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 Stern-Gerlach effect in the time domain.

The Stern-Gerlach experiment, a seminal quantum physics experiment, demonstrated the intriguing phenomenon of particle spin quantization, leading to applications in matter-wave interferometry and weak-value measurements. Over the years, several optical experiments have exhibited similar behavior to the Stern-Gerlach experiment, revealing splitting in both spatial and angular domains. Here we show, theoretically and experimentally, that the Stern-Gerlach effect can be extended into the time and frequency domains. By harnessing Kerr nonlinearity in optical fibers, we couple signal and idler pulses using two pump pulses, resulting in the emergence of two distinct eigenstates whereby the signal and idler are either in phase or out of phase. This nonlinear coupling emulates a synthetic magnetization, and by varying it linearly in time, one eigenstate deflects towards a higher frequency, while the other deflects towards a lower frequency. This effect can be utilized to realize an all-optical, phase-sensitive frequency beam splitter, establishing a new paradigm for classical and quantum data processing of frequency-bin superposition states.

Two-dimensional control of a biphoton joint spectrum.

Control over the joint spectral amplitude of a photon pair has proved highly desirable for many quantum applications, since it contains the spectral quantum correlations, and has crucial effects on the indistinguishability of photons, as well as promising emerging applications involving complex quantum functions and frequency encoding of qudits. Until today, this has been achieved by engineering a single degree of freedom, either by custom poling nonlinear crystal or by shaping the pump pulse. We present a combined approach where two degrees of freedom, the phase-matching function, and the pump spectrum, are controlled. This approach enables the two-dimensional control of the joint spectral amplitude, generating a variety of spectrally encoded quantum states - including frequency uncorrelated states, frequency-bin Bell states, and biphoton qudit states. In addition, the joint spectral amplitude is controlled by photon bunching and anti-bunching, reflecting the symmetry of the phase-matching function.

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.

Near index matching enables solid diffractive optical element fabrication via additive manufacturing.

Diffractive optical elements (DOEs) have a wide range of applications in optics and photonics, thanks to their capability to perform complex wavefront shaping in a compact form. However, widespread applicability of DOEs is still limited, because existing fabrication methods are cumbersome and expensive. Here, we present a simple and cost-effective fabrication approach for solid, high-performance DOEs. The method is based on conjugating two nearly refractive index-matched solidifiable transparent materials. The index matching allows for extreme scaling up of the elements in the axial dimension, which enables simple fabrication of a template using commercially available 3D printing at tens-of-micrometer resolution. We demonstrated the approach by fabricating and using DOEs serving as microlens arrays, vortex plates, including for highly sensitive applications such as vector beam generation and super-resolution microscopy using MINSTED, and phase-masks for three-dimensional single-molecule localization microscopy. Beyond the advantage of making DOEs widely accessible by drastically simplifying their production, the method also overcomes difficulties faced by existing methods in fabricating highly complex elements, such as high-order vortex plates, and spectrum-encoding phase masks for microscopy.

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.

Direct generation of spatially entangled qudits using quantum nonlinear optical holography.

Nonlinear holography shapes the amplitude and phase of generated new harmonics using nonlinear processes. Classical nonlinear holography influenced many fields in optics, from information storage, demultiplexing of spatial information, and all-optical control of accelerating beams. Here, we extend the concept of nonlinear holography to the quantum regime. We directly shape the spatial quantum correlations of entangled photon pairs in two-dimensional patterned nonlinear photonic crystals using spontaneous parametric down conversion, without any pump shaping. The generated signal-idler pair obeys a parity conservation law that is governed by the nonlinear crystal. Furthermore, the quantum states exhibit quantum correlations and violate the Clauser-Horne-Shimony-Holt inequality, thus enabling entanglement-based quantum key distribution. Our demonstration paves the way for controllable on-chip quantum optics schemes using the high-dimensional spatial degree of freedom.

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.

Optical frequency combs in dispersion-controlled doubly resonant second-harmonic generation.

We report on the experimental realization and a systematic study of optical frequency comb generation in doubly resonant intracavity second harmonic generation (SHG). The efficiency of intracavity nonlinear processes usually benefits from the increasing number of resonating fields. Yet, achieving the simultaneous resonance of different fields may be technically complicated, all the more when a phase matching condition must be fulfilled as well. In our cavity we can separately control the resonance condition for the fundamental and its second harmonic, by simultaneously acting on an intracavity dispersive element and on a piezo-mounted cavity mirror, without affecting the quasi-phase matching condition. In addition, by finely adjusting the laser-to-cavity detuning, we are able to observe steady comb emission across the whole resonance profile, revealing the multiplicity of comb structures, and the substantial role of thermal effects on their dynamics. Lastly, we report the results of numerical simulations of comb dynamics, which include photothermal effects, finding a good agreement with the experimental observations. Our system provides a framework for exploring the richness of comb dynamics in doubly resonant SHG systems, assisting the design of chip-scale quadratic comb generators.

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.

Effect of spatial variation of the duty cycle in transverse second-harmonic generation.

Transverse second-harmonic generation, in which the emission angles of the second harmonic are determined by the spatial modulation of the quadratic nonlinearity, has important applications in nonlinear optical imaging, holography, and beam shaping. Here we study the role of the local duty cycle of the nonlinearity on the light intensity distribution in transverse second-harmonic generation, taking the generation of perfect vortices in periodically poled ferroelectric crystal as an example. We show, theoretically and experimentally, that spatial variations of the nonlinearity modulation must be accompanied by the corresponding changes of the width of inverted ferroelectric domains, to ensure uniformity of the light intensity distribution in the generated second harmonic. This work provides a fundamental way to achieve high-quality transverse second-harmonic generation and, hence, opens more possibilities in applications based on harmonic generation and its control.

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.

Integrated orbital angular momentum mode sorters on vortex fibers.

We design, fabricate, and characterize integrated mode sorters for multimode fibers that guide well-separated vortex modes. We use 3D direct laser printing to print a collimator and a Cartesian to a log-polar mode transformer on the tip of the fiber. This polarization insensitive device can send different modes into different exit angles and is therefore useful for space division multiplexed optical communication. Two types of fibers with two corresponding sorters are used, enabling the sorting of either four or eight different modes in a compact and robust manner. The integration of the vortex fiber and multiplexer opens the door for widespread exploitation of orbital angular momentum (OAM) for data multiplexing in fiber networks.

Periodic Wave Trains in Nonlinear Media: Talbot Revivals, Akhmediev Breathers, and Asymmetry Breaking.

We study theoretically and observe experimentally the evolution of periodic wave trains by utilizing surface gravity water wave packets. Our experimental system enables us to observe both the amplitude and the phase of these wave packets. For low steepness waves, the propagation dynamics is in the linear regime, and these waves unfold a Talbot carpet. By increasing the steepness of the waves and the corresponding nonlinear response, the waves follow the Akhmediev breather solution, where the higher frequency periodic patterns at the fractional Talbot distance disappear. Further increase in the wave steepness leads to deviations from the Akhmediev breather solution and to asymmetric breaking of the wave function. Unlike the periodic revival that occurs in the linear regime, here the wave crests exhibit self acceleration, followed by self deceleration at half the Talbot distance, thus completing a smooth transition of the periodic pulse train by half a period. Such phenomena can be theoretically modeled by using the Dysthe equation.

Shaping of Electron Beams Using Sculpted Thin Films.

Electron beam shaping by sculpted thin films relies on electron-matter interactions and the wave nature of electrons. It can be used to study physical phenomena of special electron beams and to develop technological applications in electron microscopy that offer new and improved measurement techniques and increased resolution in different imaging modes. In this Perspective, we review recent applications of sculpted thin films for electron orbital angular momentum sorting, improvements in phase contrast transmission electron microscopy, and aberration correction. For the latter, we also present new results of our work toward correction of the spherical aberration of Lorentz scanning transmission electron microscopes and suggest a method to correct chromatic aberration using thin films. This review provides practical insight for researchers in the field and motivates future progress in electron microscopy.

Storing and retrieving multiple images in 3D nonlinear photonic crystals.

A nonlinear hologram enables to record the amplitude and phase of a waveform by spatially modulating the second order nonlinear coefficient, so that when a pump laser illuminates it, this waveform is reconstructed at the second harmonic frequency. The concept was now extended to enable the generation of multiple waveforms from a single hologram, with potential applications in high density storage, quantum optics, and optical microscopy.

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.

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.

Diffractive Guiding of Waves by a Periodic Array of Slits.

We show that in order to guide waves, it is sufficient to periodically truncate their edges. The modes supported by this type of wave guide propagate freely between the slits, and the propagation pattern repeats itself. We experimentally demonstrate this general wave phenomenon for two types of waves: (i) plasmonic waves propagating on a metal-air interface that are periodically blocked by nanometric metallic walls, and (ii) surface gravity water waves whose evolution is recorded, the packet is truncated, and generated again to show repeated patterns. This guiding concept is applicable for a wide variety of waves.

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.