Coherent radiation at visible wavelengths from sub-keV electron beams.

The Smith-Purcell effect allows for coherent free-electron-driven compact light sources over the entire electromagnetic spectrum. Intriguing interaction regimes, with prospects for quantum optical applications, are expected when the driving free electron enters the sub-keV range, though this has until now remained an experimental challenge. Here, we demonstrate the Smith-Purcell light emission from UV to visible using engineerable, fabricated gratings with periodicities as low as 19 nm and with electron energies as low as 300 eV. Our findings constitute a major step toward broadband, highly tunable, on-chip light sources, observation of quantum recoil effects, and tunable EUV and x ray sources from swift electrons.

All-optical spin valve effect in nonlinear optics.

More than three decades after the inception of electron spin-based information encoding inspired by nonlinear electro-optic devices, we present a complementary approach: nonlinear optical devices directly inspired by spintronics. We theoretically propose an all-optical spin-valve device and a spin-dependent beam splitter, where the optical pseudospin is a superposition of signal and idler beams undergoing a sum-frequency generation process inside a 2D nonlinear photonic crystal. We delve into the operation of these devices, examining key properties such as the transmission angle and splitting ratio, optically controlled by the pump beam. Our findings open new avenues for both classical and quantum optical information processing in the frequency domain.

Frequency-domain engineering of bright squeezed vacuum for continuous-variable quantum information.

Multimode bright squeezed vacuum is a non-classical state of light hosting a macroscopic photon number while offering promising capacity for encoding quantum information in its spectral degree of freedom. Here, we employ an accurate model for parametric down-conversion in the high-gain regime and use nonlinear holography to design quantum correlations of bright squeezed vacuum in the frequency domain. We propose the design of quantum correlations over two-dimensional lattice geometries that are all-optically controlled, paving the way toward continuous-variable cluster state generation on an ultrafast timescale. Specifically, we investigate the generation of a square cluster state in the frequency domain and calculate its covariance matrix and the quantum nullifier uncertainties, that exhibit squeezing below the vacuum noise level.

Cylindrical Metalens for Generation and Focusing of Free-Electron Radiation.

Metasurfaces constitute a powerful approach to generate and control light by engineering optical material properties at the subwavelength scale. Recently, this concept was applied to manipulate free-electron radiation phenomena, rendering versatile light sources with unique functionalities. In this Letter, we experimentally demonstrate spectral and angular control over coherent light emission by metasurfaces that interact with free-electrons under grazing incidence. Specifically, we study metalenses based on chirped metagratings that simultaneously emit and shape Smith-Purcell radiation in the visible and near-infrared spectral regime. In good agreement with theory, we observe the far-field signatures of strongly convergent and divergent cylindrical radiation wavefronts using in situ hyperspectral angle-resolved light detection in a scanning electron microscope. Furthermore, we theoretically explore simultaneous control over the polarization and wavefront of Smith-Purcell radiation via a split-ring-resonator metasurface, enabling tunable operation by spatially selective mode excitation at nanometer resolution. Our work highlights the potential of merging metasurfaces with free-electron excitations for versatile and highly tunable radiation sources in wide-ranging spectral regimes.

Direct generation of high brightness path entangled N00N states using structured crystals and shaped pump beams.

Optical N00N states are N-photon path entangled states with important applications in quantum metrology. However, their use was limited till now owing to the difficulties of generating them in an efficient and robust manner. Here we propose and experimentally demonstrate two new simple, compact and robust schemes to generate path entangled N00N states with N = 2 that emerge directly from the nonlinear interaction. The first scheme is based on shaping the pump beam, and the second scheme is based on modulating the nonlinear coefficient of the crystal. These new methods exhibit high coincidence count rates for the detection of a N00N state, reaching record value of 2 × 105 coincidences per second. We observe super-resolution by measuring the second order correlation on the generated N = 2 state in an interferometric setup, showing the distinct fringe periodicity at half of the optical wavelength. Our findings may pave the way towards scalable and efficient sources for super-resolved quantum metrology applications and for the generation of bright squeezed vacuum states.

Superradiance and Subradiance due to Quantum Interference of Entangled Free Electrons.

When multiple quantum emitters radiate, their emission rate may be enhanced or suppressed due to collective interference in a process known as super- or subradiance. Such processes are well known to occur also in light emission from free electrons, known as coherent cathodoluminescence. Unlike atomic systems, free electrons have an unbounded energy spectrum, and, thus, all their emission mechanisms rely on electron recoil, in addition to the classical properties of the dielectric medium. To date, all experimental and theoretical studies of super- and subradiance from free electrons assumed only classical correlations between particles. However, dependence on quantum correlations, such as entanglement between free electrons, has not been studied. Recent advances in coherent shaping of free-electron wave functions motivate the investigation of such quantum regimes of super- and subradiance. In this Letter, we show how a pair of coincident path-entangled electrons can demonstrate either super- or subradiant light emission, depending on the two-particle wave function. By choosing different free-electron Bell states, the spectrum and emission pattern of the light can be reshaped, in a manner that cannot be accounted for by a classical mixed state. We show these results for light emission in any optical medium and discuss their generalization to many-body quantum states. Our findings suggest that light emission can be sensitive to the explicit quantum state of the emitting matter wave and possibly serve as a nondestructive measurement scheme for measuring the quantum state of many-body systems.

Observing the Quantum Wave Nature of Free Electrons through Spontaneous Emission.

We investigate, both experimentally and theoretically, the interpretation of the free-electron wave function using spontaneous emission. We use a transversely wide single-electron wave function to describe the spatial extent of transverse coherence of an electron beam in a standard transmission electron microscope. When the electron beam passes next to a metallic grating, spontaneous Smith-Purcell radiation is emitted. We then examine the effect of the electron wave function transversal size on the emitted radiation. Two interpretations widely used in the literature are considered: (1) radiation by a continuous current density attributed to the quantum probability current, equivalent to the spreading of the electron charge continuously over space; and (2) interpreting the square modulus of the wave function as a probability distribution of finding a point particle at a certain location, wherein the electron charge is always localized in space. We discuss how these two interpretations give contradictory predictions for the radiation pattern in our experiment, comparing the emission from narrow and wide wave functions with respect to the emitted radiation's wavelength. Matching our experiment with a new quantum-electrodynamics derivation, we conclude that the measurements can be explained by the probability distribution approach wherein the electron interacts with the grating as a classical point charge. Our findings clarify the transition between the classical and quantum regimes and shed light on the mechanisms that take part in general light-matter interactions.

Fully controllable adiabatic geometric phase in nonlinear optics.

We propose and analyze a new way for obtaining an adiabatic geometric phase for light, via the sum-frequency-generation nonlinear process. The state of light is represented by the complex amplitudes at two different optical frequencies, coupled by the second order nonlinearity of the medium. The dynamics of this system is then shown to be equivalent to that of a spin-1/2 particle in a magnetic field, which in turn can be rotated adiabatically on the Bloch sphere. When the input wave itself is an eigenstate of the magnetic field equivalent, the geometric phase is manifested as a pure phase factor. Two adiabatic rotation schemes, based on specific modulations of the quasi-phase-matching poling parameters, are discussed. In the first, the geometric phase is shown to be sensitive to the pump intensity variations, as a result of the Bloch sphere deformation. The second can be utilized for the realization of nonlinear-optics-based geometric phase plates. Moreover, non-closed adiabatic trajectories are investigated, which are expected to provide a robust and broadband geometric wavefront shaping in the sum frequency.

All-Optical Stern-Gerlach Effect.

We introduce a novel formalism in which the paraxial coupled wave equations of the nonlinear optical sum-frequency generation process are shown to be equivalent to the Pauli equation describing the dynamics of a spin-1/2 particle in a spatially varying magnetic field. This interpretation gives rise to a new classical state of paraxial light, described by a mutual beam comprising of two frequencies. As a straightforward application, we propose the existence of an all-optical Stern-Gerlach effect, where an idler beam is deflected by a gradient in the nonlinear coupling, into two mutual beams of the idler and signal waves (equivalent to oppositely oriented spinors), propagating in two discrete directions. The Stern-Gerlach deflection angle and the intensity pattern in the far field are then obtained analytically, in terms of the parameters of the original optical system, laying the grounds for future experimental realizations.

Surface Pressure of Charged Colloids at the Air/Water Interface.

Charged colloidal monolayers at the interface between water and air (or oil) are used in a large number of chemical, physical, and biological applications. Although considerable experimental and theoretical effort has been devoted in the past few decades to the investigation of such monolayers, some of their fundamental properties are not yet fully understood. In this article, we model charged colloidal monolayers as a continuum layer of finite thickness, with a separate charge distribution on the water and air sides. The electrostatic surface free energy and surface pressure are calculated via the charging method and within the Debye-Hückel approximation. We obtain the dependence of surface pressure on several system parameters: the monolayer thickness, its distinct dielectric permittivity, and the ionic strength of the aqueous subphase. The surface pressure scaling with the area per particle, a, is found to be between a-2 in the close-packing limit and a-5/2 in the loose-packing limit. In general, it is found that the surface pressure is strongly influenced by charges on the air side of the colloids. However, when the larger charge resides on the water side, a more subtle dependence on salt concentration emerges. This corrects a common assumption that the charges on the water side can always be neglected due to screening. Finally, using a single fit parameter, our theory is found to fit the experimental data well for strong- to intermediate-strength electrolytes. We postulate that an anomalous scaling of a-3/2, recently observed in low ionic concentrations, cannot be accounted for within a linear theory, and its explanation requires a fully nonlinear analysis.

Free-electron crystals for enhanced X-ray radiation.

Bremsstrahlung-the spontaneous emission of broadband radiation from free electrons that are deflected by atomic nuclei-contributes to the majority of X-rays emitted from X-ray tubes and used in applications ranging from medical imaging to semiconductor chip inspection. Here, we show that the bremsstrahlung intensity can be enhanced significantly-by more than three orders of magnitude-through shaping the electron wavefunction to periodically overlap with atoms in crystalline materials. Furthermore, we show how to shape the bremsstrahlung X-ray emission pattern into arbitrary angular emission profiles for purposes such as unidirectionality and multi-directionality. Importantly, we find that these enhancements and shaped emission profiles cannot be attributed solely to the spatial overlap between the electron probability distribution and the atomic centers, as predicted by the paraxial and non-recoil theory for free electron light emission. Our work highlights an unprecedented regime of free electron light emission where electron waveshaping provides multi-dimensional control over practical radiation processes like bremsstrahlung. Our results pave the way towards greater versatility in table-top X-ray sources and improved fundamental understanding of quantum electron-light interactions.

Jaynes-Cummings interaction between low-energy free electrons and cavity photons.

The Jaynes-Cummings Hamiltonian is at the core of cavity quantum electrodynamics; however, it relies on bound-electron emitters fundamentally limited by the binding Coulomb potential. In this work, we propose theoretically a new approach to realizing the Jaynes-Cummings model using low-energy free electrons coupled to dielectric microcavities and exemplify several quantum technologies made possible by this approach. Using quantum recoil, a large detuning inhibits the emission of multiple consecutive photons, effectively transforming the free electron into a few-level system coupled to the cavity mode. We show that this approach can be used for generation of single photons, photon pairs, and even a quantum SWAP gate between a photon and a free electron, with unity efficiency and high fidelity. Tunable by their kinetic energy, quantum free electrons are inherently versatile emitters with an engineerable emission wavelength. Hence, they pave the way toward new possibilities for quantum interconnects between photonic platforms at disparate spectral regimes.

Quantum sensing of strongly coupled light-matter systems using free electrons.

Strong coupling in light-matter systems is a central concept in cavity quantum electrodynamics and is essential for many quantum technologies. Especially in the optical range, full control of highly connected multi-qubit systems necessitates quantum coherent probes with nanometric spatial resolution, which are currently inaccessible. Here, we propose the use of free electrons as high-resolution quantum sensors for strongly coupled light-matter systems. Shaping the free-electron wave packet enables the measurement of the quantum state of the entire hybrid systems. We specifically show how quantum interference of the free-electron wave packet gives rise to a quantum-enhanced sensing protocol for the position and dipole orientation of a subnanometer emitter inside a cavity. Our results showcase the great versatility and applicability of quantum interactions between free electrons and strongly coupled cavities, relying on the unique properties of free electrons as strongly interacting flying qubits with miniscule dimensions.

The coherence of light is fundamentally tied to the quantum coherence of the emitting particle.

Coherent emission of light by free charged particles is believed to be successfully captured by classical electromagnetism in all experimental settings. However, recent advances triggered fundamental questions regarding the role of the particle wave function in these processes. Here, we find that even in seemingly classical experimental regimes, light emission is fundamentally tied to the quantum coherence and correlations of the emitting particle. We use quantum electrodynamics to show how the particle's momentum uncertainty determines the optical coherence of the emitted light. We find that the temporal duration of Cherenkov radiation, envisioned for almost a century as a shock wave of light, is limited by underlying entanglement between the particle and light. Our findings enable new capabilities in electron microscopy for measuring quantum correlations of shaped electrons. Last, we propose new Cherenkov detection schemes, whereby measuring spectral photon autocorrelations can unveil the wave function structure of any charged high-energy particle.

Emulating spin transport with nonlinear optics, from high-order skyrmions to the topological Hall effect.

Exploring material magnetization led to countless fundamental discoveries and applications, culminating in the field of spintronics. Recently, research effort in this field focused on magnetic skyrmions - topologically robust chiral magnetization textures, capable of storing information and routing spin currents via the topological Hall effect. In this article, we propose an optical system emulating any 2D spin transport phenomena with unprecedented controllability, by employing three-wave mixing in 3D nonlinear photonic crystals. Precise photonic crystal engineering, as well as active all-optical control, enable the realization of effective magnetization textures beyond the limits of thermodynamic stability in current materials. As a proof-of-concept, we theoretically design skyrmionic nonlinear photonic crystals with arbitrary topologies and propose an optical system exhibiting the topological Hall effect. Our work paves the way towards quantum spintronics simulations and novel optoelectronic applications inspired by spintronics, for both classical and quantum optical information processing.

Imprinting the quantum statistics of photons on free electrons.

The interaction between free electrons and light stands at the base of both classical and quantum physics, with applications in free-electron acceleration, radiation sources, and electron microscopy. Yet to this day, all experiments involving free-electron­light interactions are fully explained by describing the light as a classical wave. We observed quantum statistics effects of photons on free-electron­light interactions. We demonstrate interactions that pass continuously from Poissonian to super-Poissonian and up to thermal statistics, revealing a transition from quantum walk to classical random walk on the free-electron energy ladder. The electron walker serves as the probe in nondestructive quantum detection, measuring the second-order photon-correlation g(2)(0) and higher-orders g(n)(0). Unlike conventional quantum-optical detectors, the electron can perform both quantum weak measurements and projective measurements by evolving into an entangled joint state with the photons. These findings inspire hitherto inaccessible concepts in quantum optics, including free-electron­based ultrafast quantum tomography of light.