Ultrafast photoemission electron microscopy:A multidimensional probe of nonequilibrium physics

Exploring the realms of physics that extend beyond thermal equilibrium has emerged as a crucial branch of condensed matter physics research.It aims to unravel the intricate processes involving the excitations,interactions,and annihilations of quasi-and many-body particles,and ultimately to achieve the manipulation and engineering of exotic non-equilibrium quantum phases on the ultrasmall and ultrafast spatiotemporal scales.Given the inherent complexities arising from many-body dynamics,it therefore seeks a technique that has efficient and diverse detection degrees of freedom to study the underlying physics.By combining high-power femtosecond lasers with real-or momentum-space photoemission electron microscopy(PEEM),imaging excited state phenomena from multiple perspectives,including time,real space,energy,momentum,and spin,can be conveniently achieved,making it a unique technique in studying physics out of equilibrium.In this context,we overview the working principle and technical advances of the PEEM apparatus and the related laser systems,and survey key excited-state phenomena probed through this surface-sensitive methodology,including the ultrafast dynamics of electrons,excitons,plasmons,spins,etc.,in materials ranging from bulk and nano-structured metals and semiconductors to low-dimensional quantum materials.Through this review,one can further envision that time-resolved PEEM will open new avenues for investigating a variety of classical and quantum phenomena in a multidimensional parameter space,offering unprecedented and comprehensive insights into important questions in the field of condensed matter physics.

Characterization of local chemical ordering and deformation behavior in high entropy alloys by transmission electron microscopy

Short-range ordering(SRO)is one of the most important structural features of high entropy alloys(HEAs).However,the chemical and structural analyses of SROs are very difficult due to their small size,complexed compositions,and varied locations.Transmission electron microscopy(TEM)as well as its aberration correction techniques are powerful for characterizing SROs in these compositionally complex alloys.In this short communication,we summarized recent progresses regarding characterization of SROs using TEM in the field of HEAs.By using advanced TEM techniques,not only the existence of SROs was confirmed,but also the effect of SROs on the deformation mechanism was clarified.Moreover,the perspective related to application of TEM techniques in HEAs are also discussed.

Probing the Nucleation and Growth Kinetics of Bismuth Nanoparticles via In-situ Transmission Electron Microscopy

The nucleation and growth mechanism of nanoparticles is an important theory,which can guide the preparation of nanomaterials.However,it is still lacking in direct observation on the details of the evolution of intermediate state structure during nucleation and growth.In this work,the evolution process of bismuth nanoparticles induced by electron beam was revealed by in-situ transmission electron microscopy(TEM)at atomic scale.The experimental results demonstrate that the size,stable surface and crystallographic defect have important influences on the growth of Bi nanoparticles.Two non-classical growth paths including single crystal growth and polycrystalline combined growth,as well as,corresponding layer-by-layer growth mechanism along{012}stable crystal plane of Bi nanoparticles with dodecahedron structure were revealed by in-situ TEM directly.These results provide important guidance and a new approach for in-depth understanding of the nucleation and growth kinetics of nanoparticles.

Revealing the microstructures of metal halide perovskite thin films via advancedtransmission electron microscopy

Metal halide perovskites (MHPs) are excellent semiconductors that have led to breakthroughs in applications in thinfilmsolar cells, detectors, and light-emitting diodes due to their remarkable optoelectronic properties and defect tolerance.However, the performance and stability of MHP-based devices are significantly influenced by their microstructures includingthe formation of defects, composition fluctuations, structural inhomogeneity, etc. Transmission electron microscopy(TEM) is a powerful tool for direct observation of microstructure at the atomic-scale resolution and has been used to correlatethe microstructure and performance of MHP-based devices. In this review, we highlight the application of TEMtechniques in revealing the microstructures of MHP thin films at the atomic scale. The results provide critical understandingof the performance of MHP devices and guide the design of strategies for improving the performance and stability ofMHP devices.

Recent progress about transmission electron microscopy characterizations on lithium-ion batteries

With the rapid development of portable electronics,new energy vehicles,and smart grids,ion batteries are becoming one of the most widely used energy storage devices,while the safety concern of ion batteries has always been an urgent problem to be solved.To develop a safety-guaranteed battery,the characterization of the internal structure is indispensable,where electron microscopy plays a crucial role.Based on this,this paper summarizes the application of transmission electron microscopy(TEM)in battery safety,further concludes and analyzes the aspects of dendrite growth and solid electrolyte interface(SEI)formation that affect the safety of ion batteries,and emphasizes the importance of electron microscopy in battery safety research and the potential of these techniques to promote the future development of this field.These advanced electron microscopy techniques and their prospects are also discussed.

A review of in situ transmission electron microscopy study on the switching mechanism and packaging reliability in non-volatile memory

Non-volatile memory(NVM)devices with non-volatility and low power consumption properties are important in the data storage field.The switching mechanism and packaging reliability issues in NVMs are of great research interest.The switching process in NVM devices accompanied by the evolution of microstructure and composition is fast and subtle.Transmission electron microscopy(TEM)with high spatial resolution and versatile external fields is widely used in analyzing the evolution of morphology,structures and chemical compositions at atomic scale.The various external stimuli,such as thermal,electrical,mechanical,optical and magnetic fields,provide a platform to probe and engineer NVM devices inside TEM in real-time.Such advanced technologies make it possible for an in situ and interactive manipulation of NVM devices without sacrificing the resolution.This technology facilitates the exploration of the intrinsic structure-switching mechanism of NVMs and the reliability issues in the memory package.In this review,the evolution of the functional layers in NVM devices characterized by the advanced in situ TEM technology is introduced,with intermetallic compounds forming and degradation process investigated.The principles and challenges of TEM technology on NVM device study are also discussed.

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 photoinduced 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.

Recent progress on advanced transmission electron microscopy characterization for halide perovskite semiconductors

Halide perovskites are strategically important in the field of energy materials. Along with the rapid development of the materials and related devices, there is an urgent need to understand the structure–property relationship from nanoscale to atomic scale. Much effort has been made in the past few years to overcome the difficulty of imaging limited by electron dose,and to further extend the investigation towards operando conditions. This review is dedicated to recent studies of advanced transmission electron microscopy(TEM) characterizations for halide perovskites. The irradiation damage caused by the interaction of electron beams and perovskites under conventional imaging conditions are first summarized and discussed. Low-dose TEM is then discussed, including electron diffraction and emerging techniques for high-resolution TEM(HRTEM) imaging. Atomic-resolution imaging, defects identification and chemical mapping on halide perovskites are reviewed. Cryo-TEM for halide perovskites is discussed, since it can readily suppress irradiation damage and has been rapidly developed in the past few years. Finally, the applications of in-situ TEM in the degradation study of perovskites under environmental conditions such as heating,biasing, light illumination and humidity are reviewed. More applications of emerging TEM characterizations are foreseen in the coming future, unveiling the structural origin of halide perovskite’s unique properties and degradation mechanism under operando conditions, so to assist the design of a more efficient and robust energy material.

Femtosecond Time-Resolved Spectroscopic Photoemission Electron Microscopy for Probing Ultrafast Carrier Dynamics in Heterojunctions

The fast developing semiconductor industry is pushing to shrink and speed up transistors. This trend requires us to understand carrier dynamics in semiconductor heterojunctions with both high spatial and temporal resolutions. Recently, we have successfully set up a timeresolved photoemission electron microscopy (TR-PEEM), which integrates the spectroscopic technique to measure electron densities at specific energy levels in space. This instrument provides us an unprecedented access to the evolution of electrons in terms of spatial location, time resolution, and energy, representing a new type of 4D spectro-microscopy. Here in this work, we present measurements of semiconductor performance with a time resolution of 184 fs, electron kinetic energy resolution of 150 meV, and spatial resolution of about 150 nm or better. We obtained time-resolved micro-area photoelectron spectra and energy-resolved TR-PEEM images on the Pb island on Si(111). These experimental results suggest that this instrument has the potential to be a powerful tool for investigating the carrier dynamics in various heterojunctions, which will deepen our understanding of semiconductor properties in the submicron/nanometer spatial scales and ultrafast time scales.

In situ observation of the electrochemical behavior of Li–CO_(2)/O_(2)batteries in an environmental transmission electron microscope

Li–CO_(2)/O_(2)batteries,a promising energy storage technology,not only provide ultrahigh discharge capacity but also capture CO_(2)and turn it into renewable energy.Their electrochemical reaction pathways'ambiguity,however,creates a hurdle for their practical application.This study used copper selenide(CuSe)nanosheets as the air cathode medium in an environmental transmission electron microscope to in situ study Li–CO_(2)/O_(2)(mix CO_(2)as well as O_(2)at a volume ratio of 1:1)and Li–O_(2)batteries as well as Li–CO_(2)batteries.Primary discharge reactions take place successively in the Li–CO_(2)/O_(2)–CuSe nanobattery:(I)4Li^(+)+O_(2)+4e^(−)→2Li_(2)O;(II)Li_(2)O+CO_(2)→Li_(2)CO_(3).The charge reaction proceeded via(III)2Li_(2)CO_(3)→4Li^(+)+2CO_(2)+O_(2)+4e^(−).However,Li–O_(2)and Li–CO_(2)nanobatteries showed poor cycling stability,suggesting the difficulty in the direct decomposition of the discharge product.The fluctuations of the Li–CO_(2)/O_(2)battery's electrochemistry were also shown to depend heavily on O_(2).The CuSe‐based Li–CO_(2)/O_(2)battery showed exceptional electrochemical performance.The Li^–CO_(2)/O_(2)battery offered a discharge capacity apex of 15,492 mAh g^(−1) and stable cycling 60 times at 100 mA g^(−1).Our research offers crucial insight into the electrochemical behavior of Li–CO_(2)/O_(2),Li–O_(2),and Li–CO_(2)nanobatteries,which may help the creation of high‐performance Li–CO_(2)/O_(2)batteries for energy storage applications.

Movement of Dislocations in the Sub-Surface of a Polycrystalline Metal by Cavitation Peening Observed by Transmission Electron Microscopy

The impact produced when cavitation bubbles collapse can be utilized to modify surfaces in the same way as shot peening and it is called cavitation peening (CP). CP is one of a number of surface modification techniques used to improve the fatigue strength of metallic materials by introducing compressive residual stress. Although it has been shown by an X-ray diffraction method that CP decreases the micro-strain related to dislocations in the sub-surface of a polycrystalline material, the mechanism for this decrease is unclear. In this paper, the movement of dislocations by CP was observed using transmission electron microscopy (TEM).

Heterogeneity of mature oligodendrocytes in the central nervous system

Mature oligodendrocytes form myelin sheaths that are crucial for the insulation of axons and efficient signal transmission in the central nervous system.Recent evidence has challenged the classical view of the functionally static mature oligodendrocyte and revealed a gamut of dynamic functions such as the ability to modulate neuronal circuitry and provide metabolic support to axons.Despite the recognition of potential heterogeneity in mature oligodendrocyte function,a comprehensive summary of mature oligodendrocyte diversity is lacking.We delve into early 20th-century studies by Robertson and Río-Hortega that laid the foundation for the modern identification of regional and morphological heterogeneity in mature oligodendrocytes.Indeed,recent morphologic and functional studies call into question the long-assumed homogeneity of mature oligodendrocyte function through the identification of distinct subtypes with varying myelination preferences.Furthermore,modern molecular investigations,employing techniques such as single cell/nucleus RNA sequencing,consistently unveil at least six mature oligodendrocyte subpopulations in the human central nervous system that are highly transcriptomically diverse and vary with central nervous system region.Age and disease related mature oligodendrocyte variation denotes the impact of pathological conditions such as multiple sclerosis,Alzheimer's disease,and psychiatric disorders.Nevertheless,caution is warranted when subclassifying mature oligodendrocytes because of the simplification needed to make conclusions about cell identity from temporally confined investigations.Future studies leveraging advanced techniques like spatial transcriptomics and single-cell proteomics promise a more nuanced understanding of mature oligodendrocyte heterogeneity.Such research avenues that precisely evaluate mature oligodendrocyte heterogeneity with care to understand the mitigating influence of species,sex,central nervous system region,age,and disease,hold promise for the development of therapeutic interventions targeting varied central nervous system pathology.

Scanning Electron Acoustic Microscopy of GaInAsSb by Metalorganic Chemical Vapor Deposition

Scanning electron acoustic microscopy (SEAM) is a new technique for imasing and characterization ofthermal, elastic and pyroelectric property variations on a microscale resolution. The signal generation mechanisms and the application of scanning electron acoustic microscopy in GalnAsSb alloy grown by MOCVD wereinvestigated. Defects below the surface of GalnAsSb alloy were found by SEAM images and cathodelumi-nescence. The results show that electronacoustic imaging has its own features over secondary electron imag-ing.

Transmission Electron Microscopy Investigation of the Ar^+ Ion Irradiation Effect in Semiconductor GaAs

Room temperature irradiation effect of GaAs compound semiconductor by 100 keV Ar+ ions has been systematically studied by means of transmission electron microscopy. The dose dependenceoof the Ar+ ion irradiation and room temperature annealing effects have been investigated. The experimental results show that the structure of GaAs transforms from perfect crystalline through weakly and severely damaged crystalline to amorphous states with the increase of the irradiation dose and the damaged states are changed during room temperature annealing.

Scanning Electron Microscopy(SEM) Observations of Antennal Sensilla of Chrysopa pallens Rambur(Neuroptera：Chrysopidae)

[Objectives]The paper was to provide background information for ongoing research on relationship between smell and behavior of the green lacewing Chrysopa pallens（ Rambur）（ Neuroptera： Chrysopidae）. [Methods]The submicroscopic structure of antennal sensilla of C. pallens was examined using scanning electron microscopy. [Results]Antennae of female and male C. pallens were linear in shape and（ 1. 52 ± 0. 08） and（ 1. 58 ± 0. 23） cm in length,respectively. The scape and pedicel were composed of single sub-segment,while the flagellum consisted of 116 sub-segments,on which most sensilla distributed. The flagella of female and male antennae were（ 1. 44 ± 0. 04） and（ 1. 47 ± 0. 13） cm in length,respectively. Nine morphological sensilla types were recorded in both sexes,including four types of highly abundant and widely distributed sensilla trichodea（ ST Ⅰ,ST Ⅱ,ST Ⅲ and ST Ⅳ）,three types of sensilla basiconica（ SB Ⅰ,SB Ⅱ,and SB Ⅲ）,and one of each type of sensilla chaetica and B9 hm bristles. Although the shape,structure,numbers,and distribution of antennae of females and males were basically similar,major differences were recorded between the sexes in the length of some sensilla types. Both the ST Ⅲ and SB Ⅰ in female adults were significantly longer than that in male ones. Notably,SB Ⅱ was found only in female. [Conclusions]The paper laid a foundation for revealing the relationship between smell and behavior,playing a crucial role in promoting the important biological control effect of C. pallens in farmland ecological system.

CONTAMINATION LINE METHOD AND COMPARISON OF FOIL THICKNESS MEASUREMENT METHODS IN TRANSMISSION ELECTRON MICROSCOPY

The paper briefly introduces the Contamination Line Method for foil thickness measurement in transmission electron microscopy and compares it with four conventional methods: the convergent beam diffraction method, the contamination spot method, the methods hased on characteristic X-ray emission and continuous X-ray emission on the application, aperation and accuracy etc.

Ultrastructural Analysis of the Ontogenetic Development of Shoot Induced from Embryonic Axes of Costa Rican Bean Varieties (<i>Phaseolus vulgaris</i>L.) under <i>in Vitro</i>Conditions by Scanning Electronic Microscopy

Common bean (Phaseolus vulgaris L.) is an economic important crop and one of the major grain legumes for human consumption in Latin America, Africa and Asia. A morphological study of shoot induced from embryonic axes development in four Costa Rican bean varieties (Brunca, Huetar, Guaymi and Bribri) cultivated on MS media with or without 5 mg·L–1 de N6-benzylaminopurine (BAP) by scanning electron microscopy (SEM) was developed in the present work. Micrographs showed similarities and differences in the ultrastructure of the apical dome, epidermal surface, stomata and different types of trichomes in the varieties cultivated on organogenesis media. Genotypes with advantageous morphological characteristics for genetic transformation, in particular an exposed apical dome, were identified. This work will contribute to the optimization of the in vitro regeneration of four common bean varieties.

MORPHOLOGICAL CHANGES OF RATS MUSCLES AT VARIOUS POSTMORTEM INTERVALS BY SCANNING ELECTRON MICROSCOPY

The aim of this study was to observe the morphological changes of muscle in the process of rigor mortis. The quadriceps of 40 rats at various postmortem intervals were observed under the scanning electron microscope(SEM) and the light microscope by phosphotungstic acid haematoxylin(PTAH) stain. The results showed that the striations of muscle were blurred within 4 h, but they became apparent from 6 h to 24 h after death. The authors suggest that this phenomenon be associated with the increased resistance of muscle against the postmortal changes. The observations by scanning electron microscopy and light microscopy have revealed that the muscles do contract in the process of rigor mortis because the distance between two Z lines shortens and the I band narrows, compared with those in anaesthetised animals. The basic biochemical process for the formation of rigor mortis is the same as that of muscle contraction except that the former happens postmortem and the latter antemortem.

Imaging Ultrafast Plasmon Dynamics within a Complex Dolmen Nanostructure Using Photoemission Electron Microscopy

We report direct nanoscale imaging of ultrafast plasmon in a gold dolmen nanostructure excited with the 7is laser pulses by combining the interferometric time-resolved technology with the three-photon photoemission electron microscopy （PEEM）. The interferometric time-resolved traces show that the plasmon mode beating pattern appears at the ends of the dimer slabs in the dolmen nanostructure as a result of coherent superposition of multiple localized surface plasmon modes induced by broad bandwidth of the ultrafast laser pulses. The PEEM measurement further discloses that in-phase of the oscillation field of two neighbor defects are surprisingly observed, which is attributed to the plasmon coupling between them. Furthermore, the control of the temporal delay between the pump and probe laser pluses could be utilized for manipulation of the near-field distribution. These findings deepen our understanding of ultrafast plasmon dynamics in a complex nanosystem.

Improvement of femtosecond SPPs imaging by two-color laser photoemission electron microscopy

Clear imaging of surface plasmon polaritons(SPPs)is a prerequisite for SPPs-based applications.In this work,we demonstrate an improvement of near-field imaging of SPPs via directly comparing the visibility of the photoemission electron microscopy(PEEM)image of SPPs under one-and two-color laser excitation(also known as one-or two-color laser PEEM).By measuring the photoelectron yield and the contrast of the interference fringes of SPPs,we demonstrate that in addition to enhancing the photoemission yield,two-color laser PEEM can significantly improve the contrast between bright and dark fringes(nearly 4 times higher than that of one-color laser case).By recording the nonlinear order of the photoelectrons ejected from the bright and dark fringes,respectively,the underlying mechanism for the improved visibility is revealed.In addition,the influences of the polarization direction of 400-nm laser on the PEEM images of the SPPs with different wave vector directions are shown.These results can provide technical support for the development of SPPs-based communication devices and catalysis.