Ultrafast Electron Microscopy Research Articles

Precision-controlled ultrafast electron microscope platforms. A case study: Multiple-order coherent phonon dynamics in 1T-TaSe2 probed at 50 fs-10 fm scales.

We report on the first detailed beam tests attesting the fundamental principle behind the development of high-current-efficiency ultrafast electron microscope systems where a radio frequency (RF) cavity is incorporated as a condenser lens in the beam delivery system. To allow for the experiment to be carried out with a sufficient resolution to probe the performance at the emittance floor, a new cascade loop RF controller system is developed to reduce the RF noise floor. Temporal resolution at 50 fs in full-width-at-half-maximum and detection sensitivity better than 1% are demonstrated on exfoliated 1T-TaSe2 system under a moderate repetition rate. To benchmark the performance, multi-terahertz edge-mode coherent phonon excitation is employed as the standard candle. The high temporal resolution and the significant visibility to very low dynamical contrast in diffraction signals via high-precision phase-space manipulation give strong support to the working principle for the new high-brightness femtosecond electron microscope systems.

Spatiotemporal Visualization of Photogenerated Carriers on an Avalanche Photodiode Surface Using Ultrafast Scanning Electron Microscopy

The spatiotemporal evolution of photogenerated charge carriers on surfaces and at interfaces of photoactive materials is an important issue for understanding fundamental physical processes in optoelectronic devices and advanced materials. Conventional optical probe-based microscopes that provide indirect information about the dynamic behavior of photogenerated carriers are inherently limited by their poor spatial resolution and large penetration depth. Herein, we develop an ultrafast scanning electron microscope (USEM) with a planar emitter. The photoelectrons per pulse in this USEM can be two orders of magnitude higher than that of a tip emitter, allowing the capture of high-resolution spatiotemporal images. We used the contrast change of the USEM to examine the dynamic nature of surface carriers in an InGaAs/InP avalanche photodiode (APD) after femtosecond laser excitation. It was observed that the photogenerated carriers showed notable longitudinal drift, lateral diffusion, and carrier recombination associated with the presence of photovoltaic potential at the surface. This work demonstrates an in situ multiphysics USEM platform with the capability to stroboscopically record carrier dynamics in space and time.

Characterization of a LaB6 tip as a thermionically enhanced photoemitter

There is a widespread interest in time-resolved electron spectroscopies such as ultrafast electron diffraction, ultrafast electron microscopy, and ultrafast electron energy loss spectroscopy. These techniques require pulsed electron beams with both high current and brightness. LaB6 is commonly used as a thermionic emitter because of its low work function and high electron yield. However, its use as a pulsed photocathode has not been widely explored. Here, we present measurements of the electron yield from a LaB6 filament exposed to 392 nm UV ultrafast laser pulses under a wide range of filament temperatures. We find that sample heating strongly enhances photoelectron yield, an effect known as thermionically enhanced photoemission. However, it also creates potentially undesirable, continuous thermionic background. We conclude that the ideal optimal operating conditions strongly depend on the type of measurement and require defining and quantifying an appropriate figure of merit.

(Invited) Photo-Assisted Electron Emission from Silicon-Based Electron Emission Devices

Ultrafast pulsed electron sources with spatial coherence have attracted significant interest in emerging applications such as scientific instruments of ultrafast electron microscopy [1-3] and electron beam lithography [4], and also as sources of X-ray [5] and micro- and THz-waves [6-9]. In particular, high-frequency electron bunch trains generated directly from the cathode surface can not only dramatically reduce dimensions and weight through the elimination of the pre-modulation circuit, but can also provide extremely high efficiency and improve the power in the electron beam devices due to coherence effects.One solution is employing photoemission from electron sources driven by ultrashort laser pulses for such emerging applications. Metallic flat photocathodes and recently metallic nanotips have been employed. However, a low quantum efficiency (QE), typically of approximately 0.01 %, and a large work function require a high-power UV laser to generate an intense electron beam. Negative electron affinity (NEA) semiconductor photocathodes such as NEA GaAs can provide QE as high as ~ 10 % [10], operating using visible laser light irradiation. However, the NEA surface is fragile and easily damaged by residual gas adsorption or beam extraction.In this presentation, we introduce the research and development of gated Si-FEAs with a volcano structure and planar-type electron emission devices based on a MOS diode structure and discuss the potential of the devices as a photocathode of the devices operating without NEA surface treatment. We investigate the optical properties of emitted electrons from the devices under visible laser light irradiation. The results indicate that Si-based electron emission devices with a fully optimized structure hold promise as a photocathode with a high QE and a high-speed response for generating a train of ultrashort electron bunches, operating without NEA surface treatment.

Ultrafast dynamics of a photoinduced phase transition in single-crystal trititanium pentoxide

We investigate photoinduced phase transition of Ti3O5 using the pump-probe method in an ultrafast electron microscope. We measured time-resolved electron diffraction patterns of single-crystal lamellae of Ti3O5 excited by the femtosecond laser at the wavelength of 800 and 400 nm. Under 800 nm laser excitation, the photoinduced phase transition from the β-phase to the λ-phase with a similar timescale to previous measurements conducted using nanocrystals was observed. This indicates that the photoinduced phase transition is not a phenomenon influenced by the material surface, size, or boundary, but an intrinsic property in a bulk crystal of Ti3O5. The photoinduced phase transition was not detected, when excited by the laser at the wavelength of 400 nm. The results are discussed based on the electronic states of β-Ti3O5 and λ-Ti3O5. The density of the dissociated interatomic bonds between Ti at the specific site should be an important factor for triggering the photoinduced phase transition.

Nanoscale and ultrafast in situ techniques to probe plasmon photocatalysis

Plasmonic photocatalysis uses the light-induced resonant oscillation of free electrons in a metal nanoparticle to concentrate optical energy for driving chemical reactions. By altering the joint electronic structure of the catalyst and reactants, plasmonic catalysis enables reaction pathways with improved selectivity, activity, and catalyst stability. However, designing an optimal catalyst still requires a fundamental understanding of the underlying plasmonic mechanisms at the spatial scales of single particles, at the temporal scales of electron transfer, and in conditions analogous to those under which real reactions will operate. Thus, in this review, we provide an overview of several of the available and developing nanoscale and ultrafast experimental approaches, emphasizing those that can be performed in situ. Specifically, we discuss high spatial resolution optical, tip-based, and electron microscopy techniques; high temporal resolution optical and x-ray techniques; and emerging ultrafast optical, x-ray, tip-based, and electron microscopy techniques that simultaneously achieve high spatial and temporal resolution. Ab initio and classical continuum theoretical models play an essential role in guiding and interpreting experimental exploration, and thus, these are also reviewed and several notable theoretical insights are discussed.

Research on the ultrafast laser in microscopy

Ultrafast laser technology has been making a huge difference in different areas, such as material processing, laser surgery, and military usage. In parallel with the development of ultrafast lasers, microscopy also greatly promotes modern science, even though there are still some shortcomings, and one of them is that it is hard to obtain information about dynamic samples. However, this shortcoming can be solved by using ultrafast laser technology. This review will introduce the concept of ultrafast laser technology and electron microscopy, while several limitations of conventional electron microscopy will be mentioned. This paper also introduces two advanced technology in ultrafast microscopy. Nowadays, by taking advantage of ultrafast laser technology, the dynamic sample can be observed with highly improved temporal resolutions, which are basically restricted by the duration of pulses, but the ultrafast laser technology makes the duration even reach the range of attoseconds. However, there are some limitations, such as aberration, still hamper the development of high spatial resolution in microscopy. It is hoped that the ultrafast microscopy will break through the bottleneck of traditional microscopy in the future.

Perspective andprospects ofin situ transmission/scanning transmission electron microscopy.

In situ transmission/scanning transmission electron microscopy (TEM/STEM) measurements have taken a central stage for establishing structure-chemistry-property relationship over the past couple of decades. The challenges for realizing 'a lab-in-gap', i.e.gap between the objective lens pole pieces, or 'a lab-on-chip', to be used to carry out experiments are being met through continuous instrumental developments. Commercially available TEM columns and sample holder, that have been modified for in situ experimentation, have contributed to uncover structural and chemical changes occurring in the sample when subjected to external stimulus such as temperature, pressure, radiation (photon, ions and electrons), environment (gas, liquid and magnetic or electrical field) or a combination thereof. Whereas atomic resolution images and spectroscopy data are being collected routinely using TEM/STEM, temporal resolution is limited to millisecond. On the other hand, better than femtosecond temporal resolution can be achieved using an ultrafast electron microscopy or dynamic TEM, but the spatial resolution is limited to sub-nanometers. In either case, in situ experiments generate large datasets that need to be transferred, stored and analyzed. The advent of artificial intelligence, especially machine learning platforms, is proving crucial to deal with this big data problem. Further developments are still needed in order to fully exploit our capability to understand, measure and control chemical and/or physical processes. We present the current state of instrumental and computational capabilities and discuss future possibilities.

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.

Photodiode-based time zero determination for ultrafast electron microscopy.

Pump-probe experiments in ultrafast electron microscopy require temporal overlap between the pump and probe pulses. Accurate measurements of the time delay between them allows for the determination of the time zero, the moment in time where both pulses perfectly overlap. In this work, we present the use of a photodiode-based alignment method for these time zero measurements. The cheap and easy-to-use device consists of a photodiode in a sample holder and enables us to temporally align individual, single-electron pulses with femtosecond laser pulses. In a first device, a temporal resolution of 24 ps is obtained, limited by the photodiode design. Future work will utilize a smaller photodiode with a lower capacitance, which will increase the temporal resolution and add spatial resolution as well. This upgrade will bring the method toward the micrometer and picosecond spatiotemporal resolution.

Sub-terahertz nearfields for electron-pulse compression.

The advent of ultrafast science with pulsed electron beams raised the need to control the temporal features of the electron pulses. One promising suggestion is the nano-selective quantum optics with multi-electrons, which scales quadratically with the number of electrons within the coherence time of the quantum system. Terahertz (THz) radiation from optical nonlinear crystals is an attractive methodology to generate the rapidly varying electric fields necessary for electron compression, with the advantage of an inherent temporal locking to laser-triggered electrons, such as in ultrafast electron microscopes. Longer (picosecond-) pulses require a sub-THz field for their compression. However, the generation of such low frequencies requires pumping with energetic optical pulses and their focusability is fundamentally limited by their mm-wavelength. This work proposes electron-pulse compression with sub-THz fields directly in the vicinity of their dipolar origin, thereby avoiding mediation through radiation. We analyze the merits of nearfields for compression of slow electrons, particularly in challenging regimes for THz radiation, such as small numerical apertures, micro-joule-level optical pump pulses, and low frequencies. This scheme can be implemented within the tight constraints of electron microscopes and reach fields of a few kV/cm below 0.1 THz at high repetition rates. Our paradigm offers a realistic approach for controlling electron pulses spatially and temporally in many experiments, opening the path of flexible multi-electron manipulation for analytic and quantum sciences.

Capturing the non-equilibrium state in light–matter–free-electron interactions through ultrafast transmission electron microscopy

Ultrafast transmission electron microscope (UTEM) with the multimodality of time-resolved diffraction, imaging, and spectroscopy provides a unique platform to reveal the fundamental features associated with the interaction between free electrons and matter. In this review, we summarize the principles, instrumentation, and recent developments of the UTEM and its applications in capturing dynamic processes and non-equilibrium transient states. The combination of the transmission electron microscope with a femtosecond laser via the pump–probe method guarantees the high spatiotemporal resolution, allowing the investigation of the transient process in real, reciprocal and energy spaces. Ultrafast structural dynamics can be studied by diffraction and imaging methods, revealing the coherent acoustic phonon generation and photo-induced phase transition process. In the energy dimension, time-resolved electron energy-loss spectroscopy enables the examination of the intrinsic electronic dynamics of materials, while the photon-induced near-field electron microscopy extends the application of the UTEM to the imaging of optical near fields with high real-space resolution. It is noted that light–free-electron interactions have the ability to shape electron wave packets in both longitudinal and transverse directions, showing the potential application in the generation of attosecond electron pulses and vortex electron beams.

Real-time electron clustering in an event-driven hybrid pixel detector

Event-driven hybrid pixel detectors with nanosecond time resolution have opened up novel pathways in modern ultrafast electron microscopy, for example in hyperspectral electron-energy loss spectroscopy or free-electron quantum optics. However, the impinging electrons typically excite more than one pixel of the device, and an efficient algorithm is therefore needed to convert the measured pixel hits to real single-electron events. Here we present a robust clustering algorithm that is fast enough to find clusters in a continuous stream of raw data in real time. Each tuple of position and arrival time from the detector is continuously compared to a buffer of previous hits until the probability of a merger with an old event becomes irrelevant. In this way, the computation time becomes independent of the density of electron arrival and the algorithm does not break the operation chain. We showcase the performance of the algorithm with a ‘timepix’ camera in two regimes of electron microscopy, in continuous beam emission and laser-triggered femtosecond mode.

Lossless Monochromator in an Ultrafast Electron Microscope Using Near-Field THz Radiation.

The ability to form monoenergetic electron beams is vital for high-resolution electron spectroscopy and imaging. Such capabilities are commonly achieved using an electron monochromator, which energy filters a dispersed electron beam, thus reducing the electron flux to yield down to meV energy resolution. This reduction in flux hinders the use of monochromators in many applications, such as ultrafast transmission electron microscopes (UTEMs). Here, we develop and demonstrate a mechanism for electron energy monochromation that does not reduce the flux-a lossless monochromator. The mechanism is based on the interaction of free-electron pulses with single-cycle THz near fields, created by nonlinear conversion of an optical laser pulse near the electron beam path inside a UTEM. Our experiment reduces the electron energy spread by a factor of up to 2.9 without compromising the beam flux. Moreover, as the electron-THz interaction takes place over an extended region of many tens of microns in free space, the realized technique is highly robust-granting uniform monochromation over a wide area, larger than the electron beam diameter. We further demonstrate the wide tunability of our method by monochromating the electron beam at multiple primary electron energies from 60 to 200keV, studying the effect of various electron and THz parameters on its performance. Our findings have direct applications in the fast-growing field of ultrafast electron microscopy, allowing time- and energy-resolved studies of exciton physics, phononic vibrational resonances, charge transport effects, and optical excitations in the mid IR to the far IR.

Efficiently accelerated free electrons by metallic laser accelerator

Strong electron-photon interactions occurring in a dielectric laser accelerator provide the potential for development of a compact electron accelerator. Theoretically, metallic materials exhibiting notable surface plasmon-field enhancements can possibly generate a high electron acceleration capability. Here, we present a design for metallic material-based on-chip laser-driven accelerators that show a remarkable electron acceleration capability, as demonstrated in ultrafast electron microscopy investigations. Under phase-matching conditions, efficient and continuous acceleration of free electrons on a periodic nanostructure can be achieved. Importantly, an asymmetric spectral structure in which the vast majority of the electrons are in the energy-gain states has been obtained by means of a periodic bowtie-structure accelerator. Due to the presence of surface plasmon enhancement and nonlinear optical effects, the maximum acceleration gradient can reach as high as 0.335 GeV/m. This demonstrates that metallic laser accelerator could provide a way to develop compact accelerators on chip.

Probing electron and lattice dynamics by ultrafast electron microscopy: Principles and applications

AbstractMicroscale charge and energy transfer is an ultrafast process that can determine the photoelectrochemical performance of devices. However, nonlinear and nonequilibrium properties hinder our understanding of ultrafast processes; thus, the direct imaging strategy has become an effective means to uncover ultrafast charge and energy transfer processes. Due to diffraction limits of optical imaging, the obtained optical image has insufficient spatial resolution. Therefore, electron beam imaging combined with a pulse laser showing high spatial–temporal resolution has become a popular area of research, and numerous breakthroughs have been achieved in recent years. In this review, we cover three typical ultrafast electron beam imaging techniques, namely, time‐resolved photoemission electron microscopy, scanning ultrafast electron microscopy, and ultrafast transmission electron microscopy, in addition to the principles and characteristics of these three techniques. Some outstanding results related to photon–electron interactions, charge carrier transport and relaxation, electron–lattice coupling, and lattice oscillation are also reviewed. In summary, ultrafast electron beam imaging with high spatial–temporal resolution and multidimensional imaging abilities can promote the fundamental understanding of physics, chemistry, and optics, as well as guide the development of advanced semiconductors and electronics.

Artifact Elimination in Ultrafast Electron Microscopy.

Artifact Elimination in Ultrafast Electron Microscopy.

Laser-Driven Transient Phase Oscillations in Individual Spin Crossover Particles.

An unusual expansion dynamics of individual spin crossover nanoparticles is studied by ultrafast transmission electron microscopy. After exposure to nanosecond laser pulses, the particles exhibit considerable length oscillations during and after their expansion. The vibration period of 50-100ns is of the same order of magnitude as the time that the particles need for a transition from the low-spin to the high-spin state. The observations are explained in Monte Carlo calculations using a model where elastic and thermal coupling between the molecules within a crystalline spin crossover particle govern the phase transition between the two spin states. The experimentally observed length oscillations are in agreement with the calculations, and it is shown that the system undergoes repeated transitions between the two spin states until relaxation in the high-spin state occurs due to energy dissipation. Spin crossover particles are therefore a unique system where a resonant transition between two phases occurs in a phase transformation of first order.

Characterization of transverse electron pulse trains using RF powered traveling wave metallic comb striplines

Advancements in ultrafast electron microscopy have allowed elucidation of spatially selective structural dynamics. However, as the spatial resolution and imaging capabilities have made progress, quantitative characterization of the electron pulse trains has not been reported at the same rate. In fact, inexperienced users have difficulty replicating the technique because only a few dedicated microscopes have been characterized thoroughly. Systems replacing laser driven photoexcitation with electrically driven deflectors especially suffer from a lack of quantified characterization because of the limited quantity. The primary advantages to electrically driven systems are broader frequency ranges, ease of use and simple synchronization to electrical pumping. Here, we characterize the technical parameters for electrically driven UEM including the shape, size and duration of the electron pulses using low and high frequency chopping methods. At high frequencies, pulses are generated by sweeping the electron beam across a chopping aperture. For low frequencies, the beam is continuously forced off the optic axis by a DC potential, then momentarily aligned by a countering pulse. Using both methods, we present examples that measure probe durations of 2 ns and 10 ps for the low and high frequency techniques, respectively. We also discuss how the implementation of a pulsed probe affects STEM imaging conditions by adjusting the first condenser lens.

Development and applications ofultrafast transmission electron microscopy.

We present a review on the development and applications of the ultrafast transmission electron microscopy (UTEM) at RIKEN. We introduce the UTEM system for the pump-probe TEM observation in a wide temporal range. By combining the UTEM and pixelated detector, we further develop five-dimansional scanning TEM (5D STEM) which provides the ultrafast nanoscale movie of physical quantities in nano-materials, such as crystal lattice information and electromagnetic field, by convergent-beam electron diffraction (CBED) and differential phase contrast (DPC) imaging technique. We show our recent results on the nanosecond-to-microsecond magnetic skyrmion dynamics observed by Lorentz TEM (LTEM) and photo-induced acoustic wave generation in picosecond regime by bright-field TEM and electron diffraction measurements by UTEM. We also show the demonstartion of the 5D STEM on the quantitative time (t)-dependent strain mapping by CBED with an accuracy of 4 ps and 8 nm, and the ultrafast demagnetization under zero magnetic field observed by DPC with 10 ns and 400 nm resolution.