Ultrafast Electron Microscopy Research Articles

Scanning ultrafast electron microscopy reveals photovoltage dynamics at a deeply buried p−Si/SiO2 interface

The understanding and control of charge carrier interactions with defects at buried insulator/semiconductor interfaces is essential for achieving optimum performance in modern electronics. Here, we report on the use of scanning ultrafast electron microscopy (SUEM) to remotely probe the dynamics of excited carriers at a Si surface buried below a thick thermal oxide. Our measurements illustrate a previously unidentified SUEM contrast mechanism, whereby optical modulation of the space-charge field in the semiconductor modulates the electric field in the thick oxide, thus affecting its secondary electron yield. By analyzing the SUEM contrast as a function of time and laser fluence we demonstrate the diffusion mediated capture of excited carriers by interfacial traps.

Transient Strain-Induced Electronic Structure Modulation in a Semiconducting Polymer Imaged by Scanning Ultrafast Electron Microscopy.

Understanding the optoelectronic properties of semiconducting polymers under external strain is essential for their applications in flexible devices. Although prior studies have highlighted the impact of static and macroscopic strains, assessing the effect of a local transient deformation before structural relaxation occurs remains challenging. Here, we employ scanning ultrafast electron microscopy (SUEM) to image the dynamics of a photoinduced transient strain in the semiconducting polymer poly(3-hexylthiophene) (P3HT). We observe that the photoinduced SUEM contrast, corresponding to the local change of secondary electron emission, exhibits an unusual ring-shaped profile. We attribute the observation to the electronic structure modulation of P3HT caused by a photoinduced strain field owing to its low modulus and strong electron-lattice coupling, supported by a finite-element analysis. Our work provides insights into tailoring optoelectronic properties using transient mechanical deformation in semiconducting polymers and demonstrates the versatility of SUEM to study photophysical processes in diverse materials.

Photo-Thermal Switching of Individual Plasmonically Activated Spin Crossover Nanoparticle Imaged by Ultrafast Transmission Electron Microscopy.

Spin crossover (SCO) is a promising switching phenomenon when implemented in electronic devices as molecules, thin films or nanoparticles. Among the properties modulated along this phenomenon, optically induced mechanical changes are of tremendous importance as they can work as fast light-induced mechanical switches or allow to investigate and control microstructural strains and fatigability. The development of characterization techniques probing nanoscopic behavior with high spatio-temporal resolution allows to trigger and visualize such mechanical changes of individual nanoscopic objects. Here, ultrafast transmission electron microscopy (UTEM) is used to precisely probe the length changes of individual switchable nanoparticles induced thermally by nanosecond laser pulses. This allows revealing of the mechanisms of spin switching, leading to the macroscopic expansion of SCO materials. This study is conducted on individual pure SCO nanoparticles and SCO nanoparticles encapsulating gold nanorods that serve for plasmonic heating under laser pulses. Length changes are compared with time-resolved optical measurements performed on an assembly of these particles.

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

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 5fs are measured at >10^{9} electrons per second in a high-brightness beam.

Phyllotaxis-inspired nanosieves with multiplexed orbital angular momentum

Nanophotonic platforms such as metasurfaces, achieving arbitrary phase profiles within ultrathin thickness, emerge as miniaturized, ultracompact and kaleidoscopic optical vortex generators. However, it is often required to segment or interleave independent sub-array metasurfaces to multiplex optical vortices in a single nano-device, which in turn affects the device’s compactness and channel capacity. Here, inspired by phyllotaxis patterns in pine cones and sunflowers, we theoretically prove and experimentally report that multiple optical vortices can be produced in a single compact phyllotaxis nanosieve, both in free space and on a chip, where one meta-atom may contribute to many vortices simultaneously. The time-resolved dynamics of on-chip interference wavefronts between multiple plasmonic vortices was revealed by ultrafast time-resolved photoemission electron microscopy. Our nature-inspired optical vortex generator would facilitate various vortex-related optical applications, including structured wavefront shaping, free-space and plasmonic vortices, and high-capacity information metaphotonics.

Correction to: Unconventional light‑induced states visualized by ultrafast electron diffraction and microscopy

Correction to: Unconventional light‑induced states visualized by ultrafast electron diffraction and microscopy

Ultrafast Transmission Electron Microscopy: Techniques and Applications

Abstract:With the growing applications of temporally resolved electron microscopy for probing basic phenomena and reducing beam-induced damage, a multifaceted introduction to the field of ultrafast transmission electron microscopy is provided. This primer includes techniques and equipment as well as implementation perspectives. Historical developments and recent technical advances will provide insight into ultrafast capabilities for research as well as educate electron microscopists on the general techniques. This technology review also includes applications enabled by ultrafast techniques using various sample stimuli from multidisciplinary fields.

Tunable Plasma Linearizer for Compensation of Nonlinear Energy Chirp

The removal of undesired nonlinear time-energy correlation (energy chirp) present in relativistic electron beams is crucial for many accelerator-based scientific applications, such as free-electron lasers, high-energy electron radiography, and MeV ultrafast electron microscopy. Here, we propose and demonstrate that a low-density plasma section can be used as a passive ``linearizer'' to significantly compensate for the nonlinear energy chirp imprinted on a beam by the curvature of the radio-frequency field in a conventional accelerator. Physically, the passage of the beam through the plasma excites a strong quasi-cosinoidal longitudinal decelerating wakefield that acts to mitigate the beam's nonlinear energy chirp by superimposing a reverse chirp on the beam. Time-resolved phase-space measurements, combined with high-fidelity three-dimensional particle-in-cell simulations show that the longitudinal phase space of the beam core is almost completely linearized, leading to a fourfold reduction of the beam overall energy spread from $0.148\mathrm{%}$ to $0.036\mathrm{%}$ (FWHM).

Point-to-point Coulomb effects in high brightness photoelectron beam lines for ultrafast electron diffraction

In an effort to increase spatial and temporal resolution of ultrafast electron diffraction and microscopy, ultra-high brightness photocathodes are actively sought to improve electron beam quality. Beam dynamics codes often approximate the Coulomb interaction with mean-field space charge, which is a good approximation in traditional beams. However, point-to-point Coulomb effects, such as disorder induced heating and the Boersch effect, can not be neglected in cold, dense beams produced by such photocathodes. In this paper, we introduce two new numerical methods to calculate the important effects of the photocathode image charge when using a point-to-point interaction model. Equipped with an accurate model of the image charge, we calculate the effects of point-to-point interactions on two high brightness photoemission beamlines for ultrafast diffraction. The first beamline uses a 200 keV gun, whereas the second uses a 5 MeV gun, each operating in the single-shot diffraction regime with $10^5$ electrons/pulse. Assuming a zero photoemission temperature, it is shown that including stochastic Coulomb effects increases the final emittance of these beamlines by over a factor of 2 and decreases the peak transverse phase space density by over a factor of 3 as compared to mean-field simulations. We then introduce a method to compute the energy released by disorder induced heating using the pair correlation function. This disorder induced heating energy was found to scale very near the theoretical result for stationary ultracold plasmas, and it accounts for over half of the emittance growth above mean-field simulations.

Imaging Nanometer Phonon Softening at Crystal Surface Steps with 4D Ultrafast Electron Microscopy.

Step edges are an important and prevalent topological feature that influence catalytic, electronic, vibrational, and structural properties arising from modulation of atomic-scale force fields due to edge-atom relaxation. Direct probing of ultrafast atomic-to-nanoscale lattice dynamics at individual steps poses a particularly significant challenge owing to demanding spatiotemporal resolution requirements. Here, we achieve such resolutions with femtosecond 4D ultrafast electron microscopy and directly image nanometer-variant softening of photoexcited phonons at individual surface steps. We find large degrees of softening precisely at the step position, with a thickness-dependent, strain-induced frequency modulation extending tens of nanometers laterally from the atomic-scale discontinuity. The effect originates from anisotropic bond dilation and photoinduced incoherent atomic displacements delineated by abrupt molecular-layer cessation. The magnitude and spatiotemporal extent of softening is quantitatively described with a finite-element transient-deformation model. The high spatiotemporal resolutions demonstrated here enable uncovering of new insights into atomic-scale structure-function relationships of highly defect-sensitive, functional materials.

Time-resolved cathodoluminescence in an ultrafast transmission electron microscope

Ultrafast transmission electron microscopy (UTEM) combines sub-picosecond time-resolution with the versatility of TEM spectroscopies. It allows us to study the ultrafast materials' response using complementary techniques. However, until now, time-resolved cathodoluminescence was unavailable in UTEM. In this paper, we report time-resolved cathodoluminescence measurements in an ultrafast transmission electron microscope. We mapped the spatial variations of the emission dynamics from nano-diamonds with a high density of NV centers with a 12 nm spatial resolution and sub-nanosecond temporal resolution. This development will allow us to study the emission dynamics from quantum emitters with a unique spatiotemporal resolution and benefit from the wealth of complementary signals provided by transmission electron microscopes. It will further expand the possibilities of ultrafast transmission electron microscopes, paving the way to the investigation of the quantum aspects of an electron/sample interaction.

Study on characteristics and beam emission theory of UTEM electron gun

In the ultrafast transmission electron microscopy (UTEM), the speed of the electron will be close to the light, when the electron pulse passes through the acceleration field. So the radiation effect will be produced when the electron beam moves at high speed, which will cause energy loss. In this paper, the performance of femtosecond mode photoemission gun is analyzed and studied by simplifying the electron gun model. According to the knowledge of electrodynamics, the radiation power of pulsed electron beam is deduced, and the corresponding radiation energy is obtained, which can provide a reference for the ultrafast dynamics research and design of the photoemission gun.

Unconventional light-induced states visualized by ultrafast electron diffraction and microscopy

Exciting electrons in solids with intense light pulses offers the possibility of generating new states of matter through nonthermal means and controlling their macroscopic properties on femto- to picosecond timescales. One way to manipulate a solid is by altering its lattice structure, which often underlies the electronic, magnetic and other phases. Here, we review how structures of solids are affected by photoexcitation and how their ultrafast dynamics are captured with time-resolved electron diffraction and microscopy. Specifically, we survey how a strong light pulse has been used to tailor the nonequilibrium characteristics to yield on-demand properties in various material classes. In the existing literature, four main routes have been exploited to control material structures: (i) phase competition, (ii) electronic correlations, (iii) excitation of coherent modes, and (iv) defect generation. In this review, we discuss experiments relevant to all four schemes and finish by speculating about future directions.

Transient lensing from an electron gas imaged by ultrafast electron microscopy

Transient lensing from an electron gas imaged by ultrafast electron microscopy

Radiation damage study of organic molecules via laser-free ultrafast transmission electron microscopy

Radiation damage study of organic molecules via laser-free ultrafast transmission electron microscopy

Ultrafast dynamics of photoinduced terahertz electron-hole plasma waves in semiconductor junctions

The ultrafast transport processes of electrons and holes excited by femtosecond laser pulses are essential for a better understanding of carrier dynamics in semiconductors. Transient optical techniques are commonly used to investigate the carrier excitation and transport in these materials. Recently, ultrafast scanning electron microscopy has been employed to elucidate the ballistic dynamics of such hot carriers near a $p\text{\ensuremath{-}}n$ junction. We provide here a model not only to explain the previously reported superfast expansion of electron-hole clouds but also to predict plasma wave behavior at high laser fluences. In addition to a bipolar junction, we also investigate the well structure of a $p\text{\ensuremath{-}}n\text{\ensuremath{-}}p$ junction sandwiched by insulating layers. By confining hot carriers inside junctions, these carriers begin to oscillate as a result of Coulomb interactions among carriers and with the intrinsic field at the depletion zone, leading to the occurrence of terahertz-scale plasma waves for potential applications as pulsed terahertz light sources.

Coherent Phonon Disruption and Lock-In during a Photoinduced Charge-Density-Wave Phase Transition.

Ultrafast manipulation of phase domains in quantum materials is a promising approach to unraveling and harnessing interwoven charge and lattice degrees of freedom. Here we find evidence for coupling of displacively excited coherent acoustic phonons (CAPs) and periodic lattice distortions (PLDs) in the intensely studied charge-density-wave material, 1T-TaS2, using 4D ultrafast electron microscopy (UEM). Initial photoinduced Bragg-peak dynamics reveal partial CAP coherence and localized c-axis dilations. Weak, partially coherent dynamics give way to higher-amplitude, increasingly coherent oscillations, the transition period of which matches that of photoinduced incommensurate domain growth and stabilization from the nearly-commensurate phase. With UEM imaging, it is found that phonon wave trains emerge from linear defects 100 ps after photoexcitation. The CAPs consist of coupled longitudinal and transverse character and propagate at anomalously high velocities along wave vectors independent from PLDs, instead being dictated by defect orientation. Such behaviors illustrate a means to control phases in quantum materials using defect-engineered coherent-phonon seeding.

Accurate prediction of mega-electron-volt electron beam properties from UED using machine learning

To harness the full potential of the ultrafast electron diffraction (UED) and microscopy (UEM), we must know accurately the electron beam properties, such as emittance, energy spread, spatial-pointing jitter, and shot-to-shot energy fluctuation. Owing to the inherent fluctuations in UED/UEM instruments, obtaining such detailed knowledge requires real-time characterization of the beam properties for each electron bunch. While diagnostics of these properties exist, they are often invasive, and many of them cannot operate at a high repetition rate. Here, we present a technique to overcome such limitations. Employing a machine learning (ML) strategy, we can accurately predict electron beam properties for every shot using only parameters that are easily recorded at high repetition rate by the detector while the experiments are ongoing, by training a model on a small set of fully diagnosed bunches. Applying ML as real-time noninvasive diagnostics could enable some new capabilities, e.g., online optimization of the long-term stability and fine single-shot quality of the electron beam, filtering the events and making online corrections of the data for time-resolved UED, otherwise impossible. This opens the possibility of fully realizing the potential of high repetition rate UED and UEM for life science and condensed matter physics applications.

Spatiotemporal Imaging of Thickness-Induced Band-Bending Junctions.

van der Waals materials exhibit naturally passivated surfaces and an ability to form versatile heterostructures to enable an examination of carrier transport mechanisms not seen in traditional materials. Here, we report a new type of homojunction termed a "band-bending junction" whose potential landscape depends solely on the difference in thickness between the two sides of the junction. Using MoS2 on Au as a prototypical example, we find that surface potential differences can arise from the degree of vertical band bending in thin and thick regions. Furthermore, by using scanning ultrafast electron microscopy, we examine the spatiotemporal dynamics of charge carriers generated at this junction and find that lateral carrier separation is enabled by differences in the band bending in the vertical direction, which we verify with simulations. Band-bending junctions may therefore enable new optoelectronic devices that rely solely on band bending arising from thickness variations to separate charge carriers.

Visualization of Plasmonic Couplings Using Ultrafast Electron Microscopy.

Hybrids of graphene and metal plasmonic nanostructures are promising building blocks for applications in optoelectronics, surface-enhanced scattering, biosensing, and quantum information. An understanding of the coupling mechanism in these hybrid systems is of vital importance to its applications. Previous efforts in this field mainly focused on spectroscopic studies of strong coupling within the hybrids with no spatial resolution. Here we report direct imaging of the local plasmonic coupling between single Au nanocapsules and graphene step edges at the nanometer scale by photon-induced near-field electron microscopy in an ultrafast electron microscope for the first time. The proximity of a step in the graphene to the nanocapsule causes asymmetric surface charge density at the ends of the nanocapsules. Computational electromagnetic simulations confirm the experimental observations. The results reported here indicate that this hybrid system could be used to manipulate the localized electromagnetic field on the nanoscale, enabling promising future plasmonic devices.