Electron Energy Loss Research Articles

Synergistic Active Heterostructure Design for Enhanced Two Electron Oxygen Reduction via Chemical and Electrochemical Reconstruction of Heterosulfides

AbstractTransition metal sulfides, particularly heterostructures, represent a promising class of electrocatalysts for two electron oxygen reduction (2e− ORR), however, understanding the dynamic structural evolution of these catalysts during alkaline ORR remains relatively unexplored. Herein, NiS2/In2.77S4 heterostructure was synthesized as a precatalyst and through a series of comprehensive ex situ and in situ characterizations, including X‐ray absorption spectroscopy, Raman spectroscopy, transient photo‐induced voltage measurements, electron energy loss spectroscopy, and spherical aberration‐corrected electron microscopy, it was revealed that nickel/indium (oxy)hydroxides (NiOOH/In(OH)3) could be evolved from the initial NiS2/In2.77S4 via both electrochemical and chemical‐driven methods. The electrochemical‐driven phase featured abundant bridging oxygen‐deficient [NiO6]‐[InO6] units at the interfaces of NiOOH/In(OH)3, facilitating a synergistic effect between active Ni and In sites, thus enabling an enhanced alkaline 2e− ORR capability than that of chemical‐driven process. Remarkably, electrochemically induced NiOOH/In(OH)3 exhibited exceptional performance, achieving H2O2 selectivity of >90 % across the wide potential window (up to 0.4 V) with a peak selectivity of >99 %. Notably, within the three‐electrode flow cell, a current density of 200 mA cm−2 was sustained over 20 h, together with an impressive Faradaic efficiency of ~90 % during the whole cycle process.

Synergistic Active Heterostructure Design for Enhanced Two Electron Oxygen Reduction via Chemical and Electrochemical Reconstruction of Heterosulfides.

Transition metal sulfides, particularly heterostructures, represent a promising class of electrocatalysts for two electron oxygen reduction (2e- ORR), however, understanding the dynamic structural evolution of these catalysts during alkaline ORR remains relatively unexplored. Herein, NiS2/In2.77S4 heterostructure was synthesized as a precatalyst and through a series of comprehensive ex situ and in situ characterizations, including X-ray absorption spectroscopy, Raman spectroscopy, transient photo-induced voltage measurements, electron energy loss spectroscopy, and spherical aberration-corrected electron microscopy, it was revealed that nickel/indium (oxy)hydroxides (NiOOH/In(OH)3) could be evolved from the initial NiS2/In2.77S4 via both electrochemical and chemical-driven methods. The electrochemical-driven phase featured abundant bridging oxygen-deficient [NiO6]-[InO6] units at the interfaces of NiOOH/In(OH)3, facilitating a synergistic effect between active Ni and In sites, thus enabling an enhanced alkaline 2e- ORR capability than that of chemical-driven process. Remarkably, electrochemically induced NiOOH/In(OH)3 exhibited exceptional performance, achieving H2O2 selectivity of >90 % across the wide potential window (up to 0.4 V) with a peak selectivity of >99 %. Notably, within the three-electrode flow cell, a current density of 200 mA cm-2 was sustained over 20 h, together with an impressive Faradaic efficiency of ~90 % during the whole cycle process.

Prediction of the Cu oxidation state from EELS and XAS spectra using supervised machine learning

Electron energy loss spectroscopy (EELS) and X-ray absorption spectroscopy (XAS) provide detailed information about bonding, distributions and locations of atoms, and their coordination numbers and oxidation states. However, analysis of XAS/EELS data often relies on matching an unknown experimental sample to a series of simulated or experimental standard samples. This limits analysis throughput and the ability to extract quantitative information from a sample. In this work, we have trained a random forest model capable of predicting the oxidation state of copper based on its L-edge spectrum. Our model attains an R2 score of 0.85 and a root mean square error of 0.24 on simulated data. It has also successfully predicted experimental L-edge EELS spectra taken in this work and XAS spectra extracted from the literature. We further demonstrate the utility of this model by predicting simulated and experimental spectra of mixed valence samples generated by this work. This model can be integrated into a real-time EELS/XAS analysis pipeline on mixtures of copper-containing materials of unknown composition and oxidation state. By expanding the training data, this methodology can be extended to data-driven spectral analysis of a broad range of materials.

Effects of irradiation on interfacial strength and microstructure of double-layer mullite and alumina coating on SiC

Silicon carbide (SiC) ceramics hold great potential for use in nuclear-reactor components due to characteristics such as high-temperature strength and low activation. Despite their resistance against corrosion in harsh environments, they suffer elevated corrosion rates under particle irradiation. Thin anti-corrosion coatings, such as mullite bond layers and alumina top layers, are essential to enhance the irradiation stability of SiC. The objective of this study was to evaluate the irradiation stability of a double-layer coating developed to enhance the corrosion resistance of SiC in nuclear applications. The coating, which comprised a mullite bond layer and an alumina top layer, was applied to a SiC substrate using laser chemical vapor deposition. Irradiation experiments were conducted at 300 °C with 5.1-MeV Si ions up to 10 displacements per atom. To assess the interfacial strength, a novel testing method, called the double-notch shear compression testing method, was developed based on ASTM standards and was implemented using a nanoindenter. This approach enabled precise measurements of the mechanical integrity at the interfaces of the coating under irradiation. The results showed an increase in the interfacial strength at the SiC/mullite and alumina/mullite interfaces with irradiation. Microstructural analysis of the fracture surface through scanning electron microscopy–energy-dispersive X-ray spectroscopy revealed that cracks propagated within the mullite layer, indicating the presence of mullite on the fracture surface. Transmission electron microscopy (TEM) images indicated that a 2-µm-thick transition layer existed at the SiC/mullite interface but not at the alumina/mullite interface. The TEM–electron energy loss spectroscopy suggested that the Al-O bonding structures in the transition layer were changed from tetrahedral (AlO4) to octahedral (AlO6) through irradiation, and this structural transition may directly affect the strength.

Elemental Distribution and Melting Characteristics of FeNi nanoparticles on W(110) surfaces

In this report we describe new findings on the structure, composition and thermal stability of FexNi1−x nanoparticles, synthesized via a magnetron sputtering source and deposited on a clean W(110) surface. The elemental distribution of the nanoparticles was determined by energy dispersive X-ray (EDX) and electron energy loss spectroscopy (EELS). The melting behavior of the nanoparticles was studied under UHV by scanning tunneling microscopy (STM) upon heating. Notably, it has been observed that the nanoparticle’s core is characterized by an enrichment of Ni atoms, while the shell shows a higher amount of Fe atoms. Specifically, in the case of Fe0.75Ni0.25 and Fe0.25Ni0.75, where a Ni core is surrounded by a Fe shell, all nanoparticles completely liquefy after heating at 540 K. In contrast, the Fe0.50Ni0.50 nanoparticles, which exhibit a homogeneous distribution of both elements, only begin to melt around 540 K.

Theoretical and experimental study of plasmon oscillation dispersion in Si and Ge crystals

Plasma fluctuation dispersion has been theoretically and experimentally studied in monocrystal samples of Si (111) and Ge (111). It has been shown that the dispersion depends on crystallographic orientations of materials under study. In this work, the dispersion effects in the CLEE spectra, which manifest themselves in bulk samples of Si and Ge, have been studied. The loss energy electron was studied by the CLEE method upon their reflection from Si(111) and Ge(111) at different angles of incidence of the electron beam on the surface. Calculation of the total electron energy loss with formula (5) shows that the form of the CLEE spectrum of primary electrons depends on the nature and magnitude of the electron density in a given direction and is in satisfactory agreement with the experimental data. Thus, the theoretical and experimental results show that in the case of single-crystalline Si and Ge, with increasing k, the values of the bulk plasma oscillation increase by 2–3 eV.

Study of the physical properties of the half-heusler XBrH with (X= sr, Ca and mg) compounds

Half-Heusler alloys are among the most promising thermoelectric materials for medium- and high-temperature waste heat recovery applications. This study investigates the physical properties of Half-Heusler compounds XBrH, with X = Sr, Ca, and Mg. We explored the structural, electronic, optical, and thermoelectric properties of these compounds using density functional theory (DFT) as implemented in the Wien2k package. The Generalized Gradient Approximation (GGA) as proposed by Perdew-Burke-Ernzerhof (PBE) and the modified Becke-Johnson (mBJ) functional were employed to calculate the exchange-correlation interactions. After doing structural optimization for a range of parameters, we discovered that the SrBrH compound is more stable than the CaBrH and MgBrH compounds. Our results show that the density of state calculations indicate semiconductor behavior for the XBrH with (X = Sr, Ca, and Mg) compounds. We also evaluated the real and imaginary parts of the dielectric tensor, the refractive index, the absorption coefficient, the electron energy loss, and the real and imaginary components of the optical conductivity, among other optical parameters. Additionally, we investigated the figure of merit (ZT), electronic and lattice thermal conductivity, Seebeck coefficient, and electrical conductivity. The MgBrH, CaBrH and SrBrH compounds showed p-type behavior, with positive values for the Seebeck coefficient and the greatest value of ≈180 μV/K, according to the thermoelectric data. At 1000 K, the ZT reach their highest values for CaBrH, SrBrH, and MgBrH, respectively, at 2.9, 2.8, and 0.9. The physical properties of the XBrH with (X = Sr, Ca, and Mg) compounds have been studied in detail.

α-Ta films on c-plane sapphire with enhanced microstructure

Superconducting films of α-Ta are promising candidates for the fabrication of advanced superconducting qubits. However, α-Ta films suffer from many growth-induced structural inadequacies that negatively affect their performance. We have therefore explored a new synthesis method for α-Ta films, which allows for the growth of these films with an unprecedented quality. Using this method, high quality α-Ta films are deposited at a comparably high substrate temperature of 1150 °C. They are single-phase α-Ta and have a single out-of-plane (110) orientation. They consist of grains ≥2 μm that have one of three possible in-plane orientations. As shown by scanning transmission electron microscopy and electron energy loss studies, the substrate–film interfaces are sharp with no observable intermixing. The obtained insights into the epitaxial growth of body-centered-cubic films on quasi-hexagonal substrates lay the basis for harnessing the high structural coherence of such films in various applications.

DFT study of electron energy loss spectra of sulfur in Janus MoSSe, MoSTe, WSSe and WSTe monolayers

In this paper, electronic properties of Janus MSX monolayers (M = Mo, W; X = Se or Te), including electron energy loss near edge structures (ELNES), as K and [Formula: see text] edge spectra of sulfur atoms, have been calculated using a full potential scheme and the augmented plane wave plus local orbitals (APW+lo) method in the framework of density functional theory (DFT). Due to the lack of experimental results, the obtained spectra are compared with the corresponding spectra of MoS2 monolayer. The band structure analysis shows that the Janus MoSSe and WSSe monolayers are direct bandgap semiconductors, while the Janus MoSTe and WSTe monolayers are indirect bandgap semiconductors. In comparison to MoS2, the main structures of the K edge ELNES spectra of sulfur atoms in Janus monolayers occur at lower energies, due to the structural change and increased bond length. The relative reduction of intensities in the main structures predicts the possibility of reducing the number of partial densities of states (PDOS), that is, the reduced p PDOS for the K edge in the corresponding energy range. In the K ([Formula: see text] edge ELNES spectra of the sulfur atom in Janus monolayers and MoS2 monolayers, the main structures are due to the electron transfer to the unoccupied [Formula: see text] and [Formula: see text] states (3s of sulfur and 4d states of the transition metal).

Ultrahigh-Sensitivity and Damage-Free Detection of Single Nanometer-Sized Particle.

In the past decades, various methods, such as chemical sensing, X-ray screening, and spectroscopy, have been employed to detect explosives for environmental protection and national public security. However, achieving ultrahigh sensitivity for detection, which is crucial for some practical applications, remains challenging. This study employs scanning transmission electron microscopy and electron energy loss spectroscopy (STEM-EELS) to detect individual ∼200 nm explosive nanoparticles of octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX). The vibrational modes of HMX were acquired for each single nanoparticle under the aloof STEM-EELS mode, which ensures damage-free detection. Detailed comparisons with Raman and infrared spectra validate the acquired data's origin. This work highlights STEM-EELS as an effective tool in explosives detection, offering ultrahigh sensitivity, damage-free, and nanometer spatial resolution, with potential applications in environmental protection, public security, and criminal investigations.

A mechanical TiAl/TiAlN multinanolayer coating model based on microstructural analysis and nanoindentation

A finite element model reproducing the mechanical behaviour during nanoindentation tests on Ti0.67Al0.33/Ti0.54Al0.46N multilayer coatings was developed. Coatings with two different nanoperiods (10 and 50 nm) were deposited by radio-frequency magnetron sputtering from a single sintered titanium/aluminium target using the reactive gas pulsing process. X-ray diffraction and transmission electron microscopy confirmed the multilayer stacking of the coatings. The finite element models of coatings with these two stacking periods were built considering successive hypotheses: equal thicknesses for metal and nitride nanolayers stacked without transition layer, equal thicknesses stacking with a transition layer between each metal and nitride nanolayer and finally imbalanced thicknesses stacking with a transition layer. The elastic and plastic properties of the stacked nanolayers were determined on thick monolithic coatings of metal and nitride using indentation testing and the finite element model updating method respectively. The elastic-plastic properties of the interface were introduced in the multilayer model as a rule of mixtures of the metal and nitride properties using two hypotheses: parallel or serial. For 50 nm-period film, the interface has a negligible effect on the overall indentation response. On the other hand, for the 10 nm period, the imbalanced stacking model with precise knowledge of the transition layer thickness obtained by N K-edge electron energy loss spectroscopy is required to reproduce the experimental indentation curve. Compared to classical analytical models accounting for hardness, not only the hardnesses but also the indentation moduli appear to be well predicted and evaluated in this work.

Influence of Deposition Parameters on the Plasmonic Properties of Gold Nanoantennas Fabricated by Focused Ion Beam Lithography.

The behavior of plasmonic antennas is influenced by a variety of factors, including their size, shape, and material. Even minor changes in the deposition parameters during the thin film preparation process may have a significant impact on the dielectric function of the film, and thus on the plasmonic properties of the resulting antenna. In this work, we deposited gold thin films with thicknesses of 20, 30, and 40 nm at various deposition rates using an ion-beam-assisted deposition. We evaluate their morphology and crystallography by atomic force microscopy, X-ray diffraction, and transmission electron microscopy. Next, we examined the ease of fabricating plasmonic antennas using focused-ion-beam lithography. Finally, we evaluate their plasmonic properties by electron energy loss spectroscopy measurements of individual antennas. Our results show that the optimal gold thin film for plasmonic antenna fabrication of a thickness of 20 and 30 nm should be deposited at the deposition rate of around 0.1 nm/s. The thicker 40 nm film should be deposited at a higher deposition rate like 0.3 nm/s.

Nanoscopic analysis of rapid thermal annealing effects on InGaN grown over Si(111)

This study explores the impact of rapid thermal annealing (RTA) on InxGa1-xN grown over Si(111) by molecular beam epitaxy (MBE). Through X-ray diffraction (XRD) and reciprocal space map (RSM) characterization, notable shifts in diffraction peaks were observed post-annealing, suggesting alterations of the Indium content in the nanostructures. Morphological assessments using scanning electron microscopy (SEM) and atomic force microscopy (AFM) indicated that RTA could smooth the surface of the samples, though some instances of degradation were also noted. Energy-dispersive X-ray spectroscopy (EDS) showed further stoichiometric modification following annealing. Photoluminescence spectroscopy (PL) revealed notable shifts and increases in the intensity of the InxGa1-xN peaks, indicating the formation of regions with high Indium or Gallium concentration. The presence of these enriched regions was particularly evident from the peaks at around 540 nm and 433 nm, suggesting significant changes in the material's composition. Transmission electron microscopy combined with electron energy loss spectroscopy (TEM-EELS) corroborated the presence of In-rich and Ga-rich areas, affirming the phenomenon of Indium surface segregation. So, this study contributes to understanding the behavior of InxGa1-xN nanostructures under rapid thermal annealing, providing insights for advanced optoelectronic applications.

Space-weathered rims on lunar ilmenite as an indicator for relative exposure ages of regolith

Solar wind irradiation, as a crucial space weathering mechanism, alters the microscopic characteristics and reflectance spectrum of the lunar regolith, and its cumulative effect is strongly related to the exposure time. Ilmenite is highly resistant to solar wind irradiation. Here, we combined transmission electron microscopy, energy-dispersive X-ray spectroscopy, and electron energy loss spectroscopy to systematically illustrate the diverse space-weathered rims on the shoveled and drilled Chang’e-5 ilmenites resulting from varying degrees of solar wind irradiation, revealing that solar wind plays a key role in the early-stage alteration of exposed lunar soil. In addition, the space weathering microstructure observations are consistent with the model-predicted exposure history at the Chang’e-5 landing site and prove that the Chang’e-5 deep-layered drilled (~65 cm) and surface samples (<3 cm) have been exposed for a longer time than that of the intermediate-layered drilled samples. We conclude that the ilmenite rims have the potential to be an effective indicator for comparing the relative exposure ages of regolith on airless bodies.

First-principles calculations of structural, magneto-electronic, mechanical, optical and thermoelectric properties of novel quaternary Heusler alloys type ZrCoYAs (Y= Fe and Mn)

To determine the structural, mechanical, electronic, magnetic, optical, and thermoelectric properties of novel quaternary Heusler alloys type ZrCoYAs (Y= Fe and Mn), we used DFT with WIEN2k. Our results showed that the ferromagnetic Y-type-III phase is more stable due to the higher negative values of their formation energy. We calculated and discussed the elastic constants Cij, which are used to calculate the mechanical properties. The Spin-polarized band structure and DOS calculations using the GGA-PBE and GGA + U approach display a metallic character. However, using the mBJ-GGA-PBE and mBJ-GGA + U approach show a half-metallic character, a semiconductor for the spin-down channel with a direct band gap of 0.61 eV with mBJ-GGA-PBE and 0.74 eV with mBJ-GGA + U for ZrCoMnAs and a direct band gap of 0.43 eV with mBJ-GGA-PBE and indirect band gap with 0.39 eV with mBJ-GGA + U for ZrCoFeAs, in contrast, the spin-up channel is metallic, with 100 % spin polarization and an integer magnetic moment of 1.00 μB for ZrCoMnAs and 2.00 μB for ZrCoFeAs, obeying the Slater-Pauling rule. The estimated Curie temperatures of ZrCoMnAs and ZrCoFeAs are 204 K using the new model, 421 K using MFA, and 385 K using the new model, 1627 K using MFA, respectively. As exchange-correlation potential, MBJ and MBJ + U provide a better description of the electronic and magnetic properties of ZrCoMnAs and ZrCoFeAs compounds. Important optical properties such as dielectric function, absorption coefficient, refractive index, optical conductivity, reflectivity, and electron energy loss function are calculated in the infrared, visible, and ultraviolet range. The static dielectric function suggests that ZrCoMnAs possesses greater polarizability. Both alloys exhibit similar behavior in the far ultraviolet region range and reach a maximum absorption in the ultraviolet range. The half-metallic character of both alloys is revealed from the reflectivity at zero frequency. The calculation of the thermoelectric properties shows positive Seebeck coefficients, indicating that these Heuslers are p-type. Furthermore, the highest power factor is observed at a temperature of 1400 K. The maximum value of ZT is ∼1.1 at 1400 K for ZrCoFeAs and ZrCoMnAs. These studies show that these alloys may have potential applications in the thermoelectric applications.

A TEM Study of Structural Degradation in LiFePO4 Batteries after Hybrid Vehicle Use

Establishing a robust, efficient circular economy for batteries hinges on understanding how they decay over time under various conditions. This understanding is crucial to maximize material use before recycling or disposal. A key aspect of this endeavor is the study of lithium iron phosphate (LiFePO4), a pivotal battery technology whose structural integrity over time remains a subject of inquiry.1 Known aging mechanisms in LiFePO4 (LFP) batteries include electrode degradation, SEI growth, and electrolyte decomposition.1 These processes extend to the cathode, where degradation can manifest as Fe dissolution, Li inventory loss, Fe/Li anti-site defects, and LFP amorphization.1–3 However, these mechanisms are typically studied in lab-aged cells under controlled conditions, leaving a gap in our understanding of their behavior in real-life, commercialized applications.Our research aims to bridge this gap by characterizing the degradation mechanisms of LFP cathode material in various states of health (SOH) after use in a hybrid vehicle. We sourced our cathode samples from 26650 cells extracted from a BAE ESS-A123 hybrid bus battery pack. After selecting cells with drastically different SOHs based on previous analyses,4 we employed transmission electron microscopy (TEM) for detailed characterization.In this talk, we will share insights gained from high-resolution TEM characterization, alongside chemical analysis using energy-filtered TEM and electron energy loss spectroscopy (EELS). Our focus will be on changes in the olivine structure, including lattice parameter alterations, Li and Fe migration, and Fe oxidation. By combining cell-level SOH analyses with TEM characterization, we will highlight how electrochemical test results correlate with material degradation mechanisms, enhancing our understanding of battery health, longevity, and diagnostics. Wang, L. et al. Insights for understanding multiscale degradation of LiFePO4 cathodes. eScience 2, 125–137 (2022). Li, X. et al. First Atomic-Scale Insight into Degradation in Lithium Iron Phosphate Cathodes by Transmission Electron Microscopy. J. Phys. Chem. Lett. 11, 4608–4617 (2020). Xu, P. et al. Efficient Direct Recycling of Lithium-Ion Battery Cathodes by Targeted Healing. Joule 4, 2609–2626 (2020). Ramirez-Meyers, K., Rawn, B. & Whitacre, J. F. A statistical assessment of the state-of-health of LiFePO4 cells harvested from a hybrid-electric vehicle battery pack. J. Energy Storage 59, 106472 (2023).

Analysis of the Ag M4,5 EELS edge to study silver nanoparticle corrosion.

Electron energy loss spectra collected from fresh and corroded silver nanoparticles are compared with those from a number of reference materials, focusing on the M4,5 edge. Chemical shifts and changes in the energy loss near edge structure (ELNES) are described and found to be sufficient to distinguish metallic silver from chemically oxidised silver. The measurements, in conjunction with electron energy loss spectrum imaging, are used to assess the mechanisms for atmospheric corrosion of silver nanoparticles. We unambiguously assign the corrosion product under atmospheric conditions to be silver sulphide, but show the reaction process to be distinctly inhomogeneous, producing a variety of types of corroded particles. LAY DESCRIPTION: >Here, we use analytical electron microscopy to track the corrosion of silver nanoparticles and present chemical maps of the corrosion products. We show clear spectroscopic differences between metallic and corroded silver using the M4,5 electron energy loss spectral feature, which is not commonly studied. Our study shows that corrosion is due to interactions with sulphur in the atmosphere; and the corrosion is not uniform, but appears to develop from specific points on the surface of the nanoparticles.

Embedded Hybrid-Dimensional Heterointerface for Filament Modulation in 2D Material-Based Artificial Nociceptor.

Nociceptors are key sensory receptors that transmit warning signals to the central nervous system in response to painful stimuli. This fundamental process is emulated in an electronic device by developing a novel artificial nociceptor with an ultrathin, nonstoichiometric gallium oxide (GaOx)-silicon oxide heterostructure. A large-area 2D-GaOx film is printed on a substrate through liquid metal printing to facilitate the production of conductive filaments. This nociceptive structure exhibits a unique short-term temporal response following stimulation, enabling a facile demonstration of threshold-switching physics. The developed heterointerface 2D-GaOx film enables the fabrication of fast-switching, low-energy, and compliance-free 2D-GaOx nociceptors, as confirmed through experiments. The accumulation and extrusion of Ag in the oxide matrix are significant for inducing plastic changes in artificial biological sensors. High-resolution transmission electron microscopy and electron energy loss spectroscopy demonstrate that Ag clusters in the material dispersed under electrical bias and regrouped spontaneously when the bias is removed owing to interfacial energy minimization. Moreover, 2D nociceptors are stable; thus, heterointerface engineering can enable effective control of charge transfer in 2D heterostructural devices. Furthermore, the diffusive 2D-GaOx device and its Ag dynamics enable the direct emulation of biological nociceptors, marking an advancement in the hardware implementation of artificial human sensory systems.

Spectroscopic analysis of color origins in titanium-based thin films deposited by cathodic arc deposition

The distinctive colors observed in titanium-based (Ti-based) decorative coatings fabricated by cathodic arc deposition originate from the unique electronic, morphological, and chemical properties of these films. Most Ti-based film colors arise from their surface band gaps, as measured by electron energy loss spectroscopy, with the exception of the lowest brightness (TLB) and green hues. The green color in titanium dioxide films typically results from interference between light reflected from the film and substrate interfaces. In contrast, the black color in Ti-based coatings stems from the chemical structure, specifically the presence of Ti-C and C=C(sp2) bonds within the film. Moreover, the large band gap of the TLB film surface is attributed to surface oxidation, as detected by soft X-ray spectroscopy. Significantly, the film thickness and surface roughness are characterized by field emission secondary electron microscopy and atomic force microscopy, respectively.

Real-time tracking of structural evolution in 2D MXenes using theory-enhanced machine learning

In situ Electron Energy Loss Spectroscopy (EELS) combined with Transmission Electron Microscopy (TEM) has traditionally been pivotal for understanding how material processing choices affect local structure and composition. However, the ability to monitor and respond to ultrafast transient changes, now achievable with EELS and TEM, necessitates innovative analytical frameworks. Here, we introduce a machine learning (ML) framework tailored for the real-time assessment and characterization of in operando EELS Spectrum Images (EELS-SI). We focus on 2D MXenes as the sample material system, specifically targeting the understanding and control of their atomic-scale structural transformations that critically influence their electronic and optical properties. This approach requires fewer labeled training data points than typical deep learning classification methods. By integrating computationally generated structures of MXenes and experimental datasets into a unified latent space using Variational Autoencoders (VAE) in a unique training method, our framework accurately predicts structural evolutions at latencies pertinent to closed-loop processing within the TEM. This study presents a critical advancement in enabling automated, on-the-fly synthesis and characterization, significantly enhancing capabilities for materials discovery and the precision engineering of functional materials at the atomic scale.