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We attain N-polar and Al-polar AlN thin films on Si(111) substrates by plasma-assisted molecular beam epitaxy. The polarity of AlN epilayers has been validated by wet chemical etching using tetramethylammonium hydroxide and by the direct cross-sectional observation of atomic stacking under high-angle annular dark-field scanning transmission electron microscopy. For the 290 nm-thick as-grown N-polar AlN epilayer, x-ray diffraction (XRD) (002) and (102) ω rocking curve peak full width half maximums (FWHMs) are 475 and 1177 arcsec, and the surface mean square roughness (RMS) is 0.30 nm. We flipped the polarity using the metal-flux-modulation-epitaxy (MME) strategy. The MME strategy promotes anti-phase boundaries (APBs) on the { 2 2 ¯ 01 } crystalline planes instead of commonly observed lateral planar APBs in AlN epilayers. Merging of the tilted APBs at ∼50 nm leads to a complete Al-polar surface. For the 180 nm-thick Al-polar AlN epilayer, XRD (002) and (102) peak FWHMs are 1505 and 2380 arcsec, and the surface RMS is 1.41 nm. Strain analysis by XRD and Raman spectroscopy indicates a uniform tensile strain of 0.160% across the N-polar AlN epilayer surface and a strain distribution of 0.113%–1.16% through the epilayer. In contrast, the Al-polar AlN epilayer exhibits a much broader tensile strain distribution of 0.482%–2.406% along the growth direction, potentially due to the interaction of polarity inversion and strain relaxation. [ABSTRACT FROM AUTHOR]

Hafnium diboride (HfB2) is a promising candidate as a seed layer for GaN growth on Si substrates due to its excellent lattice and thermal coefficients matching with both materials. This work investigates the epitaxial growth of AlB2-type non-stoichiometric HfB2 (HfB2+δ with −0.1 < δ < 0.6) thin films on Si(111) using magnetron co-sputtering. We demonstrated that the process temperature significantly affected the surface roughness (RRMS ∼ 0.5–4 nm), film composition, and the nucleation of secondary impurity phases. Films deposited between 700 and 900 °C exhibit epitaxial growth on the Si substrate with a well-defined relationship of (0001) HfB 2 ‖ (111) Si and [ 11 2 ¯ 0 ] HfB 2 ‖ [ 1 1 ¯ 0 ] Si . Detailed x-ray diffraction and scanning transmission electron microscopy analyses reveal that impurity phases detected at high temperatures are primarily carbon-rich phases, identified as HfCx or HfCxBy. Interestingly, this secondary phase's crystal orientation follows the orientation of its surroundings. The different findings in terms of contamination (C and O) and deposition temperature offer valuable insights for further growth optimizing of high-quality epitaxial HfB2 thin films on Si(111) for future GaN-on-Si integration. [ABSTRACT FROM AUTHOR]

Ag-induced crystallization and layer exchange (AgILE) in a stack of amorphous Si/Ag/quartz substrate has been investigated using optical microscopy, scanning electron microscopy, transmission electron microscopy (TEM), scanning TEM-high angle annular dark field (STEM-HAADF) imaging, and electron tomography, covering length scales from a few tens of micrometers to a few tens of nanometers. The size of Ag grains in the underlying as-deposited Ag film varied from ∼10 to 500 nm. The following processes could be discerned using in situ heating of plan-view samples at 500 °C in STEM: (i) AgILE propagation preferentially along regions of small Ag grains, (ii) formation of pushed-up Ag in the vicinity of AgILE reaction cells, (iii) migration and agglomeration of pushed-up Ag on small and large Ag grains, which tend to inhibit AgILE and promote dendricity, and (iv) dispersion of pushed-up Ag, which tend to reduce dendricity. The resulting dendricity was largely confined to the peripheral regions of the impinging reaction cells and decreased with annealing time. In contrast, dendricity due to AgILE and crystallization at 550 °C is stable and extends right from the center to the periphery of the reaction cells. The microscopic mechanism of AgILE and, in particular, the effect of annealing temperature is investigated. The results are discussed in the light of existing literature and compared with Al-induced layer exchange. Annealing at temperature equal to or slightly less than 500 °C is found to be necessary in the case of AgILE to avoid dendricity and to obtain a continuous Si layer with large Si grains. [ABSTRACT FROM AUTHOR]

Achieving high material perfection in aluminum (Al) films and their associated Al/AlOx heterostructures is essential for enhancing the coherence time in superconducting quantum circuits. We grew Al films with thicknesses ranging from 3 to 30 nanometers (nm) epitaxially on sapphire substrates using molecular beam epitaxy (MBE). An integral aspect of our work involved electron-beam (e-beam) evaporation to directly deposit aluminum oxide (Al2O3) films on the freshly grown ultrathin epitaxial Al films in an ultra-high-vacuum (UHV) environment. This in situ oxide deposition is critical for preventing the oxidation of parts of the Al films, avoiding the formation of undesired native oxides, and thereby preserving the nm-thick Al films in their pristine conditions. The thicknesses of our Al films in the study were accurately determined; for example, coherence lengths of 3.0 and 20.2 nm were measured in the nominal 3.0 and 20 nm thick Al films, respectively. These Al films were epitaxially grown on sapphire substrates, showing an orientational relationship, denoted as Al (111) ⟨ 2 1 ¯ 1 ¯ ⟩ ∥ sapphire (0001) [ 2 1 ¯ 1 ¯ 0 ]. The Al/sapphire interface was atomically ordered without any interfacial layers, as confirmed by in situ reflection high-energy electron diffraction (RHEED) and cross-sectional scanning transmission electron microscopy (STEM). All sample surfaces exhibited smoothness with a roughness in the range of 0.1–0.2 nm. The Al films are superconducting with critical temperatures ranging from 1.23 to around 2 K, depending on the film thickness. [ABSTRACT FROM AUTHOR]

Bragg interferometry (BI) is an imaging technique based on four-dimensional scanning transmission electron microscopy (4D-STEM) wherein the intensities of select overlapping Bragg disks are fit or more qualitatively analyzed in the context of simple trigonometric equations to determine local stacking order. In 4D-STEM based approaches, the collection of full diffraction patterns at each real-space position of the scanning probe allows the use of precise virtual apertures much smaller and more variable in shape than those used in conventional dark field imaging such that even buried interfaces marginally twisted from other layers can be targeted. With a coarse-grained form of dark field ptychography, BI uses simple physically derived fitting functions to extract the average structure within the illumination region and is, therefore, viable over large fields of view. BI has shown a particular advantage for selectively investigating the interlayer stacking and associated moiré reconstruction of bilayer interfaces within complex multi-layered structures. This has enabled investigation of reconstruction and substrate effects in bilayers through encapsulating hexagonal boron nitride and of select bilayer interfaces within trilayer stacks. However, the technique can be improved to provide a greater spatial resolution and probe a wider range of twisted structures, for which current limitations on acquisition parameters can lead to large illumination regions and the computationally involved post-processing can fail. Here, we analyze these limitations and the computational processing in greater depth, presenting a few methods for improvement over previous works, discussing potential areas for further expansion, and illustrating the current capabilities of this approach for extracting moiré-scale strain. [ABSTRACT FROM AUTHOR]

An area-selectable Mg doping via ion implantation (I/I) is essential to realize gallium nitride (GaN) based power switching devices. Conventional post-implantation annealing forms considerable defects in the GaN, resulting in extremely low activation efficiency. The recent invention of ultrahigh-pressure annealing (UHPA) has substantially improved the p-type activation efficiency; however, the UHPA causes an unexpected Mg diffusion. Thus, both annealing processes resulted in a much lower Mg concentration in the GaN matrix than the Mg dose. In this study, the effect of a sequential N I/I for p-type Mg-implanted GaN was investigated by the correlative cathodoluminescence, transfer length method, scanning transmission electron microscopy, and atom probe tomography (APT) analyses. APT results have revealed that the sequential N I/I can successfully maintain the Mg concentration in the GaN matrix in the higher range of 1018 cm−3 or more. Our investigation suggests that sequential N I/I is a promising technique to maintain the Mg concentration higher and improve the p-type activation efficiency. [ABSTRACT FROM AUTHOR]

Dislocations have been proposed to affect the performance and reliability of GaN power semiconductors by being conductive pathways for leakage current. However, no direct evidence of a link between their electrical behavior and physical nature in carbon-doped semi-insulating GaN buffer layers has been obtained. Therefore, we investigate the electrical activity of dislocations by conductive atomic force microscopy and electron beam induced current to distinguish electrically active dislocations from non-active ones. We investigated six electrically active dislocations and discovered distinct carbon enrichment in the vicinity of all six dislocations, based on cross-sectional scanning transmission electron microscopy using electron energy loss spectrometry. Electrically non-active dislocations, which are the vast majority, sometimes also showed carbon enrichment, however, in only two out of seven cases. Consequently, carbon segregation seems to be a requirement for electrical activity, but a carbon surplus is not sufficient for electrical activity. We also performed first-principles total-energy calculations for mixed type threading dislocations, which validates carbon accumulation in the dislocation vicinity. The electrical and physical characterization results, complemented by density functional theory simulations, support the previously hypothesized existence of a carbon defect band and add new details. [ABSTRACT FROM AUTHOR]

Conductive-bridge random access memory can be used as a physical reservoir for temporal learning in reservoir computing owing to its volatile nature. Herein, a scaled Cu/HfOx/n+-Si memristor was fabricated and characterized for reservoir computing. The scaled, silicon nanofin bottom electrode formation is verified by scanning electron and transmission electron microscopy. The scaled device shows better cycle-to-cycle switching variability characteristics compared with those of large-sized cells. In addition, synaptic characteristics such as conductance changes due to pulses, paired-pulse facilitation, and excitatory postsynaptic currents are confirmed in the scaled memristor. High-pattern accuracy is demonstrated by deep neural networks applied in neuromorphic systems in conjunction with the use of the Modified National Institute of Standards and Technology database. Furthermore, a reservoir computing system is introduced with six different states attained by adjusting the amplitude of the input pulse. Finally, high-performance and efficient volatile reservoir computing in the scaled device is demonstrated by conductance control and system-level reservoir computing simulations. [ABSTRACT FROM AUTHOR]

This study explores the effect of molecular permanent dipole moment (PDM) on aggregation of guest molecules in phosphorescent host–guest organic light-emitting diodes (OLEDs). Through a combination of photoluminescence measurements, high-angle annular dark-field scanning transmission electron microscopy analysis, and an Ising model based physical vapor-deposition simulation, we show that higher PDM of tris[2-phenylpyridinato-C2,N]iridium(III) guest can actually lead to a reduced aggregation relative to tris[bis[2-(2-pyridinyl-N)phenyl-C] (acetylacetonato)iridium(III) when doped into a non-polar host 1,3,5-tris(carbazol-9-yl)benzene. This study further explores the effect of host polarity by using a polar host 3′,5′-di(carbazol-9-yl)-[1,1′-biphenyl]-3,5-dicarbonitrile, and it is shown that the polar host leads to reduced guest aggregation. This study provides a comprehensive understanding of the impact of molecular PDM on OLED material efficiency and stability, providing insights for optimizing phosphorescent OLED materials. [ABSTRACT FROM AUTHOR]

Energy-dispersive x-ray spectroscopy and high-angle annular dark-field in a Cs-corrected scanning transmission electron microscope are employed to characterize the atomic-scale strain distribution in the active region of the InAs-based interband cascade laser. For the first time, energy-dispersive x-ray spectroscopy is utilized for the quantitative calculation of the zero-strain region, by which the geometric phase analysis of high-angle annular dark-field imaging has been carried out. The strain distribution of the active region with high accuracy has been obtained. The analysis of the out-of-plane strain shows that the active region in the InAs-based interband cascade laser is strain-compensated, while a certain degree of elemental intermixing still exists in the active region. This detailed strain distribution can provide valuable insights into the optimization of the growth conditions for the active region such as growth temperature, V/III flux ratio, and growth process to minimize the elemental intermixing and obtain a better performance interface while maintaining the strain-compensated state. [ABSTRACT FROM AUTHOR]

Domain boundaries in perovskite oxides often exhibit abundant physical properties and phenomena. Here, epitaxial LaTiO3 thin films on (100) SrTiO3 substrates are prepared by pulsed-laser deposition. X-ray diffraction and transmission electron microscopy investigations reveal that the epitaxial LaTiO3 thin films have good crystallinity but a high density of domain boundaries. Atomic-scale scanning transmission electron microscopy observations reveal that two types of domain boundaries are formed in the LaTiO3 thin films. The type I domain boundaries are formed on the {100} crystal planes, while the type II domain boundaries on the {110} crystal planes. Electron energy-loss spectroscopy analyses suggest that the valence states of Ti ions at the type I domain boundaries are +3, while those at the type II domain boundaries are +4. First-principles calculations reveal that the bandgap decreases at both domain boundaries compared to the bulk. The carrier concentration at the type I domain boundaries is significantly higher than that of the bulk, while the carrier concentration at the type II domain boundaries is lower. These findings suggest that domain boundaries play an important role in tailoring the electrical properties of the LaTiO3 thin films, thereby promoting the potential applications and property modulation of related materials and devices. [ABSTRACT FROM AUTHOR]

Past functional toxicogenomic studies have indicated that genes relevant to membrane lipid synthesis are important for tolerance to the lanthanides. Moreover, previously reported imaging of patient's brains following administration of gadolinium-based contrast agents shows gadolinium lining the vessels of the brain. Taken together, these findings suggest the disruption of cytoplasmic membrane integrity as a mechanism by which lanthanides induce cytotoxicity. In the presented work we used scanning transmission electron microscopy and spatially resolved elemental spectroscopy to image the morphology and composition of gadolinium, europium, and samarium precipitates that formed on the outside of yeast cell membranes. In no sample did we find that the lanthanide contaminant had crossed the cell membrane, even in experiments using yeast mutants with disrupted genes for sphingolipid synthesis-the primary lipids found in yeast cytoplasmic membranes. Rather, we have evidence that lanthanides are co-located with phosphorus outside the yeast cells. These results lead us to hypothesize that the lanthanides scavenge or otherwise form complexes with phosphorus from the sphingophospholipid head groups in the cellular membrane, thereby compromising the structure or function of the membrane, and gaining the ability to disrupt membrane function without entering the cell.

We describe the development, operation, and application of the 4D Camera-a 576 by 576 pixel active pixel sensor for scanning/transmission electron microscopy which operates at 87,000 Hz. The detector generates data at ∼480 Gbit/s which is captured by dedicated receiver computers with a parallelized software infrastructure that has been implemented to process the resulting 10-700 Gigabyte-sized raw datasets. The back illuminated detector provides the ability to detect single electron events at accelerating voltages from 30 to 300 kV. Through electron counting, the resulting sparse data sets are reduced in size by 10--300× compared to the raw data, and open-source sparsity-based processing algorithms offer rapid data analysis. The high frame rate allows for large and complex scanning diffraction experiments to be accomplished with typical scanning transmission electron microscopy scanning parameters.

Ferroelectric domain walls are a rich source of emergent electronic properties and unusual polar order. Recent studies show that the configuration of ferroelectric walls can go well beyond the conventional Ising-type structure. Néel-, Bloch-, and vortex-like polar patterns have been observed, displaying strong similarities with the spin textures at magnetic domain walls. Here, the discovery of antiferroelectric domain walls in the uniaxial ferroelectric Pb5Ge3O11 is reported. Highly mobile domain walls with an alternating displacement of Pb atoms are resolved, resulting in a cyclic 180° flip of dipole direction within the wall. Density functional theory calculations show that Pb5Ge3O11 is hyperferroelectric, allowing the system to overcome the depolarization fields that usually suppress the antiparallel ordering of dipoles along the longitudinal direction. Interestingly, the antiferroelectric walls observed under the electron beam are energetically more costly than basic head-to-head or tail-to-tail walls. The results suggest a new type of excited domain-wall state, expanding previous studies on ferroelectric domain walls into the realm of antiferroic phenomena.

We report on the magnetic coupling behavior in all-ferromagnetic La0.7Sr0.3MnO3/SrRuO3 (LSMO/SRO) heterostructures deposited on the SrTiO3 (111) substrate, where the interface leads to an enhanced exchange field as compared to the one deposited on SrTiO3 (001). Importantly, high-resolution scanning transmission electron microscopy reveals distinct interface structures of the (111) heterostructures depending on the growth sequence. The heterostructure with an SRO bottom layer shows an atomically flat and abrupt interface, while the one with an LSMO bottom layer shows a deformed interface due to the surface roughening of LSMO deposited directly on SrTiO3 (111). As a result, the heterostructure with an abrupt interface exhibits a robust antiferromagnetic coupling between LSMO and SRO, while the one with a rough interface shows negligible magnetic coupling. Our results demonstrate the key role of an abrupt interface in determining the magnetic properties of oxide heterostructures. [ABSTRACT FROM AUTHOR]

MnO(001) thin films were grown on commercial MgO(001) substrates at 520 °C by reactive molecular beam epitaxy (MBE) using Mn vapor and O2-seeded supersonic molecular beams (SMBs) both with and without radio frequency (RF) plasma excitation. For comparison, MnO(001) films were grown by reactive MBE using O2 from a leak valve. X-ray photoelectron spectroscopy confirmed the Mn2+ oxidation state and 10%–15% excess oxygen near the growth surface. Reflection high-energy electron diffraction and x-ray diffraction evidenced that the films were rock salt cubic MnO with very strong (001) orientation. High-angle annular dark field scanning transmission electron microscopy with energy-dispersive x-ray spectroscopy demonstrated abrupt MnO/MgO interfaces and indicated [(001)MnO||(001)MgO] epitaxial growth. Ex situ atomic force microscopy of films deposited without RF excitation revealed smooth growth surfaces. An SMB-grown MnO(001) film was converted to Mn3O4 with strong (110) orientation by post-growth exposure to an RF-discharge (RFD) SMB source providing O atoms; the surface of the resultant film contained elongated pits aligned with the MgO 110 directions. In contrast, using the RFD-SMB source for growth resulted in MnO(001) films with elongated growth pits and square pyramidal hillocks aligned along the MgO 110 and 100 directions, respectively. [ABSTRACT FROM AUTHOR]

A unique on-chip method for the direct correlation of optical properties, with atomic-scale chemical–structural characteristics for a single quantum dot (QD), is developed and utilized in various examples. This is based on performing single QD optical characterization on a modified glass substrate, followed by the extraction of the relevant region of interest by focused-ion-beam–scanning electron microscope processing into a lamella for high resolution scanning transmission electron microscopy (STEM) characterization with atomic scale resolution. The direct correlation of the optical response under an electric field with STEM analysis of the same particle allows addressing several single particle phenomena: first, the direct correlation of single QD photoluminescence (PL) polarization and its response to the external field with the QD crystal lattice alignment, so far inferred indirectly; second, the identification of unique yet rare few-QD assemblies, correlated directly with their special spectroscopic optical characteristics, serving as a guide for future designed assemblies; and third, the study on the effect of metal island growth on the PL behavior of hybrid semiconductor–metal nanoparticles, with relevance for their possible functionality in photocatalysis. This work, therefore, establishes the use of the direct on-chip optical–structural correlation method for numerous scenarios and timely questions in the field of QD research. [ABSTRACT FROM AUTHOR]

This paper explores the fundamental structural origins of the 0.7 eV band emission peak, known as D07. The increased attention on these d-band emission lines originates mainly from the correlation between crystal defect and the intensified recombination of less dominant charge carriers. This association holds substantial importance, impacting not just the electronics sector but also raising concerns about reduced efficiency in silicon solar cells. By employing hyperspectral photoluminescence imaging, we pinpointed regions manifesting high D07 peak emissions on a microscopic scale. Subsequently, we conducted a structural investigation utilizing scanning electron microscopy and electron backscatter diffraction. Following this, we used a focused ion beam to extract areas of interest, allowing for a detailed characterization of the sample using high-resolution scanning transmission electron microscopy at the atomic scale. This approach aids in identifying defects and determining grain boundary orientation. In areas of high D07 band emission, we found Σ 3 { 114 } { 101 } grain boundaries decorated with two-layer fault twin and/or an extrinsic two-layer stacking faults. In addition, density functional theory calculations suggest oxygen impurities as a possibility for substitutional segregation to these types of defects. It is therefore plausible that the D07 line might be attributed to stacking faults featuring oxygen agglomerates. [ABSTRACT FROM AUTHOR]

For two-dimensional (2D) materials, the exact thickness of the material often dictates its physical and chemical properties. The 2D quantum material WTe2 possesses properties that vary significantly from a single layer to multiple layers, yet it has a complicated crystal structure that makes it difficult to differentiate thicknesses in atomic-resolution images. Furthermore, its air sensitivity and susceptibility to electron beam-induced damage heighten the need for direct ways to determine the thickness and atomic structure without acquiring multiple measurements or transferring samples in ambient atmosphere. Here, we demonstrate a new method to identify the thickness up to ten van der Waals layers in Td-WTe2 using atomic-resolution high-angle annular dark-field scanning transmission electron microscopy image simulation. Our approach is based on analyzing the intensity line profiles of overlapping atomic columns and building a standard neural network model from the line profile features. We observe that it is possible to clearly distinguish between even and odd thicknesses (up to seven layers), without using machine learning, by comparing the deconvoluted peak intensity ratios or the area ratios. The standard neural network model trained on the line profile features allows thicknesses to be distinguished up to ten layers and exhibits an accuracy of up to 94% in the presence of Gaussian and Poisson noise. This method efficiently quantifies thicknesses in Td-WTe2, can be extended to related 2D materials, and provides a pathway to characterize precise atomic structures, including local thickness variations and atomic defects, for few-layer 2D materials with overlapping atomic column positions. [ABSTRACT FROM AUTHOR]

The exploration of 1D magnetism, frequently portrayed as spin chains, constitutes an actively pursued research field that illuminates fundamental principles in many-body problems and applications in magnonics and spintronics. The inherent reduction in dimensionality often leads to robust spin fluctuations, impacting magnetic ordering and resulting in novel magnetic phenomena. Here, structural, magnetic, and optical properties of highly anisotropic 2D van der Waals antiferromagnets that uniquely host spin chains are explored. First-principle calculations reveal that the weakest interaction is interchain, leading to essentially 1D magnetic behavior in each layer. With the additional degree of freedom arising from its anisotropic structure, the structure is engineered by alloying, varying the 1D spin chain lengths using electron beam irradiation, or twisting for localized patterning, and spin textures are calculated, predicting robust stability of the antiferromagnetic ordering. Comparing with other spin chain magnets, these materials are anticipated to bring fresh perspectives on harvesting low-dimensional magnetism.

Optimizing thermal anneals of Si-implanted β-Ga2O3 is critical for low resistance contacts and selective area doping. We report the impact of annealing ambient, temperature, and time on the activation of room temperature ion-implanted Si in β-Ga2O3 at concentrations from 5 × 1018 to 1 × 1020 cm−3, demonstrating full activation (>80% activation, mobilities >70 cm2/V s) with contact resistances below 0.29 Ω mm. Homoepitaxial β-Ga2O3 films, grown by plasma-assisted molecular beam epitaxy on Fe-doped (010) substrates, were implanted at multiple energies to yield 100 nm box profiles of 5 × 1018, 5 × 1019, and 1 × 1020 cm−3. Anneals were performed in an ultra-high vacuum-compatible quartz furnace at 1 bar with well-controlled gas compositions. To maintain β-Ga2O3 stability, pO2 must be greater than 10−9 bar. Anneals up to pO2 = 1 bar achieve full activation at 5 × 1018 cm−3, while 5 × 1019 cm−3 must be annealed with pO2 ≤ 10−4 bar, and 1 × 1020 cm−3 requires pO2 < 10−6 bar. Water vapor prevents activation and must be maintained below 10−8 bar. Activation is achieved for anneal temperatures as low as 850 °C with mobility increasing with anneal temperatures up to 1050 °C, though Si diffusion has been reported above 950 °C. At 950 °C, activation is maximized between 5 and 20 min with longer times resulting in decreased carrier activation (over-annealing). This over-annealing is significant for concentrations above 5 × 1019 cm−3 and occurs rapidly at 1 × 1020 cm−3. Rutherford backscattering spectrometry (channeling) suggests that damage recovery is seeded from remnant aligned β-Ga2O3 that remains after implantation; this conclusion is also supported by scanning transmission electron microscopy showing retention of the β-phase with inclusions that resemble the γ-phase. [ABSTRACT FROM AUTHOR]

We study epitaxial growth, crystal structures, and magnetic properties of Fe–As compound thin films grown on GaAs (111)B substrates at various values of the As4:Fe flux ratio γ, using molecular beam epitaxy. The samples grown at low As4 flux (γ = 0.3, sample A) show mainly a body-centered-cubic (bcc) crystal structure, exhibiting ferromagnetic properties similar to bcc Fe. Meanwhile, the Fe–As samples grown at medium γ (2.7–4.5, sample group B) comprise regions of Ni2In-type FeAs (a hexagonal crystal with lattice constants of a = 0.399 nm and c = 0.536 nm), which are grown at the bottom and interface with the GaAs buffer layer, and a layer of non-stoichiometric FeAs with a DO3 structure (a = 0.522 nm) formed on the top. The DO3-structure FeAs phase contains partially transformed regions, which are characterized by thin stripes in a scanning transmission electron microscopy image. Furthermore, in the sample grown with high γ = 8.5 (sample C), a hexagonal Fe–As crystal with a large in-plane lattice constant (a = 0.691 nm and c = 0.542 nm) and threefold screw axes are observed. None of these crystal structures of Fe–As compounds has ever been reported. While sample C shows no ferromagnetism, the samples in group B exhibit strong ferromagnetism with high Curie temperature TC above 400 K. These new ferromagnetic Fe–As compounds are promising for spintronic device applications. [ABSTRACT FROM AUTHOR]

Load-dependent and angle-dependent nanoindentation tests were performed on a ( 2 ¯ 01) -oriented single-crystal β-Ga2O3 substrate to study the mechanical properties of the material. The anisotropy of the mechanical properties was examined, especially with regard to the dependence of the elastic modulus (E), hardness (H), and form of plastic deformation on the rotation angle of a Berkovich indenter with respect to the monoclinic structure. E reached a maximum value and H a minimum value when the sample was rotated to such an angle that one of the three facets of the Berkovich indenter was parallel to the [010] direction. To compare our experimental results with the theoretical calculation based on the monoclinic structure, the elastic surface of β-Ga2O3 was calculated using fourth-rank stiffness and compliance tensors and visualized in three-dimensional space. Two-dimensional sectional maps of the elastic surface were obtained for a range of crystal planes, and good agreement was obtained between the experimental observations and calculations. Plastic deformation at the indenter impressions was evaluated using scanning and transmission electron microscopy, and dislocations, cleavage, and cracks were observed. Their structure and density depended on the rotation angle. Our results clearly show a strong anisotropy of the mechanical properties of β-Ga2O3, which is very different from what is found in other compound semiconductors for power-device applications, such as GaN and 4H-SiC. This emphasizes the importance of customizing the machining process for β-Ga2O3, rather than simply using "machining recipes" for other materials. [ABSTRACT FROM AUTHOR]

GeSnC alloys offer a route to direct bandgap semiconductors for CMOS-compatible lasers, but the use of CBr4 as a carbon source was shown to reduce Sn incorporation by 83%–92%. We report on the role of thermally cracked H in increasing Sn incorporation by 6x–9.5x, restoring up to 71% of the lost Sn, and attribute this increase to removal of Br from the growth surface as HBr prior to formation of volatile groups such as SnBr4. Furthermore, as the H flux is increased, Rutherford backscattering spectroscopy reveals a monotonic increase in both Sn and carbon incorporation. X-ray diffraction reveals tensile-strained films that are pseudomorphic with the substrate. Raman spectroscopy suggests substitutional C incorporation; both x-ray photoelectron spectroscopy and Raman suggest a lack of graphitic carbon or its other phases. For the lowest growth temperatures, scanning transmission electron microscopy reveals nanovoids that may account for the low Sn substitutional fraction in those layers. Conversely, the sample grown at high temperatures displayed abrupt interfaces, notably devoid of any voids, tin, or carbon-rich clusters. Finally, the surface roughness decreases with increasing growth temperature. These results show that atomic hydrogen provides a highly promising route to increase both Sn and C to achieve a strongly direct bandgap for optical gain and active silicon photonics. [ABSTRACT FROM AUTHOR]

High quality, uni-polar, epitaxial AlN with minimum oxygen content promises excellent surface acoustic wave and bulk acoustic wave resonator characteristics such as high electromechanical coupling coefficient and power handling capabilities, which is particularly useful for RF filter applications. By systematically varying the growth temperature, the study investigates its impact on the oxygen levels, defect states, and crystallographic texture of the AlN thin films using a combination of atomic force microscopy, X-ray diffraction, time-of-flight secondary ion mass spectrometry, spectroscopic ellipsometry, scanning transmission electron microscopy, as well as room temperature and temperature dependent I–V measurements. The research demonstrates that the films grown at a temperature of 700 ° C exhibit the most favorable results. These films exhibit the lowest oxygen levels, possess epitaxial growth, and display the highest crystalline quality (XRD AlN 0002 ω − FWHM = 1.3 °). Additionally, these films demonstrate a significant reduction in sub-bandgap absorption. By comparing the cathode current measured during deposition, we suggest that the presence of an impurity layer formed during idle time between depositions as a possible source of oxygen in the sputter chamber. In addition, the study presents a possible model to explain the mixed polarity observed in AlN and proposes various ways to achieve uni-polar AlN on silicon substrates. [ABSTRACT FROM AUTHOR]

Here, we describe a fully in situ method of fabricating light-scattering structures on III-V materials that generates a rough morphology via vapor phase etching and redeposition. Fully in situ methods support higher industrial throughput by utilizing the growth reactor to generate the light-trapping structures after device growth without removal from the reactor. We use HCl and PH3 to etch and redeposit scattering morphologies on Ga0.5In0.5P in a dynamic hydride vapor phase epitaxy (D-HVPE) reactor. We show that the addition of PH3 leads to redeposition during the vapor phase HCl etching of Ga0.5In0.5P and that HCl flow rate and time exposed to HCl-PH3 each independently cause a linear increase in the redeposited feature size, indicating that redeposition proceeds by island growth in a III-Cl-limited, hydride-enhanced HVPE regime. Auger electron spectroscopy and scanning transmission electron microscopy with energy dispersive spectroscopy (STEM-EDS) reveal redeposition to be highly Ga-rich GaInP, i.e., Ga(In)P. The Ga-rich nature of the redeposition results from the higher thermodynamic driving force for Ga incorporation than for In during HVPE growth and the difference in the volatility of the III-Cl etch products. The resulting morphologies have high broadband scattering, as determined by normal specular reflectance and integrating sphere measurements, indicating effectiveness as light-scattering structures. In a 270-nm-thick GaAs photovoltaic device with a textured back surface, we achieve a 4.9% increase in short circuit current density (JSC) without any loss in open-circuit voltage (VOC) relative to a planar control using only a 60 s in situ texturing treatment. [ABSTRACT FROM AUTHOR]

Crystallographic defects play a crucial role in cement hydration, with initial dissolution being dominated by the formation of etch pits that rely on the intersection of defects on surfaces. However, the defects present in cement particles have remained a mystery due to the lack of detailed direct observation at the atomic scale. In this study, we used scanning transmission electron microscopy to unravel the defects in alite particles at the single-atom level. Our observations identified different types of defects, including vacancies, doping, dislocations, rough surfaces, and grain boundaries. Atomic ordering in the alite crystal was further examined based on our single-atom recognition method. Our findings indicate that defects in cement particles may serve as reactive sites during the early hydration stage, facilitating the initial dissolution and providing nucleation sites for hydration products. This work provides insights into cement defect formation at the single-atom level and offers new opportunities in tuning the hydration process through defect engineering of cement particles.

Hollow vaterite microspheres are important materials for biomedical applications such as drug delivery and regenerative medicine owing to their biocompatibility, high specific surface area, and ability to encapsulate a large number of bioactive molecules and compounds. We demonstrated that hollow vaterite microspheres are produced by an Escherichia coli strain engineered with a urease gene cluster from the ureolytic bacteria Sporosarcina pasteurii in the presence of bovine serum albumin. We characterized the 3D nanoscale morphology of five biogenic hollow vaterite microspheres using 3D high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) tomography. Using automated high-throughput HAADF-STEM imaging across several sample tilt orientations, we show that the microspheres evolved from a smaller more ellipsoidal shape to a larger more spherical shape while the internal hollow core increased in size and remained relatively spherical, indicating that the microspheres produced by this engineered strain likely do not contain the bacteria. The statistical 3D morphology information demonstrates the potential for using biogenic calcium carbonate mineralization to produce hollow vaterite microspheres with controlled morphologies. STATEMENT OF SIGNIFICANCE: The nanoscale 3D structures of biomaterials determine their physical, chemical, and biological properties, however significant efforts are required to obtain a statistical understanding of the internal 3D morphology of materials without damaging the structures. In this study, we developed a non-destructive, automated technique that allows us to understand the nanoscale 3D morphology of many unique hollow vaterite microspheres beyond the spectroscopy methods that lack local information and microscopy methods that cannot interrogate the full 3D structure. The method allowed us to quantitatively correlate the external diameters and aspect ratios of vaterite microspheres with their hollow internal structures at the nanoscale. This work demonstrates the opportunity to use automated transmission electron microscopy to characterize nanoscale 3D morphologies of many biomaterials and validate the chemical and biological functionality of these materials.

Scanning transmission electron microscopy is a common tool used to study the atomic structure of materials. It is an inherently multimodal tool allowing for the simultaneous acquisition of multiple information channels. Despite its versatility, however, experimental workflows currently rely heavily on experienced human operators and can only acquire data from small regions of a sample at a time. Here, we demonstrate a flexible pipeline-based system for high-throughput acquisition of atomic-resolution structural data using an all-piezo sample stage applied to large-scale imaging of nanoparticles and multimodal data acquisition. The system is available as part of the user program of the Molecular Foundry at Lawrence Berkeley National Laboratory.

Single-atom catalysts exhibit immense potential across diverse reactions, yet their synthesis and stability in acidic environments pose significant challenges. Herein, we introduce a facile one-step hydrothermal approach to fabricate Ru single-atom alloy catalysts (Ru SAAC) through the reaction of Ru and Ti precursors, followed by annealing in an argon atmosphere. Analysis via extended X-ray absorption fine structure spectroscopy and aberration-corrected scanning transmission electron microscopy confirms the atomically dispersed Ru alloy catalyst anchored on a TiO 2 support. Remarkably, Ru SAAC demonstrates exceptional electrocatalytic performance in the iodide oxidation reaction (IOR), achieving a benchmark current density of 10 mA/cm2 at a mere voltage of 0.64 V in acidic conditions within a three-electrode electrolyzer setup. Surpassing nanoscale Ru/TiO 2 and RuO 2 /TiO 2 counterparts, Ru SAAC exhibits the highest voltage efficiency (84.4%), lowest Tafel slope (36 mV/dec), and lowest overpotential (100 mV) under identical experimental conditions. This method enables facile control over Ru morphology. It enhances the kinetics and thermodynamic favorability of Ru SAAC in acidic media, opening avenues for synthesizing diverse transition metal-based single-alloy catalysts for varied applications. [Display omitted] • A simple one-step hydrothermal method to fabricate Ru single-atom alloy catalysts. • Achieving a low potential of 0.64 V at 10 mA/cm2, outperforming other Ru/TiO₂ catalysts. • Energy-saving iodide oxidation reaction favorable for coupling hydrogen production. • It gives highest voltage efficiency (84.4%), lowest Tafel slope (36 mV/dec), lowest overpotential. • Method offers easy control over Ru morphology, enhancing kinetics and stability in acidic media. [ABSTRACT FROM AUTHOR]

A hybrid material consisting of an array of vertically ordered carbon nanotubes (CNTs) in porous anodic alumina was fabricated directly on oxidized Si substrates. Individual CNTs with vertical orientation were grown using the catalyst Ni nanoparticles (NPs) embedded in the pore walls of a thin template based on porous anodic alumina with a pore diameter of 40 ± 5 nm. The initial film was a two-layer Ti-Al structure on a Si/SiO 2 substrate. A vertically oriented porous structure was formed by anodizing the Al layer. Electrochemical deposition was used to form the catalyst Ni-NPs with dimensions of 30 ± 5 nm. CNTs were synthesized by high-temperature chemical vapor deposition. Scanning and transmission electron microscopy, Raman spectroscopy, and X-ray diffraction were used to analyze the surface morphology and microstructure of the composite nanostructures. The CNT length was (0.6–1.5) μm, and the CNT spacing was 110 ± 10 nm. It is expected that the resulting structure will serve as a basis for the development of CNT-based electrodes for electrochemical impedance biosensors. Electrochemical impedance spectroscopy was used for the electrochemical characterization of the fabricated CNT-based electrodes. The results showed that the CNT-based electrodes are characterized by improved electron transfer kinetics. [ABSTRACT FROM AUTHOR]

The objective of this work was to synthesize a new catalyst x-MoO 3 /Ni 0.5 Zn 0.5 Fe 2 O 4 using the combustion reaction method and to evaluate its catalytic potential and reuse in biodiesel production from waste oil, optimizing the process through experimental design. The catalysts were characterized in terms of structure by X-ray diffraction and phase quantification by Rietveld refinement, surface area by the Brunauer-Emmett-Teller technique, experimental density by helium pycnometry, acidity tests by ammonia desorption at programmed temperature, chemical analysis by X-ray fluorescence, morphology by scanning and transmission electron microscopy, and catalytic properties. The products of the simultaneous transesterification and esterification reactions were characterized by gas chromatography and acidity index. The results indicate the formation of catalysts with surface area ranging from 1.5 to 1.7 m2/g and density ranging from 4.5 to 5.1 g/cm3, composed of major crystalline phases of MoO 3 in the orthorhombic configuration and cubic Ni 0.5 Zn 0.5 Fe 2 O 4 ferrite, with total acidity ranging from 70 to 182 μmol/g of NH 3. Morphological characterization revealed that the catalyst comprises irregular plates of various sizes and shapes with a wide range of cluster sizes. In the simultaneous transesterification and esterification reactions of residual oil, the catalysts were active under all conditions tested, with emphasis on the catalyst containing 50 % Mo ions and 50 % Ni 0.5 Zn 0.5 Fe 2 O4 presenting the best catalytic performance with a conversion of 95 % in ethyl esters and a reduction of 71 % in acidity, with a service life of 6 cycles, an average conversion of 90 % and good thermal and structural stability after use. The experimental design was significant and predictive, with a confidence level of 95 %. Statistical analysis identified that all input variables (temperature, time, and amount of catalyst) were significant for the adopted design. The new catalyst composed of molybdenum, iron, nickel, and zinc has a positive impact on biodiesel synthesis from frying oil and ethanol. [ABSTRACT FROM AUTHOR]

We investigated the electrocatalytic properties of Ir/β‐MnO2, with 4.2–5.6 atomic % (at %) iridium. The Ir/β‐MnO2 was synthesized by heating Ir/R‐MnO2—formed via a surfactant‐assisted (SA) method using KMnO4, IrCl3.H2O, and sodium dodecyl sulfate (SDS)—to 400 °C. The Ir/β‐MnO2 (SA) was nano‐sized based on scanning and transmission electron microscopy (SEM and TEM). Using linear sweep voltammetry (LSV), 5.6 at % Ir/β‐MnO2 (SA) exhibited an overpotential (η) ${\eta){\rm \ }}$ of 327±5 mV for the oxygen evolution reaction (OER), at 10 mAcm-2 ${\hskip0.17em{{\rm c}{\rm m}}^{-2}}$ in 0.5 M H2SO4 electrolyte. At 10 mA cm-2 ${{{\rm c}{\rm m}}^{-2}}$ the Ir/β‐MnO2 (SA) catalyzed the OER for 72 h at an η ${\eta }$ of 534 mV. During this time there was a 12 % loss in Mn and 8 % loss in Ir from the structure. An IrO2 catalyst exhibited an initial η of 420±7 for the OER, but after 20 h of operation at 10 mA cm-2 ${{{\rm c}{\rm m}}^{-2}}$ there was a steep rise in potential (>550 mV) and 12 % loss in Ir. The enhanced activity and stability of Ir/β‐MnO2 (SA) is attributed to the incorporation of Ir into the MnO2 lattice during synthesis and the formation of nano‐sized particles using the SA method. [ABSTRACT FROM AUTHOR]

In GaN‐on‐Si nanowire integration schemes, where the nanowires are contacted through the substrate, the interfaces between silicon substrate, AlN buffer layer, and GaN nanowire are of high interest. Herein, analysis by scanning transmission electron microscopy (STEM) of GaN nanowires grown on Si(111) by metal–organic vapor phase epitaxy using a polarity‐ and site‐controlled growth method is presented. This method is based on prestructuring the substrate, ex situ oxidation of the surface, and in situ oxide layer desorption. First, an AlN layer is grown to prevent melt‐back etching. Samples are prepared for STEM by focused ion beam cutting. STEM measurements in three different regions reveal that the AlN buffer material is polycrystalline. The degree of polycrystallinity is found to depend on the observed region: the highest degree exists at the field area between nanowires and the lowest at the sidewall of the Si‐pillars. On the sidewall, the c→$$ \overrightarrow{c} $$‐direction of the AlN grain is tilted by 30.1° with regard to the Si{111} sidewall plane, leading to reduced lattice mismatch at this location. The growth of GaN is competing with diffusion of Ga atoms through grain boundaries. The dominant mechanism is dependent on the region, leading to site‐controlled growth of nanowires. [ABSTRACT FROM AUTHOR]

Defect-engineered and even amorphous two-dimensional (2D) materials have recently gained interest due to properties that differ from their pristine counterparts. Since these properties are highly sensitive to the exact atomic structure, it is crucial to be able to characterize them at atomic resolution over large areas. This is only possible when the imaging process is automated to reduce the time spent on manual imaging, which at the same time reduces the observer bias in selecting the imaged areas. Since the necessary datasets include at least hundreds if not thousands of images, the analysis process similarly needs to be automated. Here, we introduce disorder into graphene and monolayer hexagonal boron nitride (hBN) using low-energy argon ion irradiation, and characterize the resulting disordered structures using automated scanning transmission electron microscopy annular dark field imaging combined with convolutional neural network-based analysis techniques. We show that disorder manifests in these materials in a markedly different way, where graphene accommodates vacancy-type defects by transforming hexagonal carbon rings into other polygonal shapes, whereas in hBN the disorder is observed simply as vacant lattice sites with very little rearrangement of the remaining atoms. Correspondingly, in the case of graphene, the highest introduced disorder leads to an amorphous membrane, whereas in hBN, the highly defective lattice contains a large number of vacancies and small pores with no indication of amorphisation. Overall, our study demonstrates that combining automated imaging and image analysis is a powerful way to characterize the structure of disordered and amorphous 2D materials, while also illustrating some of the remaining shortcomings with this methodology. [ABSTRACT FROM AUTHOR]

Metal‐coordinated N‐doped carbon (M‐N‐C) materials with highly curved structures have become a promising class of electrocatalysts for the oxygen reduction reaction (ORR). However, the stability of these electrocatalysts remains a problem due to the traditional post‐metal loading strategy. Herein, single‐atomic Co‐N‐C active sites anchored on helical carbonaceous nanotubes (HCNTs) are prepared (Co‐N‐C@HCNT) by pyrolyzing Co porphyrins and helical polypyrroles (PPys) mixtures at high‐temperature by one‐step method. Aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) and X‐ray absorption fine structure (XAFS) measurements confirm single‐atomic active sites and Co‐N4 coordination structures of Co‐N‐C@HCNT. The optimized Co‐N‐C@HCNT exhibits excellent catalytic ORR activity with a half‐wave potential (E1/2) of 0.86 V versus reversible hydrogen electrode (vs RHE) compared to Co‐N‐C@CNT without helical structures (E1/2 = 0.81 V vs RHE) measured in 0.1 m KOH. Co‐N‐C@HCNT also displays excellent stability with a slight current decrease (4%) after running for 10 h featuring Co‐N4 active sites tightly anchored on HCNTs due to electrostatic interactions between metal porphyrins and PPys. Theoretical calculations indicate that the curved structure can increase the charge and decrease d‐band center at Co active site, which enhances electrocatalytic activity. This work provides a simple but effective strategy to construct helical M‐N‐C materials. [ABSTRACT FROM AUTHOR]

Revealing the hardening mechanisms is crucial for facilitating the design of superhard high‐entropy borides. Taking high‐entropy diborides (HEB2) as the prototype, the hardening mechanisms of high‐entropy borides are thoroughly investigated. Specifically, the equiatomic 4—9‐cation single‐phase HEB2 ceramics (4—9HEB2) are fabricated by an ultra‐fast high‐temperature sintering method. The experimental results show that the hardness of the as‐fabricated 4—9HEB2 samples has an increasing tendency with the increase of metal components. With a combination of first‐principles calculations, machine‐learning‐potential‐based molecular dynamics simulations, and scanning transmission electron microscopy characterizations, lattice distortion is explicitly identified to be essential in hardening HEB2 by increasing strain field fluctuation, enlarging atomic strain energy, and strengthening B─B bonds. The results unravel the hardening mechanisms of HEB2 by intensifying lattice distortion, providing fascinating guidance for developing superhard high‐entropy borides. [ABSTRACT FROM AUTHOR]

We report on the synthesis, crystal, and electronic structure, as well as the magnetic, and electric properties of the phosphorus‐containing tantalum nitride P1−xTa8+xN13 (x=0.1–0.15). A high‐pressure high‐temperature reaction (8 GPa, 1400 °C) of Ta3N5 and P3N5 with NH4F as a mineralizing agent yields the compound in the form of black, rod‐shaped crystals. Single‐crystal X‐ray structure elucidation (space group C2/m (no. 12), a=16.202(3), b=2.9155(4), c=11.089(2) Å, β=126.698(7)°, Z=2) shows a network of face‐ and edge‐sharing Ta‐centered polyhedra that contains small vacant channels and PN6 octahedra strands. Atomic resolution transmission electron microscopy reveals an unusual P/Ta disorder. Mixed‐valent tantalum atoms exhibit interatomic distances similar to those in metallic tantalum, however, the electrical resistivity is quite high in the order of 101 Ω cm. The density of states and the electron localization function indicate localized electrons in both covalent and ionic bonds between P/Ta and N atoms, combined with less localized electrons that do not contribute to interatomic bonds. [ABSTRACT FROM AUTHOR]

Aim: To use autofluorescence multispectral imaging (AFMI) to develop a non-invasive assay for the in-depth characterisation of human bone marrow derived mesenchymal stromal cells (hBM-MSCs). Methods: hBM-MSCs were imaged by AFMI on gridded dishes, stained for endpoints of interest (STRO-1 positivity, alkaline phosphatase, beta galactosidase, DNA content) then relocated and results correlated. Intensity, texture and morphological features were used to characterise the colour distribution of regions of interest, and canonical discriminant analysis was used to separate groups. Additionally, hBM-MSC lines were cultured to arrest, with AFMI images taken after each passage to investigate whether an assay could be developed for growth potential. Results: STRO-1 positivity could be predicted with a receiver operator characteristic area under the curve (AUC) of 0.67. For spontaneous differentiation this was 0.66, for entry to the cell-cycle it was 0.77 and for senescence it was 0.77. Growth potential (population doublings remaining) was estimated with an RMSPE = 2.296. The Mean Absolute Error of the final prediction model indicated that growth potential could be predicted with an error of ± 1.86 doublings remaining. Conclusions: This non-invasive methodology enabled the in-depth characterisation of hBM-MSCs from a single assay. This approach is advantageous for clinical applications as well as research and stands out for the characterisation of both present status as well as future behaviour. The use of data from five MSC lines with heterogenous AFMI profiles supports potential generalisability. [ABSTRACT FROM AUTHOR]

Herein, triangular‐lattice nanopillar templates are fabricated on sputter‐deposited AlN/Si (111) substrates. Nanotemplate selective‐area growth via radiofrequency‐plasma‐assisted molecular beam epitaxy is employed to grow GaN nanocolumns on the nanopillars. Well‐ordered uniform GaN nanocolumn arrays are obtained by inserting a migration‐enhanced‐epitaxy grown AlN/AlGaN buffer layer, thereby aligning the polarity of GaN to Ga‐polar. Subsequently, bulk InGaN active layers are grown on top of the GaN nanocolumns with increasing growth time (tg = 10–20 min). In the initial stage of growth (tg = 10 min), low‐In‐content InGaN grows on the edges of the six‐sided pyramidal top of the GaN nanocolumns. As the growth progresses, low‐In‐composition InGaN fills the sides between InGaN on the edges, while high‐In‐composition InGaN rapidly grows on the top of the c‐plane nanocolumns. High‐angle annular dark‐field scanning transmission electron microscopy reveals the formation of an InGaN core, covered with a low‐In‐composition InGaN shell, on the top of the nanocolumns. At tg = 20 min, the photoluminescence spectrum exhibits a peak at 669 nm with a full width at half maximum value of 51.7 nm. Thus, the proposed method is suitable for growing red‐light‐emitting well‐ordered InGaN/GaN nanocolumn arrays on Si. [ABSTRACT FROM AUTHOR]

In this study, the oxidation of Ga–polar GaN(0001) surface simulated by using originally developed charge‐transfer‐type interatomic potential is reported on. The adjusted potential parameters reproduce the cohesive energies in the range of 0.3 eV atom−1 and atomic forces with correlation coefficient as high as 0.9, compared to the results of first‐principles calculations for more than 9000 structures associated with oxidation of GaN. The oxidation simulations reveal the formation of a periodic gallium oxide (GaOx) layer grown on GaN(0001) with O atoms replacing N atoms. The atomic distance between Ga–Ga in the GaOx layer along GaN[0001] direction is 3.05 Å, which is longer than wurtzite GaN (2.63 Å) and is quantitatively in agreement with the recent photoelectron holography measurement. The distances of the Ga atoms projected onto the GaN(11–20) plane are determined to be 3.19 Å for the GaOx layer and 2.79 Å for the interfacial GaN. These distances also align quantitatively with the scanning transmission electron microscopy imaging of the native oxide on GaN(0001). Further oxidation simulation in a larger model of 2304 atoms suggests the formation of the layered structure even in the subsequent layers away from the interface of GaN and gallium oxide. [ABSTRACT FROM AUTHOR]

Controlling the hierarchical self-assembly of surfactants in aqueous solutions has drawn much attention due to their broad range of applications, from targeted drug release, preparation of smart material, to biocatalysis. However, the synthetic procedures for surfactants with stimuli-responsive hydrophobic chains are complicated, which restricts the development of surfactants. Herein, a novel single-tailed responsive surfactant, 1-methyl-3-(2-(4-((tetradecylimino) methyl) phenoxy) ethyl)-3-imidazolium bromides (C14PMimBr), was facilely fabricated in situ by simply mixing an aldehyde-functionalized imidazolium cation (3-(2-(4-formylphenoxy) ethyl)-1-methyl imidazolium bromide, BAMimBr) and aliphatic amine (tetradecylamine, TDA) through dynamic imine bonding. With increasing concentration, micelles, vesicles, and hydrogels were spontaneously formed by the hierarchical self-assembly of C14PMimBr in aqueous solutions without any additives. The morphologies of vesicles and hydrogels were characterized by cryogenic transmission electron microscopy and scanning electron microscopy. The mechanical properties and microstructure information of hydrogels were demonstrated by rheological measurement, X-ray diffraction, and density functional theory calculation. In addition, the vesicles could be disassembled and reassembled with the breakage and reformation of imine bonds by adding acid/bubbling CO2 and adding alkali. This work provides a simple method for constructing stimuli-responsive surfactant systems and shows great potential application in targeted drug release, drug delivery, and intelligent materials. [ABSTRACT FROM AUTHOR]

Herein, integrating GaN quantum dots (QDs) within a resonant cavity is focused on. Utilizing metal‐organic vapor phase epitaxy, controlled growth of GaN QDs on AlN is achieved. A deep‐UV distributed Bragg reflector (DBR) with high reflectivity in the 250–300 nm range, using AlN and Al0.7Ga0.3N layers to maximize refractive index contrast, is developed. A 50‐period DBR achieves 98% reflectivity at a wavelength of 272 nm. Scanning transmission electron microscopy and electron energy loss spectroscopy analyses reveal a trisection of DBR periods, attributed to a Ga composition pulling effect during growth. The real structure's reflectivity is simulated and matched well with measured data, though actual reflectivity is lower than the ideal. Cathodoluminescence studies at T = 17 K show emission peaks from both the DBR and the GaN QDs. Further, single‐photon emission is demonstrated with a g(2)(t = 0) value of 0.41 at 272.7 nm, confirming the potential for deep‐UV single‐photon sources. Additionally, the creation of a planar resonant cavity with enhanced emission intensity and vertical nanopillar structures with an aspect ratio of 11 and a diameter of 400 nm confirm the successful integration of GaN QDs in advanced UV photonic structures. [ABSTRACT FROM AUTHOR]

Integrating epitaxial BaTiO3 (BTO) with Si is essential for leveraging its ferroelectric, piezoelectric, and nonlinear optical properties in microelectronics. Recently, heterogeneous integration approaches that involve growth of BTO on ideal substrates followed by transfer to a desired substrate show promise of achieving excellent device‐quality films. However, beyond simple demonstrations of the existence of ferroelectricity, robust devices with high endurance are not yet demonstrated on Si using the latter approach. Here, using a novel two‐step approach to synthesize epitaxial BTO using pulsed laser deposition on water‐soluble Sr3Al2O6 (on SrTiO3 substrates), successful integration of high‐quality BTO capacitors on Si is demonstrated, with remanent polarisation Pr = 7 µC cm−2, coercive field Ec = 150 kV cm−1, ferroelectric and electromechanical endurance of > 106 cycles. The study further addresses the challenge of cracking and disintegration of thicker films by first transferring a large area (5 mm x 5 mm) of the templated layer of BTO (≈30 nm thick) on the desired substrate, followed by the growth of high‐quality BTO on this substrate, as revealed by high‐resolution X‐ray diffraction (HRXRD) and high‐resolution scanning transmission electron microscopy (HRSTEM) measurements. These templated Si substrates offer a versatile platform for integrating any epitaxial complex oxides with diverse functionalities onto any inorganic substrate. [ABSTRACT FROM AUTHOR]

Adsorptive fractionation and oxidation of dissolved organic matter (DOM) on manganese (Mn) oxide surfaces alter the molecular composition and stability of DOM, but the impact of iron (Fe) oxides on the coupled adsorption-oxidation processes of DOM by Mn oxides is largely unknown. In this study, the underlying mechanisms of molecular transformation of DOM on birnessite (Bir) in the presence of ferrihydrite (Fh), with varying Fh/Bir mass ratios, were investigated at both molecular levels and microscopic scales with a suite of characterization techniques, including Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) and spherical aberration corrected scanning transmission electron microscopy (Cs-STEM). We found that higher Fh/Bir mass ratio impeded the adsorption of DOM by birnessite and the reductive dissolution of birnessite to release dissolved Mn, and the impediment on the reductive dissolution of birnessite was proportional to Fh/Bir mass ratio. Overall, during the interactions of DOM with ferrihydrite and birnessite, phenolic compounds were preferentially adsorbed by Fe and Mn minerals, and compounds with higher oxygen contents and polymeric substances were formed. FT-ICR-MS analysis further suggested that higher Fh/Bir mass ratio inhibited the occurrence of aromatic ring-opening and carboxylation of substituted groups on aromatic rings, but promoted polymerization of phenolic compounds. Cs-STEM analysis revealed that DOM distributions on ferrihydrite, birnessite, and their mixtures were regulated by their microscopic structures and reactivity. Compared with aromatic carbon (C), carboxylic and phenolic C were more likely to associate with birnessite. Our results highlighted the significance of organo-mineral associations with the mixed minerals in regulating the distribution and reactivity of organic C. This study has provided molecular evidences for molecular transformation of DOM mediated by both Mn and Fe oxides, which contributed to advancing our understanding on coupled reactions of organic C at the mineral–water interfaces in the environment. [ABSTRACT FROM AUTHOR]

The article focuses on the preparation of transmission electron microscopy (TEM) specimens using a focused ion beam (FIB) system, highlighting the advantages of plan view specimens for device failure analysis. Topics include the benefits of plan view over cross-section configurations, the use of Xe plasma FIB for efficient specimen preparation, and a study investigating phase transformation in GeTe-based phase change memory devices through plan view TEM imaging.

The article focuses on the role of ptychography in enhancing four-dimensional scanning transmission electron microscopy (4D-STEM) by recovering lost phase information. Topics include the principles of ptychography and its computational imaging techniques, the methodology for acquiring and processing electron scattering data, and the comparison of focused versus defocused electron probes for optimizing imaging resolution and throughput.

In this research, a novel Fe3O4@Ti3C2 MXene nanocomposite was prepared by a simple ultrasonic method by combining Ti3C2 MXene and Fe3O4 nanoparticles, and was used for the remediation of malachite green (MG) dye, as an example of an organic pollutant, from the environment through photocatalytic degradation under visible light irradiation. A wide variety of techniques were used to characterize the synthesized Fe3O4@Ti3C2 MXene nanohybrid, including X-ray diffraction analysis (XRD), surface area analysis, scanning and transmission electron microscopy (SEM and TEM), and Fourier transform infrared spectroscopy (FTIR) in addition to the optical properties and band gap analysis. The results showed that the Ti3AlC2 MAX phase's Al layer was successfully selectively etched, resulting in the two-dimensional layered Ti3C2 MXene (average diameter of 78 nm). Additionally, the results revealed the preparation of the cubic Fe3O4 phase (average particle size of 11 nm), which was distributed homogeneously on the Ti3C2 MXene surface, as indicated by XRD, SEM, and TEM analysis. Moreover, the Fe3O4@Ti3C2 MXene nanophotocatalyst exhibits good visible light absorption ability under visible light (> 420 nm) due to its huge surface area, excellent conductivity, and sufficient quantity of active sites, and the accessibility of all elements required for effective photocatalysis. Accordingly, under 300 min of visible light exposure, the Fe3O4@Ti3C2 MXene nanophotocatalyst successfully photodegraded MG dye more efficiently than the pure MXene with a removal percentage of 95.4% with 0.5 g/L loading. Overall, the current study has shown that the Fe3O4@Ti3C2 MXene nanophotocatalyst has the potential to be a valuable photocatalyst for exceptionally efficient wastewater treatment applications. [ABSTRACT FROM AUTHOR]

Radiotherapy (RT), which is a therapeutic treatment modality that is commonly used for cancer, employs high‐energy irradiation to induce the generation of reactive oxygen species (ROS) and to cause DNA damages. Nevertheless, the therapeutic efficacy of RT is predominantly constrained due to inadequate DNA damage in malignancies and deleterious impacts on healthy tissues. In the current study, bovine serum albumin (BSA)–coated AgBiS2 nanodots, also known as AgBiS2@ BSA nanodots, were developed for enhanced breast cancer treatment. This was accomplished by the use of an extremely simple and eco‐friendly method. Both scanning transmission electron microscopy (STEM) and scanning electron microscopy (SEM) images revealed that prepared nanoradiosensitizers, AgBiS2@ BSA, were spherical in shape and uniformly distributed. AgBiS2@ BSA nanodots possessed excellent biocompatibility and exhibit excellent monodispersity as well. Furthermore, in vitro assays such as MTT, colony formation assay, and intracellular ROS generation assay revealed the significant cell inhibitory impact of the produced AgBiS2@ BSA nanodots under X‐ray irradiation under X‐ray irradiation. Remarkably, the combined administration of AgBiS2@ BSA nanodots along with X‐ray irradiation increased ROS level within cells by increasing the localized radiation dosage and improving the anti‐tumor effectiveness of RT. [ABSTRACT FROM AUTHOR]

We report room‐temperature bulk plasticity mediated by dislocations in single‐crystal cubic potassium tantalate oxide (KTaO3), contrasting the conventional knowledge that single‐crystal KTaO3 is susceptible to brittle fracture. A mechanics‐based combinatorial experimental approach using cyclic Brinell indentation, scratching, and uniaxial bulk compression consistently demonstrates room‐temperature dislocation plasticity in KTaO3 from the mesoscale to the macroscale. This approach also delivers tunable dislocation densities and plastic zone size. Scanning transmission electron microscopy analysis underpins the activated slip system to be <110> {11¯$\bar{1}$0}. Given the growing significance of KTaO3 as an emerging electronic oxide and the increasing interest in dislocations for tuning the physical properties of oxides, our findings are expected to trigger synergistic research interest in KTaO3 with tunable dislocation densities. [ABSTRACT FROM AUTHOR]