Determining the quantum state of a given quantum-mechanical system is a fundamental task in physics. Quantum-state tomography has been pivotal for establishing quantum optics [1-4] and for revealing the properties of bound charges in materials [5-7]. An emerging other object for studying and utilizing quantum effects are free electrons, elementary particles that are central to high-resolution microscopy [8,9], electron-based quantum optics [10-17], ul-trafast electron microscopy [18-24] and particle accelerators [25-27]. However, free electrons are intrinsically incoherent, and we lack a broadly applicable method to measure and control their quantum state beyond special cases with discrete energy sidebands [28,29]. Here, we report a universal approach to measure arbitrary free-electron quantum states in continuous variables. Two monochromatic but spectrally shifted laser waves produce interfering quan-tum paths that directly reveal the density matrix and thus all essential properties of the pure wavepackets, the ensemble, and their interlinks. As a first application, we show how the quantum state of a single electron is modified by many-body Coulomb interactions of a sur-rounding electron gas. The reported concepts and results provide insight into otherwise hid-den correlations in electron beams and enable the controlled optimization of exceptional quantum states for free-electron quantum optics or quantum electron microscopy.
Determining the quantum state of a given quantum-mechanical system is a fundamental task in physics. Quantum-state tomography has been pivotal for establishing quantum optics [1-4] and for revealing the properties of bound charges in materials [5-7]. An emerging other object for studying and utilizing quantum effects are free electrons, elementary particles that are central to high-resolution microscopy [8,9], electron-based quantum optics [10-17], ul-trafast electron microscopy [18-24] and particle accelerators [25-27]. However, free electrons are intrinsically incoherent, and we lack a broadly applicable method to measure and control their quantum state beyond special cases with discrete energy sidebands [28,29]. Here, we report a universal approach to measure arbitrary free-electron quantum states in continuous variables. Two monochromatic but spectrally shifted laser waves produce interfering quan-tum paths that directly reveal the density matrix and thus all essential properties of the pure wavepackets, the ensemble, and their interlinks. As a first application, we show how the quantum state of a single electron is modified by many-body Coulomb interactions of a sur-rounding electron gas. The reported concepts and results provide insight into otherwise hid-den correlations in electron beams and enable the controlled optimization of exceptional quantum states for free-electron quantum optics or quantum electron microscopy.
Quantum entanglement is central to both the foundations of quantum mechanics and the development of new technologies in information processing, communication, and sensing. Entanglement has been realised in a variety of physical systems, spanning atoms, ions, photons, collective excitations, and hybrid combinations of particles. Remarkably, however, photons and free electrons -- the quanta of light and their most elementary sources -- have never been observed in an entangled state. Here, we demonstrate quantum entanglement between free electrons and photons. We show that entanglement is produced when an electron, prepared in a superposition of two beams, passes a nanostructure and generates transition radiation in a polarisation state tied to the electron path. By implementing quantum state tomography, we reconstruct the full density matrix of the electron-photon pair, and show that the Peres-Horodecki separability criterion is violated by more than 7 standard deviations. Based on this foundational element of emerging free-electron quantum optics, we anticipate manifold developments in enhanced electron imaging and spectroscopy beyond the standard quantum limit. More broadly, the ability to generate and measure entanglement opens electron microscopy to previously inaccessible quantum observables and correlations in solids and nanostructures.
The physical properties of a quantum system, whether pure or mixed, are described fully by its density matrix. Recovery of the density matrix through projective measurements -- referred to as quantum state tomography -- is a cornerstone of quantum optics and metrology. The implementation of this approach in transmission electron microscopy, in particular for the characterisation of an electron beam after inelastic scattering, has remained a longstanding challenge as a result of the complexity of scanning high-dimensional phase spaces, with the number of required measurements growing quadratically with space dimensionality. Here, we introduce a simplified approach by restricting tomography to the electron orbital angular momentum (OAM) subspace. By using an electron optical device known as an OAM sorter, we discretise the phase space into a finite set of measurable states, thus significantly reducing the experimental and computational burden. The resulting measurements suffice to probe essential features of inelastic scattering. We demonstrate the technique by studying the inelastic scattering of a structured electron probe exciting volume plasmons in a carbon film. The combined use of a structured beams and OAM-resolved quantum tomography reveals symmetry-breaking effects and offers insight into the coherence and evolution of the scattered quantum states. Analysis of the diagonalised density matrices further reveals the nature of the induced state transitions, demonstrating the power of the approach for quantum tomography of electron scattering.
Initializing and measuring the wave-function of single freely-propagating particles are challenging but fundamental tasks for applications in quantum information processing and enhanced sensing. Recently, continuous-variable quantum tomography techniques developed for atomic beams and photonic modes have been adapted for on-demand electronic excitations but are limited to the region in energy-time phase space immediately around the Fermi level. Here we present a general, broad-band method for mapping the single-particle phase space Wigner distribution. We reconstruct the Wigner representation of the mixed-state density matrix for \textit{solitary} electrons emitted by an on-demand source. This reveals highly localised distributions isolated from the Fermi sea. Our method can be used to test the degree of `quantumness' of an electron source from measurements of the phase-space density. While both source purity and detector fidelity are suppressed by classical fluctuations, here we resolve fine structure of the wavepackets (a chirp controlled by emission conditions) and find that the resolution should be sufficient to enable quantum-limited measurements. Our technique will provide key information required to master electron coherence and entanglement at the individual particle level, for instance to create excitations from multiple sources that are indistinguishable.
Free electrons provide a powerful tool for probing material properties at atomic resolution. Recent advances in ultrafast electron microscopy enable the manipulation of free-electron wave functions using laser pulses. It would be of great importance if one could combine the spatial resolution of electron microscopes with the ability of laser pulses to probe coherent phenomena in quantum systems. To this end, we propose a novel concept that leverages free electrons that are coherently shaped by laser pulses to measure quantum coherence in materials. We develop the quantum theory of interactions between shaped electrons and arbitrary qubit states in materials, and show how the postinteraction electron energy spectrum enables measuring the qubit state (on the Bloch sphere) and the decoherence or relaxation times (T_{2}/T_{1}). Finally, we describe how such electrons can detect and quantify superradiance from multiple qubits. Our scheme can be implemented in ultrafast transmission electron microscopes (UTEM), opening the way toward the full characterization of the state of quantum systems at atomic resolution.
Since the birth of quantum optics, the measurement of quantum states of nonclassical light has been of tremendous importance for advancement in the field. To date, conventional detectors such as photomultipliers, avalanche photodiodes, and superconducting nanowires, all rely at their core on linear excitation of bound electrons with light, posing fundamental restrictions on the detection. In contrast, the interaction of free electrons with light in the context of quantum optics is highly nonlinear and offers exciting possibilities. The first experiments that promoted this direction appeared over the past decade as part of photon-induced nearfield electron microscopy (PINEM), wherein free electrons are capable of high-order multi-photon absorption and emission. Here we propose using free electrons for quantum-optical detection of the complete quantum state of light. We show how the precise control of the electron before and after its interaction with quantum light enables to extract the photon statistics and implement full quantum state tomography using PINEM. This technique can reach sub-attosecond time resolutions, measure temporal coherence of any degree (e.g., g(1), g(2)), and simultaneously detect large numbers of photons with each electron. Importantly, the interaction of the electron with light is non-destructive, thereby leaving the photonic state (modified by the interaction) intact, which is conceptually different from conventional detectors. By using a pulse of multiple electrons, we envision how PINEM quantum detectors could achieve a single-shot measurement of the complete state of quantum light, even for non-reproducible emission events. Altogether, our work paves the way to novel kinds of photodetectors that utilize the ultrafast duration, high nonlinearity, and non-destructive nature of electron-light interactions.
Electron microscopes provide a powerful platform for exploring physical phenomena with nanoscale resolution, based on the interaction of free electrons with the excitations of a sample such as phonons, excitons, bulk plasmons, and surface plasmons. The interaction usually results in the absorption or emission of such excitations, which can be detected directly through cathodoluminescence or indirectly through electron energy loss spectroscopy (EELS). However, as we show here, the underlying interaction of a free electron and an arbitrary optical excitation goes beyond what was predicted or measured so far, due to the interplay of entanglement and decoherence of the electron-excitation system. The entanglement of electrons and optical excitations can provide new analytical tools in electron microscopy. For example, it can enable measurements of optical coherence, plasmonic lifetimes, and electronic length scales in matter (such as the Bohr radius of an exciton). We show how these can be achieved using common configurations in electron diffraction and EELS, revealing significant changes in the electron’s coherence, as well as in other quantum information theoretic measures such as purity. Specifically, we find that the purity after interaction with nanoparticles can only take discrete values, versus a continuum of values for interactions with surface plasmons. We quantify the post-interaction density matrix of the combined electron-excitation system by developing a framework based on macroscopic quantum electrodynamics. The framework enables a quantitative account of decoherence due to excitations in any general polarizable material (optical environment). This framework is thus applicable beyond electron microscopy. Particularly in electron microscopy, our work enriches analytical capabilities and informs the design of quantum information experiments with free electrons, allowing control over their quantum states and their decoherence by the optical environment.