emission processes, which can be significant even when the free electron and atom are far apart, breaking the common notion that a free electron and an atom must be close by to significantly affect each other's processes. Conclusions show that emerging quantum wave-shaping techniques unlock the door to greater versatility in light-matter interactions and other quantum processes in general.
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.