A review of understanding electrocatalytic reactions in energy conversion and energy storage systems via scanning electrochemical microscopy

To address climate change and promote environmental sustainability,electrochemical energy conversion and storage systems emerge as promising alternative to fossil fuels,catering to the escalating demand for energy.Achieving optimal energy efficiency and cost competitiveness in these systems requires the strategic design of electrocatalysts,coupled with a thorough comprehension of the underlying mechanisms and degradation behavior occurring during the electrocatalysis processes.Scanning electrochemical microscopy(SECM),an analytical technique for studying surface electrochemically,stands out as a powerful tool offering electrochemical insights.It possesses remarkable spatiotemporal resolution,enabling the visualization of the localized electrochemical activity and surface topography.This review compiles crucial research findings and recent breakthroughs in electrocatalytic processes utilizing the SECM methodology,specifically focusing on applications in electrolysis,fuel cells,and metal–oxygen batteries within the realm of energy conversion and storage systems.Commencing with an overview of each energy system,the review introduces the fundamental principles of SECM,and aiming to provide new perspectives and broadening the scope of applied research by describing the major research categories within SECM.

From static to dynamic:live observation of the support system after ischemic stroke by two photon-excited fluorescence laser-scanning microscopy

Ischemic stroke is one of the most common causes of mortality and disability worldwide.However,treatment efficacy and the progress of research remain unsatisfactory.As the critical support system and essential components in neurovascular units,glial cells and blood vessels(including the bloodbrain barrier)together maintain an optimal microenvironment for neuronal function.They provide nutrients,regulate neuronal excitability,and prevent harmful substances from entering brain tissue.The highly dynamic networks of this support system play an essential role in ischemic stroke through processes including brain homeostasis,supporting neuronal function,and reacting to injuries.However,most studies have focused on postmortem animals,which inevitably lack critical information about the dynamic changes that occur after ischemic stroke.Therefore,a high-precision technique for research in living animals is urgently needed.Two-photon fluorescence laser-scanning microscopy is a powerful imaging technique that can facilitate live imaging at high spatiotemporal resolutions.Twophoton fluorescence laser-scanning microscopy can provide images of the whole-cortex vascular 3D structure,information on multicellular component interactions,and provide images of structure and function in the cranial window.This technique shifts the existing research paradigm from static to dynamic,from flat to stereoscopic,and from single-cell function to multicellular intercommunication,thus providing direct and reliable evidence to identify the pathophysiological mechanisms following ischemic stroke in an intact brain.In this review,we discuss exciting findings from research on the support system after ischemic stroke using two-photon fluorescence laser-scanning microscopy,highlighting the importance of dynamic observations of cellular behavior and interactions in the networks of the brain’s support systems.We show the excellent application prospects and advantages of two-photon fluorescence laser-scanning microscopy and predict future research developments and directions in the study of ischemic stroke.

Single-cell volumetric imaging with light field microscopy: Advances in systems and algorithms

Single-cell volumetric imaging is essential for researching individual characteristics of cells.As a nonscanning imaging technique,lighteld microscopy(LFM)is a critical tool to achieve realtime three-dimensional imaging with the advantage of single-shot.To address the inherent limits including nonuniform resolution and block-wise artifacts,various modied LFM strategies have been developed to provide new insights into the structural and functional information of cells.This review will introduce the principle and development of LFM,discuss the improved approaches based on hardware designs and 3D reconstruction algorithms,and present the applications in single-cell imaging.

Myelin histology:a key tool in nervous system research

The myelin sheath is a lipoprotein-rich,multilayered structure capable of increasing conduction velocity in central and peripheral myelinated nerve fibers.Due to the complex structure and composition of myelin,various histological techniques have been developed over the centuries to evaluate myelin under normal,pathological or experimental conditions.Today,methods to assess myelin integrity or content are key tools in both clinical diagnosis and neuroscience research.In this review,we provide an updated summary of the composition and structure of the myelin sheath and discuss some histological procedures,from tissue fixation and processing techniques to the most used and practical myelin histological staining methods.Considering the lipoprotein nature of myelin,the main features and technical details of the different available methods that can be used to evaluate the lipid or protein components of myelin are described,as well as the precise ultrastructural techniques.

Investigation of reflection anisotropy induced by micropipe defects on the surface of a 4H-SiC single crystal using scanning anisotropy microscopy

Optical reflection anisotropy microscopy mappings of micropipe defects on the surface of a 4H-SiC single crystal are studied by the scanning anisotropy microscopy(SAM)system.The reflection anisotropy(RA)image with a'butterfly pattern'is obtained around the micropipes by SAM.The RA image of the edge dislocations is theoretically simulated based on dislocation theory and the photoelastic principle.By comparing with the Raman spectrum,it is verified that the micropipes consist of edge dislocations.The different patterns of the RA images are due to the different orientations of the Burgers vectors.Besides,the strain distribution of the micropipes is also deduced.One can identify the dislocation type,the direction of the Burgers vector and the optical anisotropy from the RA image by using SAM.Therefore,SAM is an ideal tool to measure the optical anisotropy induced by the strain field around a defect.

Correlation of work function and stacking fault energy through Kelvin probe force microscopy and nanohardness in diluteα-magnesium

Electronic interactions of the Group 2A elements with magnesium have been studied through the dilute solid solutions in binary Mg-Ca,Mg-Sr and Mg-Ba systems.This investigation incorporated the difference in the‘Work Function'(ΔWF)measured via Kelvin Probe Force Microscopy(KPFM),as a property directly affected by interatomic bond types,i.e.the electronic structure,nanoindentation measurements,and Stacking Fault Energy values reported in the literature.It was shown that the nano-hardness of the solid-solutionα-Mg phase changed in the order of Mg-Ca>Mg-Sr>Mg-Ba.Thus,it was shown,by also considering the nano-hardness levels,that SFE of a solid-solution is closely correlated with its‘Work Function'level.Nano-hardness measurements on the eutectics andΔWF difference between eutectic phases enabled an assessment of the relative bond strength and the pertinent electronic structures of the eutectics in the three alloys.Correlation withΔWF and at least qualitative verification of those computed SFE values with some experimental measurement techniques were considered important as those computational methods are based on zero Kelvin degree,relatively simple atomic models and a number of assumptions.As asserted by this investigation,if the results of measurement techniques can be qualitatively correlated with those of the computational methods,it can be possible to evaluate the electronic structures in alloys,starting from binary systems,going to ternary and then multi-elemental systems.Our investigation has shown that such a qualitative correlation is possible.After all,the SFE values are not treated as absolute values but rather become essential in comparative investigations when assessing the influences of alloying elements at a fundamental level,that is,free electron density distributions.Our study indicated that the principles of‘electronic metallurgy'in developing multi-elemental alloy systems can be followed via practical experimental methods,i.e.ΔWF measurements using KPFM and nanoindentation.

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.

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.

Estimation-free spatial-domain image reconstruction of structured illumination microscopy

Structured illumination microscopy(SIM)achieves super-resolution(SR)by modulating the high-frequency information of the sample into the passband of the optical system and subsequent image reconstruction.The traditional Wiener-filtering-based reconstruction algorithm operates in the Fourier domain,it requires prior knowledge of the sinusoidal illumination patterns which makes the time-consuming procedure of parameter estimation to raw datasets necessary,besides,the parameter estimation is sensitive to noise or aberration-induced pattern distortion which leads to reconstruction artifacts.Here,we propose a spatial-domain image reconstruction method that does not require parameter estimation but calculates patterns from raw datasets,and a reconstructed image can be obtained just by calculating the spatial covariance of differential calculated patterns and differential filtered datasets(the notch filtering operation is performed to the raw datasets for attenuating and compensating the optical transfer function(OTF)).Experiments on reconstructing raw datasets including nonbiological,biological,and simulated samples demonstrate that our method has SR capability,high reconstruction speed,and high robustness to aberration and noise.

Spatial weight matrix in dimensionality reduction reconstruction for microelectromechanical system-based photoacoustic microscopy

A micro-electromechanical system(MEMS)scanning mirror accelerates the raster scanning of optical-resolution photoacoustic microscopy(OR-PAM).However,the nonlinear tilt angular-voltage characteristic of a MEMS mirror introduces distortion into the maximum back-projection image.Moreover,the size of the airy disk,ultrasonic sensor properties,and thermal effects decrease the resolution.Thus,in this study,we proposed a spatial weight matrix(SWM)with a dimensionality reduction for image reconstruction.The three-layer SWM contains the invariable information of the system,which includes a spatial dependent distortion correction and 3D deconvolution.We employed an ordinal-valued Markov random field and the Harris Stephen algorithm,as well as a modified delay-and-sum method during a time reversal.The results from the experiments and a quantitative analysis demonstrate that images can be effectively reconstructed using an SWM;this is also true for severely distorted images.The index of the mutual information between the reference images and registered images was 70.33 times higher than the initial index,on average.Moreover,the peak signal-to-noise ratio was increased by 17.08%after 3D deconvolution.This accomplishment offers a practical approach to image reconstruction and a promising method to achieve a real-time distortion correction for MEMS-based OR-PAM.

Reperfusion after hypoxia-ischemia exacerbates brain injury with compensatory activation of the antiferroptosis system:based on a novel rat model

Hypoxic-ischemic encephalopathy,which predisposes to neonatal death and neurological sequelae,has a high morbidity,but there is still a lack of effective prevention and treatment in clinical practice.To better understand the pathophysiological mechanism underlying hypoxic-ischemic encephalopathy,in this study we compared hypoxic-ischemic reperfusion brain injury and simple hypoxic-ischemic brain injury in neonatal rats.First,based on the conventional RiceVannucci model of hypoxic-ischemic encephalopathy,we established a rat model of hypoxic-ischemic reperfusion brain injury by creating a common carotid artery muscle bridge.Then we performed tandem mass tag-based proteomic analysis to identify differentially expressed proteins between the hypoxic-ischemic reperfusion brain injury model and the conventional Rice-Vannucci model and found that the majority were mitochondrial proteins.We also performed transmission electron microscopy and found typical characteristics of ferroptosis,including mitochondrial shrinkage,ruptured mitochondrial membranes,and reduced or absent mitochondrial cristae.Further,both rat models showed high levels of glial fibrillary acidic protein and low levels of myelin basic protein,which are biological indicators of hypoxic-ischemic brain injury and indicate similar degrees of damage.Finally,we found that ferroptosis-related Ferritin(Fth1)and glutathione peroxidase 4 were expressed at higher levels in the brain tissue of rats with hypoxic-ischemic reperfusion brain injury than in rats with simple hypoxic-ischemic brain injury.Based on these results,it appears that the rat model of hypoxic-ischemic reperfusion brain injury is more closely related to the pathophysiology of clinical reperfusion.Reperfusion not only aggravates hypoxic-ischemic brain injury but also activates the anti-ferroptosis system.

Atomic Force Microscopy Measurement in the Lignosulfonate/Inorganic Silica System:From Dispersion Mechanism Study to Product Design

Designing and preparing high-performance lignin-based dispersants are crucial steps in realizing the value-added utilization of lignin on an industrial scale.Such process depends heavily on an understanding of the dispersion mechanism of lignin-based dispersants.Here,atomic force microscopy(AFM)is employed to quantitatively investigate the dispersion mechanism of a lignosulfonate/silica(LS/SiO_(2))system under different pH conditions.The results show that the repulsive force between SiO_(2)particles in LS solution is stronger than it is in water,resulting in better dispersion stability.The Derjaguin–Landau–Verwey–Overbeek(DLVO)formula as well as the DLVO formula combined with steric repulsion is utilized for the fitting of the AFM force/distance(F/D)curves between the SiO_(2)probe and substrate in water and in LS solution.Based on these fitting results,electrostatic and steric repulsive forces are respectively calculated,yielding further evidence that LS provides strong steric repulsion between SiO_(2)particles.Further studies indicate that the adsorbance of LS on SiO_(2)(Q),the normalized interaction constant(A),and the characteristic length(L)are the three critical factors affecting steric repulsion in the LS/SiO_(2)system.Based on the above conclusions,a novel quaternized grafted-sulfonation lignin(QAGSL)dispersant is designed and prepared.The QAGSL dispersant exhibits good dispersing performance for SiO_(2)and real cement particles.This work provides a fundamental and quantitative understanding of the dispersion mechanism in the LS/inorganic particle system and provides important guidance for the development of high-performance lignin-based dispersants.

High-speed all-optic optical coherence tomography and photoacoustic microscopy dual-modal system for microcirculation evaluation

We propose a high-speed all-optic dual-modal system that integrates spectral domain optical coherence tomography and photoacoustic microscopy(PAM).A 3*3 coupler-based interfer-ometer is used to remotely detect the surface vibration caused by photoacoustic(PA)waves.Three outputs of the interferometer are acquired simultaneously with a multi-channel data ac-quisition card.One channel data with the highest PA signal detection sensitivity is selected for sensitivity compensation.Experiment on the phantom demonstrates that the proposed method can sucessfully compensate for the loss of intensity caused by sensitivity variation.The imaging speed of the PAM is improved compared to our previous system.The total time to image a sample with 256×256 pixels is~20s.Using the proposed system,the microvasculature in the mouse auricle is visualized and the blood flow state is accessed.

Probing the Majorana bound states in a hybrid nanowire double-quantum-dot system by scanning tunneling microscopy

We propose an interferometer composing of a scanning tunneling microscope(STM),double quantum dots(DQDs),and a semiconductor nanowire carrying Majorana bound states(MBSs)at its ends induced by the proximity effect of an s-wave superconductor,to probe the existence of the MBSs in the dots.Our results show that when the energy levels of DQDs are aligned to the energy of MBSs,the zero-energy spectral functions of DQDs are always equal to 1/2,which indicates the formation of the MBSs in the DQDs and is also responsible for the zero-bias conductance peak.Our findings suggest that the spectral functions of the DQDs may be an excellent and convenient quantity for detecting the formation and stability of the spatially separated MBSs in quantum dots.

Nonlinear optical microscopy for skin in vivo:Basics,development and applications

Multi-photon microscopy(MPM)and coherent anti-Stokes Raman scattering(CARS)are two advanced nonlinear optical imaging techniques,which provide complementary information and have great potential in combination for noninvasive in vrito biomedical applications.This paper provides a detailed discussion of the basics,development and applications of these technologies for in vrivo skin research,covering the following topics:The principle and advantage of MPM and CARS,instrumentation development for in vino applications,MPM and CARS of normal skin,application of MPM and CARS in skin cancer and disease diagnosis;application of MPM in skin disease intervention,ie.,imaging guided two-photon photothermolysis.

Classification of Human Protein in Multiple Cells Microscopy Images Using CNN

The subcellular localization of human proteins is vital for understanding the structure of human cells.Proteins play a significant role within human cells,as many different groups of proteins are located in a specific location to perform a particular function.Understanding these functions will help in discoveringmany diseases and developing their treatments.The importance of imaging analysis techniques,specifically in proteomics research,is becoming more prevalent.Despite recent advances in deep learning techniques for analyzing microscopy images,classification models have faced critical challenges in achieving high performance.Most protein subcellular images have a significant class imbalance.We use oversampling and under sampling techniques in this research to overcome this issue.We have used a Convolutional Neural Network(CNN)model called GapNet-PL for the multi-label classification task on the Human Protein Atlas Classification(HPA)Dataset.Authors have found that the ParametricRectified LinearUnit(PreLU)activation function is better than the Scaled Exponential LinearUnit(SeLU)activation function in the GapNet-PL model in most classification metrics.The results showed that the GapNet-PL model with the PReLU activation function achieved an area under the ROC curve(AUC)equal to 0.896,an F1 score of 0.541,and a recall of 0.473.

Correlating the Interfacial Polar-Phase Structure to the Local Chemistry in Ferroelectric Polymer Nanocomposites by Combined Scanning Probe Microscopy

Ferroelectric polymer nanocomposites possess exceptional electric properties with respect to the two otherwise uniform phases,which is commonly attributed to the critical role of the matrix-particle interfacial region.However,the structure-property correlation of the interface remains unestablished,and thus,the design of ferroelectric polymer nanocompos-ite has largely relied on the trial-and-error method.Here,a strategy that combines multi-mode scanning probe microscopy-based electrical charac-terization and nano-infrared spectroscopy is developed to unveil the local structure-property correlation of the interface in ferroelectric polymer nano-composites.The results show that the type of surface modifiers decorated on the nanoparticles can significantly influence the local polar-phase content and the piezoelectric effect of the polymer matrix surrounding the nano-particles.The strongly coupled polar-phase content and piezoelectric effect measured directly in the interfacial region as well as the computed bonding energy suggest that the property enhancement originates from the formation of hydrogen bond between the surface modifiers and the ferroelectric polymer.It is also directly detected that the local domain size of the ferroelectric polymer can impact the energy level and distribution of charge traps in the interfacial region and eventually influence the local dielectric strength.

Photoacoustic microscopy based on transparent piezoelectric ultrasound transducers

Photoacoustic microscopy(PAM),due to its deep penetration depth and high contrast,is playing an increasingly important role in biomedical imaging.PAM imaging systems equipped with conventional ultrasound transducers have demonstrated excellent imaging performance.However,these opaque ultrasonic transducers bring some constraints to the further development and application of PAM,such as complex optical path,bulky size,and difficult to integrate with other modalities.To overcome these problems,ultrasonic transducers with high optical transparency have appeared.At present,transparent ultrasonic transducers are divided into optical-based and acoustic-based sensors.In this paper,we mainly describe the acoustic-based piezoelectric transparent transducers in detail,of which the research advances in PAM applications are reviewed.In addition,the potential challenges and developments of transparent transducers in PAM are also demonstrated.

DecodeSTORM:A user-friendly ImageJ plug-in for quantitative data analysis in single-molecule localization microscopy

Quantitative data analysis in single-molecule localization microscopy(SMLM)is crucial for studying cellular functions at the biomolecular level.In the past decade,several quantitative methods were developed for analyzing SMLM data;however,imaging artifacts in SMLM experiments reduce the accuracy of these methods,and these methods were seldom designed as user-friendly tools.Researchers are now trying to overcome these di±culties by developing easyto-use SMLM data analysis software for certain image analysis tasks.But,this kind of software did not pay su±cient attention to the impact of imaging artifacts on the analysis accuracy,and usually contained only one type of analysis task.Therefore,users are still facing di±culties when they want to have the combined use of different types of analysis methods according to the characteristics of their data and their own needs.In this paper,we report an ImageJ plug-in called DecodeSTORM,which not only has a simple GUI for human–computer interaction,but also combines artifact correction with several quantitative analysis methods.DecodeSTORM includes format conversion,channel registration,artifact correction(drift correction and localization¯ltering),quantitative analysis(segmentation and clustering,spatial distribution statistics and colocalization)and visualization.Importantly,these data analysis methods can be combined freely,thus improving the accuracy of quantitative analysis and allowing users to have an optimal combination of methods.We believe DecodeSTORM is a user-friendly and powerful ImageJ plug-in,which provides an easy and accurate data analysis tool for adventurous biologists who are looking for new imaging tools for studying important questions in cell biology.

Quantitative measurement of the charge carrier concentration using dielectric force microscopy

The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carrier concentrations with nanometer-scale spatial resolution.However,it is challenging to quantitatively obtain the charge carrier concentration,since the dielectric force is also affected by the mobility.Here,we quantitative measured the charge carrier concentration at the saturation mobility regime via the rectification effect-dependent gating ratio of DFM.By measuring a series of n-type GaAs and GaN thin films with mobility in the saturation regime,we confirmed the decreased DFM-measured gating ratio with increasing electron concentration.Combined with numerical simulation to calibrate the tip–sample geometry-induced systematic error,the quantitative correlation between the DFM-measured gating ratio and the electron concentration has been established,where the extracted electron concentration presents high accuracy in the range of 4×10^(16)–1×10^(18)cm^(-3).We expect the quantitative DFM to find broad applications in characterizing the charge carrier transport properties of various semiconducting materials and devices.