Interaction Of Free Electrons Research Articles

Total free-free Gaunt factors prediction using machine learning models

Gaunt factors are fundamental in describing the interaction of free electrons with photons, playing a crucial role in astrophysical processes such as radiation transport and emission spectra. Traditional methods for computing Gaunt factors involve complex integrations and intricate mathematical formulations, often being computationally expensive and time-consuming. This study explores an alternative approach using machine learning models to predict free-free Gaunt factors. Three models were employed: Artificial Neural Network (ANN), Support Vector Regression (SVR), and Gradient Boosting Regression (GBR). The obtained results demonstrate high performance, with R 2 scores ranging from 0.98 to 0.99, indicating the potential of machine learning models to accurately predict Gaunt factors.

Charge self-regulation over in-plane two-dimensional/two-dimensional hetero-cocatalyst for robust photocatalytic hydrogen generation

The rationally designing and constructing atomic-level heterointerface of two-dimensional (2D) chalcogenides is highly desirable to overcome the sluggish H2O-activation process toward efficient solar-driven hydrogen evolution. Herein, a novel in-plane 2D/2D molybdenum disulfide-rhenium disulfide (ReS2-MoS2) heterostructure is well-designed to induce the charge self-regulation of active site by forming electron-enriched Re(4−δ)+ and electron-deficient S(2−δ)− sites, thus collectively facilitating the activation of adsorbed H2O molecules and its subsequent H2 evolution. Furthermore, the obtained in-plane heterogenous ReS2-MoS2 nanosheet can powerfully transfer photoexcited electrons to inhibit photocarrier recombination as observed by advanced Kelvin probe measurement (KPFM), in-situ X-ray photoelectron spectroscopy (XPS) and femtosecond transient absorption spectroscopy (fs-TAS). As expected, the obtained ReS2-MoS2/TiO2 photocatalyst achieves an outperformed H2-generation rate of 6878.3 μmol h−1 g−1 with visualizing H2 bubbles in alkaline/neutral conditions. This work about in-plane 2D/2D heterostructure with strong free-electron interaction provides a promising strategy for designing novel and efficient catalysts for various applications.

Free-electron interaction with nonlinear optical states in microresonators.

The short de Broglie wavelength and strong interaction empower free electrons to probe structures and excitations in materials and biomolecules. Recently, electron-photon interactions have enabled new optical manipulation schemes for electron beams. In this work, we demonstrate the interaction of electrons with nonlinear optical states inside a photonic chip-based microresonator. Optical parametric processes give rise to spatiotemporal pattern formation corresponding to coherent or incoherent optical frequency combs. We couple such "microcombs" to electron beams, demonstrate their fingerprints in the electron spectra, and achieve ultrafast temporal gating of the electron beam. Our work demonstrates the ability to access solitons inside an electron microscope and extends the use of microcombs to spatiotemporal control of electrons for imaging and spectroscopy.

Free-electron-driven X-ray caustics from strained van der Waals materials

Tunable control of X-ray waves remains an open challenge of critical importance for applications in high-resolution X-ray spectroscopy, medical imaging, and radiation therapy. Unlike in the X-ray regime, control over light waves in the visible and IR regimes is ubiquitous in a vast range of applications, and typically relies on widely available optical components. However, analogous optical elements for X-rays are usually inefficient and challenging to fabricate. Here, we propose a method for shaping X-ray waves directly at the source, using the interaction of free electrons with crystalline materials. Specifically, by inducing strain on van der Waals materials, we control their interaction with free electrons in a manner that tunes the emissions of the X-rays and forms caustic X-ray beams. The development of wave-shaping concepts like caustics generation in the X-ray spectral range could benefit from achievements in this field in the optical range and may help bypass the noted limits of current X-ray optics technology. Looking forward, shaping the interference of X-rays at the atomic scale could enable further developments in high-resolution X-ray science.

Tailoring near-field-mediated photon electron interactions with light polarization

Inelastic interaction of free-electrons with optical near fields has recently attracted attention for manipulating and shaping free-electron wavepackets. Understanding the nature and the dependence of the inelastic cross section on the polarization of the optical near-field is important for both fundamental aspects and the development of new applications in quantum-sensitive measurements. Here, we investigate the effect of the polarization and the spatial profile of plasmonic near-field distributions on shaping free-electrons and controlling the energy transfer mechanisms, but also tailoring the electron recoil. We particularly show that polarization of the exciting light can be used as a control knop for disseminating the acceleration and deceleration path ways via the experienced electron recoil. We also demonstrate the possibility of tailoring the shape of the localized plasmons by incorporating specific arrangements of nanorods to enhance or hamper the transversal and longitudinal recoils of free-electrons. Our findings open up a route towards plasmonic near-fields-engineering for the coherent manipulation and control of slow electron beams for creating desired shapes of electron wavepackets.

Cavity-mediated electron-photon pairs.

Quantum information, communication, and sensing rely on the generation and control of quantum correlations in complementary degrees of freedom. Free electrons coupled to photonics promise novel hybrid quantum technologies, although single-particle correlations and entanglement have yet to be shown. In this work, we demonstrate the preparation of electron-photon pair states using the phase-matched interaction of free electrons with the evanescent vacuum field of a photonic chip-based optical microresonator. Spontaneous inelastic scattering produces intracavity photons coincident with energy-shifted electrons, which we employ for noise-suppressed optical mode imaging. This parametric pair-state preparation will underpin the future development of free-electron quantum optics, providing a route to quantum-enhanced imaging, electron-photon entanglement, and heralded single-electron and Fock-state photon sources.

Formation of Temporary Negative Ions and Their Subsequent Fragmentation upon Electron Attachment to CoQ0 and CoQ0 H2.

Ubiquinone molecules have a high biological relevance due to their action as electron carriers in the mitochondrial electron transport chain. Here, we studied the dissociative interaction of free electrons with CoQ0, the smallest ubiquinone derivative with no isoprenyl units, and its fully reduced form, 2,3‐dimethoxy‐5‐methylhydroquinone (CoQ0H2), an ubiquinol derivative. The anionic products produced upon dissociative electron attachment (DEA) were detected by quadrupole mass spectrometry and studied theoretically through quantum chemical and electron scattering calculations. Despite the structural similarity of the two studied molecules, remarkably only a few DEA reactions are present for both compounds, such as abstraction of a neutral hydrogen atom or the release of a negatively charged methyl group. While the loss of a neutral methyl group represents the most abundant reaction observed in DEA to CoQ0, this pathway is not observed for CoQ0H2. Instead, the loss of a neutral OH radical from the CoQ0H2 temporary negative ion is observed as the most abundant reaction channel. Overall, this study gives insights into electron attachment properties of simple derivatives of more complex molecules found in biochemical pathways.

High Magnetic Field Magneto-optics on Plasmonic Silica-Embedded Silver Nanoparticles

Tuning the plasmonic response with an external magnetic field is extremely promising to achieve active magnetoplasmonic devices, such as next generation refractometric sensors or tunable optical components. Noble metal nanostructures represent an ideal platform for studying and modeling magnetoplasmonic effects through the interaction of free electrons with external magnetic fields, even though their response is relatively low at the magnetic field intensities commonly applied in standard magneto-optical spectroscopies. Here we demonstrate a large magnetoplasmonic response of silver nanoparticles by performing magnetic circular dichroism spectroscopy at high magnetic fields, revealing a linear response to the magnetic field up to 30 T. The exploitation of such high fields allowed us to probe directly the field-induced splitting of circular plasmonic modes by performing absorption spectra with static circular polarizations, giving direct experimental evidence that the magneto-optical activity of plasmonic nanoparticles arises from the energy shift of field-split circular magnetoplasmonic modes.

Broadband Coupling of Fast Electrons to High-Q Whispering-Gallery Mode Resonators

Transmission electron microscopy is an excellent experimental tool to study the interaction of free electrons with nanoscale light fields. However, up to now, applying electron microscopy to quantum optical investigations was hampered by the lack of experimental platforms which allow a strong coupling between fast electrons and high-quality resonators. Here, as a first step, we demonstrate the broad-band excitation of optical whispering-gallery modes in silica microresonators by fast electrons. In the emitted coherent cathodoluminescence spectrum, a comb of equidistant peaks is observed, resulting in cavity quality factors larger than 700. These results enable the study of quantum optical phenomena in electron microscopy with potential applications in quantum electron-light metrology.

Shaping quantum photonic states using free electrons.

It is a long-standing goal to create light with unique quantum properties such as squeezing and entanglement. We propose the generation of quantum light using free-electron interactions, going beyond their already ubiquitous use in generating classical light. This concept is motivated by developments in electron microscopy, which recently demonstrated quantum free-electron interactions with light in photonic cavities. Such electron microscopes provide platforms for shaping quantum states of light through a judicious choice of the input light and electron states. Specifically, we show how electron energy combs implement photon displacement operations, creating displaced-Fock and displaced-squeezed states. We develop the theory for consecutive electron-cavity interactions with a common cavity and show how to generate any target Fock state. Looking forward, exploiting the degrees of freedom of electrons, light, and their interaction may achieve complete control over the quantum state of the generated light, leading to novel light statistics and correlations.

Quantum correlations in electron microscopy

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.

Doping and temperature dependence of nuclear spin relaxation in n -type GaAs

We investigate the strong field nuclear spin relaxation rate in $n$-type GaAs for doping densities from the quasi-insulating over the metal-to-insulator up to the quasimetallic regime. The rate measured at 6.5 K increases in the quasi-insulating regime with doping density due to nuclear spin diffusion to the donor electrons and shows a distinct maximum at the critical density of the Mott metal-to-insulator transition. The density dependence of the nuclear spin relaxation rate can be quantitatively calculated over the whole density regime taking into account the effective number of localized electrons and the interaction of free electrons via the Korringa mechanism. Only the nuclear spin relaxation rate of the very lowest doped sample shows a significant deviation from these calculations. Temperature-dependent measurements suggest in this case an additional nuclear spin relaxation channel which is negligible at higher doping densities and is linked to the electron spin relaxation time.

Coherent interaction between free electrons and a photonic cavity.

Advances in the research of interactions between ultrafast free electrons and light have introduced a previously unknown kind of quantum matter, quantum free-electron wavepackets1-5. So far, studies of the interactions of cavity-confined light with quantum matter have focused on bound electron systems, such as atoms, quantum dots and quantum circuits, which are considerably limited by their fixed energy states, spectral range and selection rules. By contrast, quantum free-electron wavepackets have no such limits, but so far no experiment has shown the influence of a photonic cavity on quantum free-electron wavepackets. Here we develop a platform for multidimensional nanoscale imaging and spectroscopy of free-electron interactions with photonic cavities. We directly measure the cavity-photon lifetime via a coherent free-electron probe and observe an enhancement of more than an order of magnitude in the interaction strength relative to previous experiments of electron-photon interactions. Our free-electron probe resolves the spatiotemporal and energy-momentum information of the interaction. The quantum nature of the electrons is verified by spatially mapping Rabi oscillations of the electron spectrum. The interactions between free electrons and cavity photons could enable low-dose, ultrafast electron microscopy of soft matter or other beam-sensitive materials. Such interactions may also open paths towards using free electrons for quantum information processing and quantum sensing. Future studies could achieve free-electron strong coupling6,7, photon quantum state synthesis8 and quantum nonlinear phenomena such as cavity electro-optomechanics9.

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.

Detection of Histamine Based on Gold Nanoparticles with Dual Sensor System of Colorimetric and Fluorescence.

Gold nanoparticles (Au-NPs), with the dual sensor system of colorimetric and fluorescence responses, were developed for the determination of histamine as a spoilage monitor for distinguishing lifetime and freshness of aquatic products. Upon addition of histamine, the absorption coefficient orders of magnitude via the interaction of free electrons and photons were affected, and the characteristic absorption peak of Au-NPs was red-shifted from 520 nm to 664 nm. Meanwhile, the large amino groups in the networks of histamine-Au-NPs with high molecular orbital exhibited excellent fluorescence behavior at 415 nm. Au-NPs offered a range of 0.001–10.0 μM and 0.01–1.0 μM with a limit of detection of 0.87 nM and 2.04 nM by UV-vis and fluorescence spectrum assay, respectively. Moreover, Au-NPs could be used to semiquantitatively analyze histamine with the naked eye, since the significant colorimetric and fluorescence reaction of Au-NPs solution that coincided with different concentrations of histamine can be observed as the histamine concentration was 0.1–1.0 μM. Both of the dual-sensor systems of Au-NPs were successfully applied to the quantitative analysis of histamine in fresh salmon muscle, suggesting the simplicity and rapidity in the dual detection approaches of Au-NPs might be suitable for spoilage assay of aquatic food to ensure food safety.

Nagaoka ferromagnetism observed in a quantum dot plaquette.

Engineered, highly controllable quantum systems are promising simulators of emergent physics beyond the simulation capabilities of classical computers1. An important problem in many-body physics is itinerant magnetism, which originates purely from long-range interactions of free electrons and whose existence in real systems has been debated for decades2,3. Here we use a quantum simulator consisting of a four-electron-site square plaquette of quantum dots4 to demonstrate Nagaoka ferromagnetism5. This form of itinerant magnetism has been rigorously studied theoretically6-9 but has remained unattainable in experiments. We load the plaquette with three electrons and demonstrate the predicted emergence of spontaneous ferromagnetic correlations through pairwise measurements of spin. We find that the ferromagnetic ground state is remarkably robust to engineered disorder in the on-site potentials and we can induce a transition to the low-spin state by changing the plaquette topology to an open chain. This demonstration of Nagaoka ferromagnetism highlights that quantum simulators can be used to study physical phenomena that have not yet been observed in any experimental system. The work also constitutes an important step towards large-scale quantum dot simulators of correlated electron systems.

Nonrelativistic electron\u2013electron M\xf8ller scattering in a nonadiabatic tunnel-ionizing surface plasmon field

Ultrafast processes occurring on nanoscale surfaces can be probed with ultrafast low-energy electron pulses. Specifically, for metallic samples, the interaction of free electrons with surface plasmon fields provides insight into the nanoscale electron dynamics at the surface. Current models and experiments include the interaction of electrons with the sample, but ignore electron–electron and electron–plasmon interactions. Here we show that secondary electrons and their interaction with the incident primary electrons via nonrelativistic Møller scattering in the presence of optical and surface plasmon fields significantly alters the electron dynamics probed with ultrafast low-energy electron microscopy. Modeling this electron–plasmon interaction is key for interpreting ultrafast electron dynamics on metallic surfaces.

Anomalous Photon-Induced Near-Field Electron Microscopy.

We reveal the classical and quantum regimes of free electron interaction with radiation, common to the general variety of radiation sources (e.g., a Smith-Purcell radiation), the dielectric laser accelerator, and photo-induced near-field electron microscopy (PINEM). Modeling the electron with initial conditions of a coherent quantum electron wave packet, its topology in phase space uniquely defines a universal distinction of three interaction regimes: point-particle-like acceleration, a quantum wave function (PINEM), and a newly reported regime of anomalous PINEM (APINEM). The quantum interference beat of APINEM is capable of improving the spectral resolution of postselective electron microscopy. The particle-wave duality transition between regimes reveals the history-dependent nature of quantum electron interaction with light.

Influence of the Local Field and Dipole-Dipole Interactions on the Spectral Characteristics of Simple Metals and Their Nanoparticles

The effect of dipole-dipole interactions of free electrons on the spectral characteristics of simple metals and their nanoparticles is analyzed using Drude theory and the model of the Lorentz local field. It is established that accounting for the dispersion of a local field under conditions of one-dimensional (1D) confinement based on the optical constants of the bulk metal allows the determination of its spectral micro-characteristics in the frequency region of the longitudinal collective motions of the free electrons. This corresponds to the spectra of the dielectric losses of bulk plasma oscillations. A similar procedure for three-dimensional (3D) confinement produces the spectrum of dielectric losses at the frequency of localized plasma oscillations. Using a number of simple metal examples, viz., Li, Na, and K, and also Al, Be, and Mg, it is shown that the frequencies of volume and localized plasma oscillations obtained from a model of dispersion of the local field in the long-wave limit are in good agreement with the actual frequencies of the plasma oscillations of the corresponding metals and the absorption maxima of their nanoparticles with a radius of 2–20 nm. It is shown that the frequencies of the main mode of longitudinal plasma oscillations and the absorption frequency of localized plasmons are well described using the dynamic theory of crystal lattice vibrations.

Harmonic generation in metal-insulator and metal-insulator-metal nanostructures

Large reduction in second and third harmonic signals is measured when a sub-nanometer-to-nanometer thick insulator film is deposited over a gold substrate. Such reduction in signal reveals the spilled-out electronic states in the insulator region at the vicinity of the metal-insulator (MI) interface, which are dubbed metal insulator gap states. For metal-insulator-metal (MIM) structures, we observe electric-field enhancement saturation and quenching of the third harmonic efficiencies well above the efficiencies for MI samples. The measured harmonics of incident light scattered from the MI and MIM systems are compared with detailed simulations that account for the nonlinear interactions of free electrons spilled out into the insulator and the nonlocality and electron quantum tunneling effects. Two insulator materials (ZnO and Al2O3) are used in the experiments, and atomic layer deposition is used to cover the gold substrate with variable thickness of the insulator films. On the basis of our simulations, we conclude that the observed MIM third-harmonic signal enhancement (and quenching) effects are primarily due to the nonlocal phenomena in an electron gas. As a consequence of our findings, second- and third-harmonic scattering signals can be analyzed to extract the spill-out electron density in the insulator.