Ultrafast Transmission Electron Microscopy Research Articles

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.

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.

Advances on in situ TEM mechanical testing techniques: a retrospective and perspective view

Over the past few decades, in situ transmission electron microscopy (TEM) has emerged as a powerful experimental technique for materials design and characterization. It offers unparalleled dynamic details of materials deformation under mechanical stimuli, providing fundamental insights into their deformation and failure mechanisms for various materials. In this review, we summarize recent advances on in situ TEM mechanical characterization techniques, including classical tension holders, nanoindentation holders, MEMS devices, thermal bimetallic-based techniques, and nanomanipulation techniques. The advantages and limitations of in situ TEM tests are also discussed. To provide a broader perspective, the article highlights promising opportunities for in situ TEM mechanical testing studies in characterization-processing-manufacturing based on nanomanipulation, ultrafast TEM, electron beam irradiation environmental conditions, data-driven machine learning, and integrated experimental and simulation characterization. This article aims to provide a comprehensive understanding of in situ TEM-based mechanical characterization techniques to promote the development of novel materials with improved mechanical properties for various applications.

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.

Dynamics of optical vortices in van der Waals materials

Quantized vortices are topological defects found in different two-dimensional geometries, from liquid crystals to ferromagnets, famously involved in spontaneous symmetry breaking and phase transitions. Their optical counterparts appear in planar geometries as a universal wave phenomenon, possessing topologically protected orbital angular momentum (OAM). So far, the spatiotemporal dynamics of optical vortices, including vortex-pair creation and annihilation, has been observed only in Bose–Einstein condensates. Here we observe optical vortices in van der Waals materials and measure their dynamics, including events of pair creation and annihilation. Vortices of opposite OAM are involved in pair creation/annihilation events, and their relative signs determine the surrounding field profile throughout their motion. The vortices are made of phonon polaritons in hexagonal boron nitride, which we directly probe using free electrons in an ultrafast transmission electron microscope. Our findings promote future investigations of vortex phenomena in van der Waals platforms, toward their use for chiral plasmonics, quantum simulators, and control over selection rules in light–matter interactions.

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.

Characterizing an Optically Induced Sub-micrometer Gigahertz Acoustic Wave in a Silicon Thin Plate.

Optically induced GHz-THz guided acoustic waves have been intensively studied because of the potential to realize noninvasive and noncontact material inspection. Although the generation of photoinduced guided acoustic waves utilizing nanostructures, such as ultrathin plates, nanowires, and materials interfaces, is being established, experimental characterization of these acoustic waves in consideration of the finite size effect has been difficult due to the lack of experimental methods with nm × ps resolution. Here we experimentally observe the sub-micrometer guided acoustic waves in a nanofabricated ultrathin silicon plate by ultrafast transmission electron microscopy with nm × ps precision. We successfully characterize the excited guided acoustic wave in frequency-wavenumber space by applying Fourier-transformation analysis on the bright-field movie. These results suggest the great potential of ultrafast transmission electron microscopy to characterize the acoustic modes realized in various nanostructures.

Plasmonic near-field spatiotemporal characterizations of an asymmetric copper bowtie nanostructure

Photon-induced near-field electron microscopy (PINEM), developed from ultrafast transmission electron microscopy, enables near-field imaging with nanometer spatial resolution and femtosecond temporal resolution. We report the plasmonic near-field distribution and lifetime analysis for an asymmetric copper bowtie nanostructure having unequal opening angles. The PINEM images show surface plasmon polaritons and local surface-plasmon resonance excitations with various polarizations. Combined with finite-element simulations, the polarization- and structure-dependent distribution and intensity variations of the near-field were analyzed. The lifetime difference of a plasmonic near-field excited by different polarizations is also discussed. The temporal and spatial characterization of the plasmonic near-field is important for the further studies of plasmonic near-field manipulation and designs of plasmonic devices having specific functions.

Femtosecond tunable-wavelength photoassisted cold field emission

We demonstrate photoassisted cold field emission (PFE) from a tungsten tip induced by tunable-wavelength low-power femtosecond laser excitation. The emission current from the apex of the (310)-oriented single-crystalline emitter is shown to linearly depend on the incident laser power, while the effective work function is reduced by the respective photon energy. Our results promote the implementation of the linear regime in laser-triggered cold field emission for ultrafast transmission electron microscopy.

Charge Dynamics Electron Microscopy: Nanoscale Imaging of Femtosecond Plasma Dynamics.

Understanding and actively controlling the spatiotemporal dynamics of nonequilibrium electron clouds is fundamental for the design of light and electron sources, high-power electronic devices, and plasma-based applications. However, electron clouds evolve in a complex collective fashion on the nanometer and femtosecond scales, producing electromagnetic screening that renders them inaccessible to existing optical probes. Here, we solve the long-standing challenge of characterizing the evolution of electron clouds generated upon irradiation of metallic structures using an ultrafast transmission electron microscope to record the charged plasma dynamics. Our approach to charge dynamics electron microscopy (CDEM) is based on the simultaneous detection of electron-beam acceleration and broadening with nanometer/femtosecond resolution. By combining experimental results with comprehensive microscopic theory, we provide a deep understanding of this highly out-of-equilibrium regime, including previously inaccessible intricate microscopic mechanisms of electron emission, screening by the metal, and collective cloud dynamics. Beyond the present specific demonstration, the here-introduced CDEM technique grants us access to a wide range of nonequilibrium electrodynamic phenomena involving the ultrafast evolution of bound and free charges on the nanoscale.

Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors.

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such nonequilibrium phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatiotemporal scales at which the charge carriers evolve. Here, we propose and demonstrate an interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction of free-electron pulses with terahertz (THz) near fields produced by the moving charges in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatiotemporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison to microscopic theory. The CDEM technique thus allows us to investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids, providing insight into the photo-Dember effect and showing oscillations of photogenerated electron-hole distributions inside a semiconductor. Our work facilitates the exploration of a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

Nanoscale subparticle imaging of vibrational dynamics using dark-field ultrafast transmission electron microscopy

An understanding of nanoscale energy transport and acoustic response is important for applications of nanomaterials but hinges on a complete characterization of their structural dynamics. The precise determination of the structural dynamics within nanoparticles, however, is still challenging and requires high spatiotemporal resolution and detection sensitivity. Here we present a centred dark-field imaging approach based on ultrafast transmission electron microscopy that is capable of directly mapping the picosecond-scale evolution of intrananoparticle vibration with a spatial resolution down to 3 nm. Using this approach, we investigated the photo-induced vibrational dynamics in individual gold heterodimers composed of a nanoprism and a nanosphere. We observed not only the retardation of in-plane vibrations in the nanoprisms, which we attribute to thermal and vibrational energy transferred from adjacent nanospheres mediated by surfactants, but also the existence of a complex multimodal oscillation and its spatial variation within individual nanoprisms. This work represents an advance in real-space mapping of vibrational dynamics on the subnanoparticle level with a high detection sensitivity.

Accurate time zero determination in an ultrafast transmission electron microscope without energy filter

In ultrafast transmission electron microscopy, time zero can be accurately determined by making use of the photon-induced near-field electron microscopy (PINEM) effect, which causes electrons interacting with the near fields of a nanoparticle to coherently gain or lose energy in multiples of the photon energy when the laser pump and electron probe pulse overlap in time. If the instrument is not equipped with an energy filter, which is required to observe the PINEM effect, the response of a sample is frequently monitored instead. However, the gradual or delayed onset of this response can render an accurate measurement as challenging. Here, we demonstrate a simple and accurate method for determining time zero without an energy filter that is based on the observation that the outline of a nanoparticle blurs when the electron and laser pulse overlap in time. We show that this phenomenon arises from the PINEM effect, which causes some electrons to gain a large energy spread, thus blurring the image due to the chromatic aberration of the imaging system. This effect can also be used to characterize the instrument response and determine the laser polarization in situ. Furthermore, it may find applications for mapping out the near fields of a nanoparticle without the help of an energy filter.

Enhancement of lattice dynamics by an azimuthal surface plasmon on the femtosecond time scale in multi-walled carbon nanotubes.

Plasmon-enhanced light-matter interactions have been widely investigated in the past decades. Here, we report surface plasmon-enhanced structural dynamics in multi-walled carbon nanotubes. The optical polarization dependent dynamic properties of multi-walled carbon nanotubes are investigated using ultrafast transmission electron microscopy. Lattice contractions in the femtosecond time regime are observed upon excitation of the azimuthal plasmon by light polarized perpendicular to the tubular axis. The polarization dependence of the plasmon near field was examined using photon-induced near-field electron microscopy. The lattice changes resulting from the azimuthal plasmon enhance ultrafast alterations in both localized evanescent fields and the collective charge excitation, which play critical roles governing the light-matter interaction. These results suggest that the ultrafast responses of lattice degrees of freedom in nanomaterials could be essential for understanding the mechanism of surface plasmon enhanced effects.

Quantifying the Local Structure of Nanocrystals, Glasses, and Interfaces Using TEM-Based Diffraction

Although order is a defining characteristic of crystals, disordered structures─especially near interfaces─often govern a material’s performance. For example, the interfaces in batteries, coatings, or catalysts exemplify systems in which disorder plays a critical role. Despite this importance, characterization of local structure in disordered materials remains a challenge. To solve this challenge, the electron pair distribution function (ePDF) method has given insight into the local structure of many complex samples because the technique can be applied to disordered materials containing as few as tens or hundreds of atoms. The ePDF method takes a transmission electron microscope (TEM) diffraction pattern and transforms this into information about the bond lengths present in a material. This information can then be used to create a 3D, atomic-scale model of local chemical structure. In this review, we introduce the theory behind ePDF, describe common methods for data acquisition, and highlight recent advances in the ePDF technique, including its combination with cryo-electron microscopy, ultrafast TEM, and precession electron diffraction. We also show how ePDF has been applied to important classes of materials, including 2D heterostructures, nanoscale interfaces, and materials fabricated by atomic layer deposition. Finally, we review how ePDF can be combined with other techniques to provide a comprehensive understanding of a material. Because ePDF can be performed on most TEMs, it is beginning to emerge as a routine method for the analysis of complex, disordered structures in technologically important 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.

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.

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.

Catching them in Action: Ultrafast Transmission Electron Microscopy

Catching them in Action: Ultrafast Transmission Electron Microscopy