Strongly correlated multielectron bunches from interaction with quantum light.

Strongly correlated electron systems are a cornerstone of modern physics, being responsible for groundbreaking phenomena from superconducting magnets to quantum computing. In most cases, correlations in electrons arise exclusively because of Coulomb interactions. In this work, we reveal that free electrons interacting simultaneously with a light field can become highly correlated via mechanisms beyond Coulomb interactions. In the case of two electrons, the resulting Pearson correlation coefficient for the joint probability distribution of the output electron energies is enhanced by more than 13 orders of magnitude compared to that of electrons interacting with the light field in succession (one after another). These highly correlated electrons are the result of momentum and energy exchange between the participating electrons via the external quantum light field. Our findings pave the way to the creation and control of highly correlated free electrons for applications including quantum information and ultrafast imaging.

The Nanoplasmonic Purcell Effect in Ultrafast and High-Light-Yield Perovskite Scintillators.

The development of X-ray scintillators with ultrahigh light yields and ultrafast response times is a long sought-after goal. In this work, a fundamental mechanism that pushes the frontiers of ultrafast X-ray scintillator performance is theoretically predicted and experimentally demonstrated: the use of nanoscale-confined surface plasmon polariton modes to tailor the scintillator response time via the Purcell effect. By incorporating nanoplasmonic materials in scintillator devices, this work predicts over tenfold enhancement in decay rate and 38% reduction in time resolution even with only a simple planar design. The nanoplasmonic Purcell effect is experimentally demonstrated using perovskite scintillators, enhancing the light yield by over 120% to 88 ± 11 ph/keV, and the decay rate by over 60% to 2.0 ± 0.2 ns for the average decay time, and 0.7 ± 0.1 ns for the ultrafast decay component, in good agreement with the predictions of our theoretical framework. Proof-of-concept X-ray imaging experiments are performed using nanoplasmonic scintillators, demonstrating 182% enhancement in the modulation transfer function at four line pairs per millimeter spatial frequency. This work highlights the enormous potential of nanoplasmonics in optimizing ultrafast scintillator devices for applications including time-of-flight X-ray imaging and photon-counting computed tomography.

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.

Multicolor x-rays from free electron-driven van der Waals heterostructures.

The emergence of van der Waals (vdW) heterostructures has led to precise and versatile methods of fabricating devices with atomic-scale accuracies. Hence, vdW heterostructures have shown much promise for technologies including photodetectors, photocatalysis, photovoltaic devices, ultrafast photonic devices, and field-effect transistors. These applications, however, remain confined to optical and suboptical regimes. Here, we theoretically show and experimentally demonstrate the use of vdW heterostructures as platforms for multicolor x-ray generation. By driving the vdW heterostructures with free electrons in a table-top setup, we generate x-ray photons whose output spectral profile can be user-customized via the heterostructure design and even controlled in real time. We show that the multicolor photon energies and their corresponding intensities can be tailored by varying the electron energy, the electron beam position, as well as the geometry and composition of the vdW heterostructure. Our results reveal the promise of vdW heterostructures in realizing highly versatile x-ray sources for emerging applications in advanced x-ray imaging and spectroscopy.

Free-electron interactions with van der Waals heterostructures: a source of focused X-ray radiation.

The science and technology of X-ray optics have come far, enabling the focusing of X-rays for applications in high-resolution X-ray spectroscopy, imaging, and irradiation. In spite of this, many forms of tailoring waves that had substantial impact on applications in the optical regime have remained out of reach in the X-ray regime. This disparity fundamentally arises from the tendency of refractive indices of all materials to approach unity at high frequencies, making X-ray-optical components such as lenses and mirrors much harder to create and often less efficient. Here, we propose a new concept for X-ray focusing based on inducing a curved wavefront into the X-ray generation process, resulting in the intrinsic focusing of X-ray waves. This concept can be seen as effectively integrating the optics to be part of the emission mechanism, thus bypassing the efficiency limits imposed by X-ray optical components, enabling the creation of nanobeams with nanoscale focal spot sizes and micrometer-scale focal lengths. Specifically, we implement this concept by designing aperiodic vdW heterostructures that shape X-rays when driven by free electrons. The parameters of the focused hotspot, such as lateral size and focal depth, are tunable as a function of an interlayer spacing chirp and electron energy. Looking forward, ongoing advances in the creation of many-layer vdW heterostructures open unprecedented horizons of focusing and arbitrary shaping of X-ray nanobeams.

Design and construction of a compact, high-repetition-rate ultrafast electron diffraction instrument.

We present the design and performance of a compact ultrafast electron diffraction instrument. The diffractometer provides a means of examining time-resolved ultrafast dynamical properties of solids. The system's utilization is discussed in terms of instrument parameters and diffraction data from selected condensed matter samples. The difractometer's performance is highlighted in terms of detection sensitivity, instrumental temporal resolution, and the electron beam transverse coherence length. Following specific details of the construction, we present a practical discussion of parameters such as repetition rate and provide advice on general construction approaches for laboratory-based, keV ultrafast electron diffractometers. In addition, design guidance for constructing a compact electron gun source that is well-suited for studying diffraction from hard condensed matter is given. A unique data acquisition scheme, utilizing high laser repetition rates, is presented.

Resolution enhancement for interrogating fiber Bragg grating sensor network using dilated U-Net.

In the fiber Bragg grating (FBG) sensor network, the signal resolution of the reflected spectrum is correlated with the network's sensing accuracy. The interrogator determines the signal resolution limits, and a coarser resolution results in an enormous uncertainty in sensing measurement. In addition, the multi-peak signals from the FBG sensor network are often overlapped; this increases the complexity of the resolution enhancement task, especially when the signals have a low signal-to-noise ratio (SNR). Here, we show that deep learning with U-Net architecture can enhance the signal resolution for interrogating the FBG sensor network without hardware modifications. The signal resolution is effectively enhanced by 100 times with an average root mean square error (RMSE) < 2.25 pm. The proposed model, therefore, allows the existing low-resolution interrogator in the FBG setup to function as though it contains a much higher-resolution interrogator.

Quantum Interference between Fundamentally Different Processes Is Enabled by Shaped Input Wavefunctions.

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.

Self-adaptive deep reinforcement learning for THz beamforming with silicon metasurfaces in 6G communications.

Exponential growth in data rate demands has driven efforts to develop novel beamforming techniques for realizing massive multiple-input and multiple-output (MIMO) systems in sixth-generation (6G) terabits per second wireless communications. Existing beamforming techniques rely on conventional optimization algorithms that are too computationally expensive for real-time applications and require complex digital processing yet to be achieved for phased array antennas at terahertz frequencies. Here, we develop an intelligent and self-adaptive beamforming scheme enabled by deep reinforcement learning, which can predict the spatial phase profiles required to produce arbitrary desired radiation patterns in real-time. Our deep learning model adaptively trains an artificial neural network in real-time by comparing the input and predicted intensity patterns via automatic differentiation of the phase-to-intensity function. As a proof of concept, we experimentally demonstrate two-dimensional beamforming by spatially modulating broadband terahertz waves using silicon metasurfaces designed with the aid of the deep learning model. Our work offers an efficient and robust deep learning model for real-time self-adaptive beamforming to enable multi-user massive MIMO systems for 6G terahertz wireless communications, as well as intelligent metasurfaces for other terahertz applications in imaging and sensing.

Enhanced Versatility of Table-Top X-Rays from Van der Waals Structures.

Van der Waals (vdW) materials have attracted much interest for their myriad unique electronic, mechanical, and thermal properties. In particular, they are promising candidates for monochromatic, table-top X-ray sources. This work reveals that the versatility of the table-top vdW X-ray source goes beyond what has been demonstrated so far. By introducing a tilt angle between the vdW structure and the incident electron beam, it is theoretically and experimentally shown that the accessible photon energy range is more than doubled. This allows for greater versatility in real-time tuning of the vdW X-ray source. Furthermore, this work shows that the accessible photon energy range is maximized by simultaneously controlling both the electron energy and the vdW structure tilt. These results will pave the way for highly tunable, compact X-ray sources, with potential applications including hyperspectral X-ray fluoroscopy and X-ray quantum optics.

Space-Time Wave Packets from Smith-Purcell Radiation.

Space-time wave packets are electromagnetic waves with strong correlations between their spatial and temporal degrees of freedom. These wave packets have gained much attention for fundamental properties like propagation invariance and user-designed group velocities, and for potential applications like optical microscopy, micromanipulation, and laser micromachining. Here, free-electron radiation is presented as a natural and versatile source of space-time wave packets that are ultra-broadband and highly tunable in frequency. For instance, ab initio theory and numerical simulations show that the intensity profile of space-time wave packets from Smith-Purcell radiation can be directly tailored through the grating properties, as well as the velocity and shape of the electron bunches. The result of this work indicates a viable way of generating space-time wave packets at exotic frequencies such as the terahertz and X-ray regimes, potentially paving the way toward new methods of shaping electromagnetic wave packets through free-electron radiation.

Propagation-invariant space-time caustics of light.

Caustics are responsible for a wide range of natural phenomena, from rainbows and mirages to sparkling seas. Here, we present caustics in space-time wavepackets, a class of pulsed beams featuring strong coupling between spatial and temporal frequencies. Space-time wavepackets have attracted much attention with their propagation-invariant intensity profiles that travel at tunable superluminal and subluminal group velocities. These intensity profiles, however, have been largely restricted to an X-shape or similar pattern. We show that space-time caustics combine the propagation invariance of space-time wavepackets with the flexible design of caustics, allowing for customizable intensity patterns in space-time wavepackets. Our method directly provides the phase distribution needed to realize user-designed caustic patterns in space-time wavepackets. We show that space-time caustics can feature in a broad range of intriguing optical phenomena, including backward traveling caustics formed from purely forward propagating waves, and nondiffracting beams that evolve with time. Our findings should open the doors to an even wider range of structured light with spatiotemporal coupling.

Dilated convolutional neural networks for fiber Bragg grating signal demodulation.

In quasi-distributed fiber Bragg grating (FBG) sensor networks, challenges are known to arise when signals are highly overlapped and thus hard to separate, giving rise to substantial error in signal demodulation. We propose a multi-peak detection deep learning model based on a dilated convolutional neural network (CNN) that overcomes this problem, achieving extremely low error in signal demodulation even for highly overlapped signals. We show that our FBG demodulation scheme enhances the network multiplexing capability, detection accuracy and detection time of the FBG sensor network, achieving a root-mean-square (RMS) error in peak wavelength determination of < 0.05 pm, with a demodulation time of 15 ms for two signals. Our demodulation scheme is also robust against noise, achieving an RMS error of < 0.47 pm even with a signal-to-noise ratio as low as 15 dB. A comparison on our high-performance computer with existing signal demodulation methods shows the superiority in RMS error of our dilated CNN implementation. Our findings pave the way to faster and more accurate signal demodulation methods, and testify to the substantial promise of neural network algorithms in signal demodulation problems.

Control of quantum electrodynamical processes by shaping electron wavepackets.

Fundamental quantum electrodynamical (QED) processes, such as spontaneous emission and electron-photon scattering, encompass phenomena that underlie much of modern science and technology. Conventionally, calculations in QED and other field theories treat incoming particles as single-momentum states, omitting the possibility that coherent superposition states, i.e., shaped wavepackets, can alter fundamental scattering processes. Here, we show that free electron waveshaping can be used to design interferences between two or more pathways in a QED process, enabling precise control over the rate of that process. As an example, we show that free electron waveshaping modifies both spatial and spectral characteristics of bremsstrahlung emission, leading for instance to enhancements in directionality and monochromaticity. The ability to tailor general QED processes opens up additional avenues of control in phenomena ranging from optical excitation (e.g., plasmon and phonon emission) in electron microscopy to free electron lasing in the quantum regime.

The Complex Charge Paradigm: A New Approach for Designing Electromagnetic Wavepackets.

Singularities in optics famously describe a broad range of intriguing phenomena, from vortices and caustics to field divergences near point charges. The diverging fields created by point charges are conventionally seen as a mathematical peculiarity that is neither needed nor related to the description of electromagnetic beams and pulses, and other effects in modern optics. This work disrupts this viewpoint by shifting point charges into the complex plane, and showing that their singularities then give rise to propagating, divergence-free wavepackets. Specifically, point charges moving in complex space-time trajectories are shown to map existing wavepackets to corresponding complex trajectories. Tailoring the complex trajectories in this "complex charge paradigm" leads to the discovery and design of new wavepacket families, as well as unprecedented electromagnetic phenomena, such as the combination of both nondiffracting behavior and abruptly-varying behavior in a single wavepacket. As an example, the abruptly focusing X-wave-a propagation-invariant X-wave-like wavepacket with prechosen self-disruptions that enhance its peak intensity by over 200 times-is presented. This work envisions a unified method that captures all existing wavepackets as corresponding complex trajectories, creating a new design tool in modern optics and paving the way to further discoveries of electromagnetic modes and waveshaping applications.

Monochromatic X-ray Source Based on Scattering from a Magnetic Nanoundulator.

We present a novel design for an ultracompact, passive light source capable of generating ultraviolet and X-ray radiation, based on the interaction of free electrons with the magnetic near-field of a ferromagnet. Our design is motivated by recent advances in the fabrication of nanostructures, which allow the confinement of large magnetic fields at the surface of ferromagnetic nanogratings. Using ab initio simulations and a complementary analytical theory, we show that highly directional, tunable, monochromatic radiation at high frequencies could be produced from relatively low-energy electrons within a tabletop design. The output frequency is tunable in the extreme ultraviolet to hard X-ray range via electron kinetic energies from 1 keV to 5 MeV and nanograting periods from 1 µm to 5 nm. The proposed radiation source can achieve the tunability and monochromaticity of current free-electron-driven sources (free-electron lasers, synchrotrons, and laser-driven undulators), yet with a significantly reduced scale, cost, and complexity. Our design could help realize the next generation of tabletop or on-chip X-ray sources.

Graphene Metamaterials for Intense, Tunable, and Compact Extreme Ultraviolet and X-Ray Sources.

The interaction of electrons with strong electromagnetic fields is fundamental to the ability to design high-quality radiation sources. At the core of all such sources is a tradeoff between compactness and higher output radiation intensities. Conventional photonic devices are limited in size by their operating wavelength, which helps compactness at the cost of a small interaction area. Here, plasmonic modes supported by multilayer graphene metamaterials are shown to provide a larger interaction area with the electron beam, while also tapping into the extreme confinement of graphene plasmons to generate high-frequency photons with relatively low-energy electrons available from tabletop sources. For 5 MeV electrons, a metamaterial of 50 layers and length 50 µm, and a beam current of 1.7 µA, it is, for instance, possible to generate X-rays of intensity 1.5 × 107 photons sr-1 s-1 1%BW, 580 times more than for a single-layer design. The frequency of the driving laser dynamically tunes the photon emission spectrum. This work demonstrates a unique free-electron light source, wherein the electron mean free path in a given material is longer than the device length, relaxing the requirements of complex electron beam systems and potentially paving the way to high-yield, compact, and tunable X-ray sources.

Ultrafast Multiharmonic Plasmon Generation by Optically Dressed Electrons.

Interactions between electrons and photons are a source of rich physics from atomic to astronomical scales. Here, we examine a new kind of electron-photon interaction in which an electron, modulated by light, radiates multiple harmonics of plasmons. The emitted plasmons can be femtosecond in duration and nanometer in spatial scale. The extreme subwavelength nature of the plasmons lowers the necessary input light intensity by at least 4 orders of magnitude relative to state-of-the-art strong-field processes involving bound or free electrons. The results presented here reveal a new means of ultrafast (10-1000 fs) interconversion between photonic and plasmonic energy, and a general scheme for generating spatiotemporally shaped ultrashort pulses in optical materials. More generally, our results suggest a route towards realizing analogues of fascinating physical phenomena like nonlinear Compton scattering in plasmonics and nanophotonics with relatively low intensities, slow electrons, and on nanometer length scales.

Metasurface-based multi-harmonic free-electron light source.

Metasurfaces are subwavelength spatial variations in geometry and material where the structures are of negligible thickness compared to the wavelength of light and are optimized for far-field applications, such as controlling the wavefronts of electromagnetic waves. Here, we investigate the potential of the metasurface near-field profile, generated by an incident few-cycle pulse laser, to facilitate the generation of high-frequency light from free electrons. In particular, the metasurface near-field contains higher-order spatial harmonics that can be leveraged to generate multiple higher-harmonic X-ray frequency peaks. We show that the X-ray spectral profile can be arbitrarily shaped by controlling the metasurface geometry, the electron energy, and the incidence angle of the laser input. Using ab initio simulations, we predict bright and monoenergetic X-rays, achieving energies of 30 keV (with harmonics spaced by 3 keV) from 5-MeV electrons using 3.4-eV plasmon polaritons on a metasurface with a period of 85 nm. As an example, we present the design of a four-color X-ray source, a potential candidate for tabletop multicolor hard X-ray spectroscopy. Our developments could help pave the way for compact multi-harmonic sources of high-energy photons, which have potential applications in industry, medicine, and the fundamental sciences.

Laser-Induced Linear-Field Particle Acceleration in Free Space.

Linear-field particle acceleration in free space (which is distinct from geometries like the linac that requires components in the vicinity of the particle) has been studied for over 20 years, and its ability to eventually produce high-quality, high energy multi-particle bunches has remained a subject of great interest. Arguments can certainly be made that linear-field particle acceleration in free space is very doubtful given that first-order electron-photon interactions are forbidden in free space. Nevertheless, we chose to develop an accurate and truly predictive theoretical formalism to explore this remote possibility when intense, few-cycle electromagnetic pulses are used in a computational experiment. The formalism includes exact treatment of Maxwell's equations and exact treatment of the interaction among the multiple individual particles at near and far field. Several surprising results emerge. We find that electrons interacting with intense laser pulses in free space are capable of gaining substantial amounts of energy that scale linearly with the field amplitude. For example, 30 keV electrons (2.5% energy spread) are accelerated to 61 MeV (0.5% spread) and to 205 MeV (0.25% spread) using 250 mJ and 2.5 J lasers respectively. These findings carry important implications for our understanding of ultrafast electron-photon interactions in strong fields.