Energy-gain Spectroscopy Research Articles

Electron energy-gain spectroscopy of optical excitations in integrated photonic structures

Electron energy-gain spectroscopy of optical excitations in integrated photonic structures

Accelerating Quantum Materials Development with Advances in Transmission Electron Microscopy.

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, superconductors, quantum dots, color center-hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, superconductivity, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the material's detailed atomic-scale structure, including atomic defects, dopants, and lattice stacking. In this review, we describe how progress in the field of electron microscopy (EM), including in situ and in operando EM, can accelerate advances in quantum materials and quantum excitations. We begin by describing fundamental EM principles and operation modes. We then discuss various EM methods such as (i) EM spectroscopies, including electron energy loss spectroscopy (EELS), cathodoluminescence (CL), and electron energy gain spectroscopy (EEGS); (ii) four-dimensional scanning transmission electron microscopy (4D-STEM); (iii) dynamic and ultrafast EM (UEM); (iv) complementary ultrafast spectroscopies (UED, XFEL); and (v) atomic electron tomography (AET). We describe how these methods could inform structure-function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable precision positioning of atomic defects and high-resolution manipulation of quantum materials. For each method, we also describe existing limitations to solve open quantum mechanical questions, and how they might be addressed to accelerate progress. Among numerous notable results, our review highlights how EM is enabling identification of the 3D structure of quantum defects; measuring reversible and metastable dynamics of quantum excitations; mapping exciton states and single photon emission; measuring nanoscale thermal transport and coupled excitation dynamics; and measuring the internal electric field and charge density distribution of quantum heterointerfaces- all at the quantum materials' intrinsic atomic and near atomic-length scale. We conclude by describing open challenges for the future, including achieving stable sample holders for ultralow temperature (below 10K) atomic-scale spatial resolution, stable spectrometers that enable meV energy resolution, and high-resolution, dynamic mapping of magnetic and spin fields. With atomic manipulation and ultrafast characterization enabled by EM, quantum materials will be poised to integrate into many of the sustainable and energy-efficient technologies needed for the 21st century.

Edge-induced excitations in Bi[formula omitted]Te[formula omitted] from spatially-resolved electron energy-gain spectroscopy

Among the many potential applications of topological insulator materials, their broad potential for the development of novel tunable plasmonics at THz and mid-infrared frequencies for quantum computing, terahertz detectors, and spintronic devices is particularly attractive. The required understanding of the intricate relationship between nanoscale crystal structure and the properties of the resulting plasmonic resonances remains, however, elusive for these materials. Specifically, edge- and surface-induced plasmonic resonances, and other collective excitations, are often buried beneath the continuum of electronic transitions, making it difficult to isolate and interpret these signals using techniques such as electron energy-loss spectroscopy (EELS). Here we focus on the experimentally clean energy-gain EELS region to characterise collective excitations in the topologically insulating material Bi2Te3 and correlate them with the underlying crystalline structure with nanoscale resolution. We identify with high significance the presence of a distinct energy-gain peak around −0.8eV, with spatially-resolved maps revealing that its intensity is markedly enhanced at the edge regions of the specimen. Our findings illustrate the reach of energy-gain EELS analyses to accurately map collective excitations in quantum materials, a key asset in the quest towards new tunable plasmonic devices.

Electron Energy-gain Spectroscopy of Optical Excitations in an Integrated Photonics Microresonator.

Electron Energy-gain Spectroscopy of Optical Excitations in an Integrated Photonics Microresonator.

Nanometer-Scale Spatial and Spectral Mapping of Exciton Polaritons in Structured Plasmonic Cavities.

Exciton polaritons (EPs) are ubiquitous light-matter excitations under intense investigation as test beds of fundamental physics and as components for all-optical computing. Owing to their unique attributes and facile experimental tunability, EPs potentially enable strong nonlinearities, condensation, and superfluidity at room temperature. However, the diffraction limit of light and the momentum content of fast electron probes preclude the characterization of EPs in nanoscale structured cavities exhibiting energy-momentum dispersion. Here we present fully relativistic analytical theory and companion numerical simulations showing that these limitations can be overcome to measure EPs in periodic nanophotonic cavities on their natural energy, momentum, and length scales via lattice electron energy gain spectroscopy. With the combined high momentum resolution of light and nanoscale spatial resolution of focused electron beams, lattice electron energy gain spectroscopy can expose deeply subwavelength EP features using currently available monochromated, aberration-corrected scanning transmission electron microscopes.

Visualizing Electric and Magnetic Field Coupling in Au-Nanorod Trimer Structures via Stimulated Electron Energy Gain and Cathodoluminescence Spectroscopy: Implications for Meta-Atom Imaging

Visualizing Electric and Magnetic Field Coupling in Au-Nanorod Trimer Structures via Stimulated Electron Energy Gain and Cathodoluminescence Spectroscopy: Implications for Meta-Atom Imaging

New Advances in Stimulated Electron Energy Gain and Loss Spectroscopy

Journal Article New Advances in Stimulated Electron Energy Gain and Loss Spectroscopy Get access Ben Wolf, Ben Wolf Waviks, Inc., Dallas, Texas, United States Search for other works by this author on: Oxford Academic Google Scholar Thomas Moore, Thomas Moore Waviks, Inc., Dallas, Texas, United States Search for other works by this author on: Oxford Academic Google Scholar Robyn Collette, Robyn Collette University of Tennessee, Knoxville, Tennessee, United States Search for other works by this author on: Oxford Academic Google Scholar David Garfinkel, David Garfinkel University of Tennessee, Knoxville, Tennessee, United States Search for other works by this author on: Oxford Academic Google Scholar Philip Rack Philip Rack University of Tennessee, Knoxville, Tennessee, United States Search for other works by this author on: Oxford Academic Google Scholar Microscopy and Microanalysis, Volume 26, Issue S2, 1 August 2020, Pages 1916–1918, https://doi.org/10.1017/S1431927620019820 Published: 01 August 2020

Nearfield excited state imaging of bonding and antibonding plasmon modes in nanorod dimers via stimulated electron energy gain spectroscopy

Stimulated electron energy loss and gain spectroscopy (sEELS and sEEGS) are used to image the nearfield of the bonding and antibonding localized surface plasmon resonance modes in nanorod dimers. A scanning transmission electron microscope equipped with an optical delivery system is used to simultaneously irradiate plasmonic nanorod dimers while electron energy loss and gain spectra of the active plasmons are collected. The length of the nanorod dimer is varied such that the bonding and antibonding modes are resonant with the laser energy. The optically bright bonding mode is clearly observed in the resonant sEEG spectrum images and, consistent with spontaneous EELS, no direct evidence of the hot spot is observed in sEEG. s-polarized irradiation does not stimulate the energy gain of the optically dark antibonding mode. However, when phase retardation is introduced by tilting the longitudinal axis, the otherwise dark antibonding mode becomes sEEG active.

Near field excited state imaging via stimulated electron energy gain spectroscopy of localized surface plasmon resonances in plasmonic nanorod antennas

Continuous wave (cw) photon stimulated electron energy loss and gain spectroscopy (sEELS and sEEGS) is used to image the near field of optically stimulated localized surface plasmon resonance (LSPR) modes in nanorod antennas. An optical delivery system equipped with a nanomanipulator and a fiber-coupled laser diode is used to simultaneously irradiate plasmonic nanostructures in a (scanning) transmission electron microscope. The nanorod length is varied such that the m = 1, 2, and 3 LSPR modes are resonant with the laser energy and the optically stimulated near field spectra and images of these modes are measured. Various nanorod orientations are also investigated to explore retardation effects. Optical and electron beam simulations are used to rationalize the observed patterns. As expected, the odd modes are optically bright and result in observed sEEG responses. The m = 2 dark mode does not produce a sEEG response, however, when tilted such that retardation effects are operative, the sEEG signal emerges. Thus, we demonstrate that cw sEEGS is an effective tool in imaging the near field of the full set of nanorod plasmon modes of either parity.

Stimulated electron energy loss and gain in an electron microscope without a pulsed electron gun

We report on a novel way of performing stimulated electron energy-loss and energy-gain spectroscopy (sEELS/sEEGS) experiments that does not require a pulsed gun. In this scheme, a regular scanning transmission electron microscope (STEM) equipped with a conventional continuous electron gun is fitted with a modified EELS detector and a light injector in the object chamber. The modification of the EELS detector allows one to expose the EELS camera during tunable time intervals that can be synchronized with nanosecond laser pulses hitting the sample, therefore allowing us to collect only those electrons that have interacted with the sample under light irradiation. Using ∼ 5 ns laser pulses of ∼ 2 eV photon energy on various plasmonic silver samples, we obtain evidence of sEELS/sEEGS through the emergence of up to two loss and gain peaks in the spectra at ± 2 and ± 4 eV. Because this approach does not involve any modification of the gun, our method retains the original performances of the microscope in terms of energy resolution and spectral imaging with and without light injection. Compared to pulsed-gun techniques, our method is mainly limited to a perturbative regime (typically no more that one gain event per incident electron), which allows us to observe resonant effects, in particular when the plasmon energy of a silver nanostructure matches the laser photon energy. In this situation, EELS and EEGS signals are enhanced in proportion to n+1 and n, respectively, where n is the average plasmon population due to the external illumination. The n term is associated with stimulated loss and gain processes, and the term of 1 corresponds to conventional (spontaneous) loss. The EELS part of the spectrum is therefore an incoherent superposition of spontaneous and stimulated EEL events. This is confirmed by a proper quantum-mechanical description of the electron/light/plasmon system incorporating light–plasmon and plasmon–electron interactions, as well as inelastic plasmon decay.

Temperature Measurement by a Nanoscale Electron Probe using Energy Gain and Loss Spectroscopy

Heat dissipation in integrated nanoscale devices is a major issue that requires the development of nanoscale temperature probes. Here, we report the implementation of a method that combines electron energy gain and loss spectroscopy to provide a direct measurement of the local temperature in the nanoenvironment. Loss and gain peaks corresponding to an optical-phonon mode in boron nitride were measured from room temperature to $\ensuremath{\sim}1600\text{ }\text{ }\mathrm{K}$. Both loss and gain peaks exhibit a shift towards lower energies as the sample is heated up. First-principles calculations of the temperature-induced phonon frequency shifts provide insights into the origin of this effect and confirm the experimental data. The experiments and theory presented here open the doors to the study of anharmonic effects in materials by directly probing phonons in the electron microscope.

Temperature Measurement by a Nanoscale Electron Probe Using Energy Gain and Loss Spectroscopy.

Heat dissipation in integrated nanoscale devices is a major issue that requires the development of nanoscale temperature probes. Here, we report the implementation of a method that combines electron energy gain and loss spectroscopy to provide a direct measurement of the local temperature in the nanoenvironment. Loss and gain peaks corresponding to an optical-phonon mode in boron nitride were measured from room temperature to ∼1600 K. Both loss and gain peaks exhibit a shift towards lower energies as the sample is heated up. First-principles calculations of the temperature-induced phonon frequency shifts provide insights into the origin of this effect and confirm the experimental data. The experiments and theory presented here open the doors to the study of anharmonic effects in materials by directly probing phonons in the electron microscope.

State-selected studies of electron capture by low-energy Neq+ (q = 3 - 5) ions from CO2 and H2O molecules

SynopsisTranslational energy-gain spectroscopy has been used to measure energy spectra and absolute total cross sections for single- and double-electron capture processes in low-energy collisions of Neq+ (q = 3 - 5) ions with H2O and CO2 at collision energies between 15 and 500 qeV.

Inverse Smith–Purcell effect near rough surfaces

Absorption of a photon by an electron moving parallel to a rough surface is studied. In the weak scattering regime we have evaluated the absorption probability of absorption of a single photon of energy ω. It is shown that the absorption probability with diffusional contribution becomes large by a lin/l ≫ 1 factor compared to the analogous result with the single scattering contribution. The maximum of probability takes place for the infrared wavelengths and strongly depends on the particle energy. We also discuss the case of two-dimensional periodical surface profile and indicate optimal conditions for maximal absorption probability. The results can be used in electron energy gain spectroscopy and in laser-driven acceleration.

Single-electron capture collisions of ground and metastable Ne2+ ions with molecular gases

Using the translational energy-gain spectroscopy technique, we have measured the energy-gain spectra and absolute total cross sections for single-electron capture in collisions of Ne2+ with N2, CO2 and H2O at laboratory impact energies between 50 and 400 eV and 0° scattering angles. In all the collision systems studied here, reaction channels have been observed which indicate the presence of the long-lived metastable states of (2s2 2p4 1D and 1S) in the Ne2+ incident beam. These measurements also indicate that capture from the metastable states into excited states of the projectile product ions is the most important inelastic process. Contributions from capture accompanied by the excitation and ionization of the target product are also detected. In addition, the energy dependence of the total single-electron capture cross sections is studied and found to slowly increase with increasing impact energy. The present data are compared with the theoretical calculations of the classical over the barrier, extended classical over the barrier and Landau–Zener models.

Multiple-electron capture by Ne6+ ions from H2O and CO2

Energy-gain spectra and total cross sections for single-, double-, and triple-electron capture processes in collisions of Ne6+ ions with H2O and CO2 at laboratory impact energies between 450 and 2400 eV have, been studied experimentally by means of translational energy-gain spectroscopy technique.

Theory of highly charged ion energy gain spectroscopy of molecular collective excitations

This paper discusses the physical mechanism by which a highly charged, energetic ion partly neutralized by electron transfers from a target—a large molecule, a cluster or a solid surface—can create target collective excitations in the process. We develop an analysis for the system of a highly charged ion flying by a fullerene molecule. Our analysis offers a new explanation for the periodic oscillations observed in the high-resolution energy gain spectra of energetic Arq+ ions (q=8, 13, 14, 15) flying by C60 molecules. For the Arq+→Ar(q−s)+ spectra with q=13–15 and s=1 or 2, the observed oscillations of 6 eV periodicity are assigned to energy losses due to multiple, Poissonian excitations of C60 π-plasmons (6 eV quantum). The excitation energy quanta are subtracted from the kinetic energy gained by the ion when one or at most two electrons are transferred to increasingly deep Rydberg states of the ion. The observed 3 eV periodicity for q=8 arises from the specific Rydberg energy levels of ArVIII (Ar7+). The first few shallow levels of this ion are separated by about 3 eV, while some of the pairs of adjacent, deeper levels are also separated by 3 eV. Each deep-level pair produces two interdigitated, Poissonian series of 6 eV π-plasmon excitation peaks resulting in an apparent periodicity of 3 eV throughout the spectra. The broad σ-plasmons (25 eV quantum) are found to contribute a background continuum to the medium- and high-energy regions of the observed spectra. The physical model analyzed here indicates that electronic collective excitations in several other systems could be studied by highly charged ion energy gain spectroscopy at sufficient resolution.

Highly charged ion energy gain spectroscopy of molecular excitations

We show that the measurement at high resolution of the kinetic-energy gain spectrum of a highly charged ion (HCI) scattered and partly neutralised by a molecule, a nanocluster or a surface can reveal the excitation spectrum of the target. As a first application of the analysis, we demonstrate that the periodic oscillations in the measured energy gain spectra of energetic Ar q + ions flying by C 60 molecules arise from the coherent multiple excitations of C 60 plasmons.

Total cross sections for electron capture processes in slow collisions of Ne6+ ions with H2O and CO2

Using the translation energy-gain spectroscopy technique, we have measured the energy-gain spectra and absolute total cross sections for single-electron capture by Ne6+ ions from H2O and CO2 at laboratory impact energies between 250 and 3000 eV.

State-selective single-electron capture in slow collisions of Neq+ (q = 2 – 5) ions with H2O

State-selective differential cross sections for single-electron capture processes in very slow collisions of Neq+ (q=2–5) ions with H2O have been studied experimentally at laboratory impact energies between 15 and 100 qeV and scattering angles between 0° and 8° by means of the translational energy-gain spectroscopy technique.