Showing papers on "Free electron model published in 2021"

Constructing Electron lever in Perovskite Nanocrystal to Regulate Local Electron Density for Intensive Chemodynamic Therapy.

Abstract: The local electron density of an atom is one key factor that determines its chemical properties Regulating electron density can promote the atom's reactivity and so reduce the reaction activation energy, which is highly desired in many chemical applications Herein, we report an intra-crystalline electron lever strategy, which can regulate the electron density of reaction centre atoms via manipulating ambient lattice states, for Fenton activity improvement Typically, with the assistance of ultrasound, the Mn4+ -O-Fe3+ bond in BiFe097 Mn003 O3 perovskite nanocrystals can drive valence electrons and free electrons to accumulate on Fe atoms by a polarization electric field originated from the designed lattice strain The increase of electron density significantly improves the catalytic activity of Fe, decreasing the activation energy of BiFe097 Mn003 O3 -mediated Fenton reaction by 5255 %, and increasing the OH yield by 921-fold This study provides a new way to understand the sono-Fenton chemistry, and the increased OH production enables a highly effective chemodynamic therapy

Quantum Entanglement and Modulation Enhancement of Free-Electron-Bound-Electron Interaction.

Abstract: The modulation and engineering of the free-electron wave function bring new ingredients to the electron-matter interaction. We consider the dynamics of a free-electron passing by a two-level system fully quantum mechanically and study the enhancement of interaction from the modulation of the free-electron wave function. In the presence of resonant modulation of the free-electron wave function, we show that the electron energy loss and gain spectrum is greatly enhanced for a coherent initial state of the two-level system. Thus, a modulated electron can function as a probe of the atomic coherence. We further find that distantly separated two-level atoms can be entangled through interacting with the same free electron. Effects of modulation-induced enhancement can also be observed using a dilute beam of modulated electrons.

Optical coherence transfer mediated by free electrons

Abstract: We theoretically investigate the quantum-coherence properties of the cathodoluminescence (CL) emission produced by a temporally modulated electron beam. Specifically, we consider the quantum-optical correlations of CL produced by electrons that are previously shaped by a laser field. Our main prediction is the presence of phase correlations between the emitted CL field and the electron-modulating laser, even though the emission intensity and spectral profile are independent of the electron state. In addition, the coherence of the CL field extends to harmonics of the laser frequency. Since electron beams can be focused to below 1 A, their ability to transfer optical coherence could enable the ultra-precise excitation, manipulation, and spectrally resolved probing of nanoscale quantum systems.

Toward Atomic-Resolution Quantum Measurements with Coherently Shaped Free Electrons.

Abstract: 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 $({\mathbit{T}}_{2}/{\mathbit{T}}_{1})$. 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.

Polarization Shaping of Free-Electron Radiation by Gradient Bianisotropic Metasurfaces

Abstract: Free-electron radiation phenomena facilitate enticing potential to create light emission with highly tunable spectra, covering hard-to-reach frequencies ranging from microwave to X-ray. Consequently, they take part in many applications such as on-chip light sources, particle accelerators, and medical imaging. While their spectral tunability is extremely high, their polarizability is usually much harder to control. Such limitations are especially apparent in all free electron based spontaneous radiation sources, such as the Smith−Purcell (SP) radiation. Here, anomalous free-electron radiation phenomenon is demonstrated at the microwave regime from gradient bianisotropic metasurfaces, by using a phased dipole array to mimics moving charged particles. The phase gradient and the bianisotropy in metasurfaces provide new degrees of freedom for the polarization shaping of free-electron radiation, going beyond the common spectral and angular shaping. Remarkably, the observed anomalous free-electron radiation obeys a generalized SP formula derived from Fermat’s principle.

Optical Coherence Transfer Mediated by Free Electrons

Abstract: We investigate the optical coherence properties carried by the quantum state of a single free-flying charged and massive p article – the electron. We propose feasible Mach-Zehnder-like linear and nonlinear optical interferometric detection, incorporating electron-microscope beams.

Screening of a test charge in a free‐electron gas at warm dense matter and dense non‐ideal plasma conditions

Abstract: The screening of a test charge by partially degenerate non-ideal free electrons at conditions related to warm dense matter and dense plasmas is investigated using linear response theory and the local field correction based on ab inito Quantum Monte-Carlo simulations data. The analysis of the obtained results is performed by comparing to the random phase approximation and the Singwi-Tosi-Land-Sjolander approximation. The applicability of the long-wavelength approximation for the description of screening is investigated. The impact of electronic exchange-correlations effects on structural properties and the applicability of the screened potential from linear response theory for the simulation of the dynamics of ions are discussed.

Spontaneous and stimulated electron-photon interactions in nanoscale plasmonic near fields.

Abstract: The interplay between free electrons, light, and matter offers unique prospects for space, time, and energy resolved optical material characterization, structured light generation, and quantum information processing. Here, we study the nanoscale features of spontaneous and stimulated electron–photon interactions mediated by localized surface plasmon resonances at the tips of a gold nanostar using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Supported by numerical electromagnetic boundary-element method (BEM) calculations, we show that the different coupling mechanisms probed by EELS, CL, and PINEM feature the same spatial dependence on the electric field distribution of the tip modes. However, the electron–photon interaction strength is found to vary with the incident electron velocity, as determined by the spatial Fourier transform of the electric near-field component parallel to the electron trajectory. For the tightly confined plasmonic tip resonances, our calculations suggest an optimum coupling velocity at electron energies as low as a few keV. Our results are discussed in the context of more complex geometries supporting multiple modes with spatial and spectral overlap. We provide fundamental insights into spontaneous and stimulated electron-light-matter interactions with key implications for research on (quantum) coherent optical phenomena at the nanoscale.

Modulation of Cathodoluminescence Emission by Interference with External Light.

Abstract: Spontaneous processes triggered in a sample by free electrons, such as cathodoluminescence, are commonly regarded and detected as stochastic events. Here, we supplement this picture by showing through first-principles theory that light and free-electron pulses can interfere when interacting with a nanostructure, giving rise to a modulation in the spectral distribution of the cathodoluminescence light emission that is strongly dependent on the electron wave function. Specifically, for a temporally focused electron, cathodoluminescence can be canceled upon illumination with a spectrally modulated dimmed laser that is phase-locked relative to the electron density profile. We illustrate this idea with realistic simulations under attainable conditions in currently available ultrafast electron microscopes. We further argue that the interference between excitations produced by light and free electrons enables the manipulation of the ultrafast materials response by combining the spectral and temporal selectivity of the light with the atomic resolution of electron beams.

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

Abstract: 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.

Quantum entanglement and modulation enhancement of free-electron–bound-electron interaction

Abstract: We study the modulation enhancement of interaction and entanglement between distant atoms in the interaction between free electron and two-level atoms.

Optical polarization analogue in free electron beams

Abstract: Spectromicroscopy techniques with fast electrons can quantitatively measure the optical response of excitations with unrivalled spatial resolution. However, owing to their inherently scalar nature, electron waves cannot access the polarization-related quantities. Despite promising attempts based on the conversion of concepts originating from singular optics (such as vortex beams), the definition of an optical polarization analogue for fast electrons has remained an open question. Here we establish such an analogue using the dipole transition vector of the electron between two well-chosen singular wave states. We show that electron energy loss spectroscopy allows the direct measurement of the polarized electromagnetic local density of states. In particular, in the case of circular polarization, it directly measures the local optical spin density. This work establishes electron energy loss spectroscopy as a quantitative technique to tackle fundamental issues in nano-optics, such as super-chirality, local polarization of dark excitations or polarization singularities at the nanoscale. The functionality of electron energy loss spectroscopy can be extended to include a polarization analogue constructed via the dipole transition vector between two electronic states, bringing it closer to its optical counterpart.

Feshbach-Fano approach for calculation of Auger decay rates using equation-of-motion coupled-cluster wave functions. I. Theory and implementation

Abstract: X-ray absorption creates electron vacancies in the core shell. These highly excited states often relax by Auger decay—an autoionization process in which one valence electron fills the core hole and another valence electron is ejected into the ionization continuum. Despite the important role of Auger processes in many experimental settings, their first-principles modeling is challenging, even for small systems. The difficulty stems from the need to describe many-electron continuum (unbound) states, which cannot be tackled with standard quantum-chemistry methods. We present a novel approach to calculate Auger decay rates by combining Feshbach–Fano resonance theory with the equation-of-motion coupled-cluster single double (EOM-CCSD) framework. We use the core–valence separation scheme to define projectors into the bound (square-integrable) and unbound (continuum) subspaces of the full function space. The continuum many-body decay states are represented by products of an appropriate EOM-CCSD state and a free-electron state, described by a continuum orbital. The Auger rates are expressed in terms of reduced quantities, two-body Dyson amplitudes (objects analogous to the two-particle transition density matrix), contracted with two-electron bound-continuum integrals. Here, we consider two approximate treatments of the free electron: a plane wave and a Coulomb wave with an effective charge, which allow us to evaluate all requisite integrals analytically; however, the theory can be extended to incorporate a more sophisticated description of the continuum orbital.

Contribution of the carbon-originated hole trap to slow decays of photoluminescence and photoconductivity in homoepitaxial n-type GaN layers

Abstract: N-type GaN epitaxial layers grown via metal organic vapor-phase epitaxy typically exhibit a yellow luminescence (YL) band owing to carbon-related deep levels in the photoluminescence spectra. The decay of YL after pulse excitation involves a long time constant (∼0.2 ms at room temperature), whereas microwave photoconductivity decay (μ-PCD) curves show the corresponding component of the time constant. To clarify the origin of the long decay time, the temperature-dependent time constants of YL decay and μ-PCD curves are analyzed using a numerical model based on rate equations for trapping and emission through a deep level. The characteristics of the decays are well reproduced by a recombination model using a hole trap H1 at an energy of EV + 0.88 eV because of the acceptor-like state of carbon on a nitrogen site (CN) whose electron capture cross section (σn) is estimated to be 3 × 10−21 cm2. The slow decay in μ-PCD signals indicates that the electrons before being captured to H1 traps are free electrons in the conduction band. These findings indicate that the slow recombination process through CN results in tail currents in the turn-off switching periods of devices.

Measurement of Temporal Coherence of Free Electrons by Time-Domain Electron Interferometry.

Abstract: The temporal properties of an electron beam are decisive for modern ultrafast electron microscopy and for the quantum optics of the free electron in laser fields. Here, we report a time-domain interferometer that measures and distinguishes the pure and ensemble coherences of a free-electron beam in a transmission electron microscope via symmetry-breaking shifts of photon-order sideband peaks. This result is a free-electron analog to the reconstruction of attosecond busts and photoemission delays in optical attosecond spectroscopy. We find a substantial pure electron coherence that is connected to the thermodynamics of the emitter material and a lower ensemble coherence that is governed by space-charge effects. Pure temporal coherences above 5 fs are measured at $g{10}^{9}$ electrons per second in a high-brightness beam.

Negative entropy production rates in Drude-Sommerfeld metals

Abstract: It is commonly accepted that in typical situations the rate of entropy production is non-negative. We show that this assertion is not entirely correct, not even in the linear regime, if a time-dependent, external perturbation is not compensated by a rapid enough decay of the response function. This is demonstrated for three variants of the Drude model to describe electrical conduction in noble metals, namely the classical free electron gas, the Drude-Sommerfeld model, and the extended Drude-Sommerfeld model. The analysis is concluded with a discussion of potential experimental verifications and ramifications of negative entropy production rates.

Ultrafast Momentum-Resolved Free-Electron Probing of Optically Pumped Plasmon Thermal Dynamics

Abstract: Current advances in ultrafast electron microscopy make it possible to combine optical pumping of a nanostructure and electron beam probing with sub-Angstrom and femtosecond spatiotemporal resolutio...

Quantum Wave-Particle Duality in Free-Electron–Bound-Electron Interaction

Abstract: We present a comprehensive relativistic quantum-mechanical theory for interaction of a free electron with a bound electron in a model, where the free electron is represented as a finite-size quantum electron wave packet (QEW) and the bound electron is modeled by a quantum two-level system (TLS). The analysis reveals the wave-particle duality nature of the QEW, delineating the point-particle-like and wavelike interaction regimes and manifesting the physical reality of the wave function dimensions when interacting with matter. This QEW size dependence may be used for interrogation and coherent control of superposition states in a TLS and for enhancement of cathodoluminescence and electron energy-loss spectroscopy in electron microscopy.

Beyond Fermi's Golden Rule in Free-Electron Quantum Electrodynamics: Acceleration/Radiation Correspondence

Abstract: In this article, we present a unified reciprocal quantum electrodynamics (QED) formulation of quantum light-matter interaction. For electron-light interactions, we bridge the underlying theories of Photon-Induced Near-field Electron Microscopy (PINEM), Laser-induced Particle Accelerators and radiation sources, such as Free Electron Laser (FEL), transition radiation and Smith-Purcell effect. We demonstrate an electron-photon spectral reciprocity relation between the electron energy loss/gain and the radiation spectra. This "Acceleration/Radiation Correspondence" (ARC) conserves the electron-energy and photon-number exchanged and in the case of a Quantum Electron Wavepacket (QEW), displays explicit dependence on the history-dependent phase and shape of the QEW. It originates from an interaction-induced quantum interference term that is usually ignored in Fermi's Golden Rule analyses. We apply the general QED formulation to both stimulated interaction and spontaneous emission of classical and quantum light by the quantum-featured electrons. The 'spontaneous' emissions of coherent states ('classical' light) and squeezed states of light are shown to be enhanced with squeezed vacuum. This reciprocal ARC formulation has promise for extension to other fundamental research problems in quantum-light and quantum-matter interactions.

Terahertz Polaron Oscillations of Electrons Solvated in Liquid Water

Abstract: The terahertz (THz) response of solvated electrons in liquid water is studied in nonlinear ultrafast pump-probe experiments. Free electrons with concentrations from c_{e}=4 to 140×10^{-6} moles/liter are generated by high-field THz or near-infrared multiphoton excitation. The time-resolved change of the dielectric function as mapped by broadband THz pulses exhibits pronounced oscillations persisting up to 30 ps. Their frequency increases with electron concentration from 0.2 to 1.5 THz. The oscillatory response is assigned to impulsively excited coherent polarons involving coupled electron and water shell motions with a frequency set by the local electric field.

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

Abstract: 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.

Spatial Variations of Plasma Parameters in a Hollow Cathode Discharge

Abstract: The transformations of the electron energy distribution (EEDF), their concentration, and plasma space potential along the discharge gap between the hollow rectangular cathode and the mesh anode were experimentally studied. The discharge was 3 cm long, with a cross-section of 10 cm2. A new version of measurements with several single probes with the formation of current-voltage characteristics (IVC) in the probe circuit was proposed with the simultaneous application of voltages in the form of a combination of periodic and noise signals. The proportions of the signals were varied for different sections of the current-voltage characteristics. Measurements along the central axis of the discharge were taken. The dynamic range of the EEDF was not less than 4 orders of magnitude at the electron concentrations of 2–13 × 1010 cm−3, which exceeds the best known achievements. Measurements for discharge in helium at reduced pressures of 1–1.2 mbar and currents of 150–400 mA showed that the EEDFs differ from Maxwell ones, with an excess of fast electrons in the region of 10–20 eV at medium energies 4–6 eV. The fraction of fast electrons decreased in regions closer to the anode, which is associated with the nonlocality of the mechanism of the spectrum formation of free electrons. EEDFs transformations led to the space dependence of electron drift velocities on the plasma area. The dependence of the voltage drop across the cathode on the gas pressure and discharge current was noted.

A new imaging concept in spin polarimetry based on the spin‐filter effect

Abstract: The concept of an imaging-type 3D spin detector, based on the combination of spin-exchange interactions in the ferromagnetic (FM) film and spin selectivity of the electron-photon conversion effect in a semiconductor heterostructure, is proposed and demonstrated on a model system. This novel multichannel concept is based on the idea of direct transfer of a 2D spin-polarized electron distribution to image cathodoluminescence (CL). The detector is a hybrid structure consisting of a thin magnetic layer deposited on a semiconductor structure allowing measurement of the spatial and polarization-dependent CL intensity from injected spin-polarized free electrons. The idea is to use spin-dependent electron transmission through in-plane magnetized FM film for in-plane spin detection by measuring the CL intensity from recombined electrons transmitted in the semiconductor. For the incoming electrons with out-of-plane spin polarization, the intensity of circularly polarized CL light can be detected from recombined polarized electrons with holes in the semiconductor. In order to demonstrate the ability of the solid-state spin detector in the image-type mode operation, a spin detector prototype was developed, which consists of a compact proximity focused vacuum tube with a spin-polarized electron source [p-GaAs(Cs,O)], a negative electron affinity (NEA) photocathode and the target [semiconductor heterostructure with quantum wells also with NEA]. The injection of polarized low-energy electrons into the target by varying the kinetic energy in the range 0.5-3.0 eV and up to 1.3 keV was studied in image-type mode. The figure of merit as a function of electron kinetic energy and the target temperature is determined. The spin asymmetry of the CL intensity in a ferromagnetic/semiconductor (FM-SC) junction provides a compact optical method for measuring spin polarization of free-electron beams in image-type mode. The FM-SC detector has the potential for realizing multichannel 3D vectorial reconstruction of spin polarization in momentum microscope and angle-resolved photoelectron spectroscopy systems.

Observation of laser-assisted electron scattering in superfluid helium

Abstract: Laser-assisted electron scattering (LAES), a light-matter interaction process that facilitates energy transfer between strong light fields and free electrons, has so far been observed only in gas phase. Here we report on the observation of LAES at condensed phase particle densities, for which we create nano-structured systems consisting of a single atom or molecule surrounded by a superfluid He shell of variable thickness (32-340 angstrom). We observe that free electrons, generated by femtosecond strong-field ionization of the core particle, can gain several tens of photon energies due to multiple LAES processes within the liquid He shell. Supported by Monte Carlo 3D LAES and elastic scattering simulations, these results provide the first insight into the interplay of LAES energy gain/loss and dissipative electron movement in a liquid. Condensed-phase LAES creates new possibilities for space-time studies of solids and for real-time tracing of free electrons in liquids.

Electron Pulse Compression with Optical Beat Note

Abstract: Compressing electron pulses is important in many applications of electron beam systems. In this study, we propose to use optical beat notes to compress electron pulses. The beat frequency is chosen to match the initial electron pulse duration, which enables the compression of electron pulses with a wide range of durations. This functionality extends the optical control of electron beams, which is important in compact electron beam systems such as dielectric laser accelerators. We also find that the dominant frequency of the electron charge density changes continuously along its drift trajectory, which may open up new opportunities in coherent interaction between free electrons and quantum or classical systems.