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At least 55 records · Page 3

Multimodal characterization of Te inclusions in Cd 1−x Zn x Te and Cd 1−x Zn x Te 1−y Se y for gamma and X-ray detectors

While CdZnTe (CZT) and CdZnTeSe (CZTS) semiconductors have emerged as compounds for room-temperature gamma and X-ray detection materials, they continue to be constrained by the formation of Te-inclusion defects generated during the growth and post-growth phases of the material, which adversely affect the detector performance. We demonstrate the utility of multimodal microscopic imaging and analysis for the characterization of the optical and electronic properties of Te inclusions in CZT and CZTS crystals at both micron and nanometer length scales. Having first identified regions with micron-scale Te inclusions using confocal Raman microscopy techniques, optically coupled infrared scattering near-field optical microscopic mapping was performed to map the distribution of these inclusions with nanometer spatial resolution and correlate the presence of Te inclusions in the matrix with other properties. Kelvin probe force microscopy was then utilized to characterize the variations of the work function associated with the presence of Te inclusions. Here, we observe an increase of ~ 240 mV in the work function associated with Te inclusions compared to the bulk CZT/CZTS crystals. Additionally, we observe that individual bulk grains in CZT can exhibit slight potential variations. Our findings develop a portrait of the charge trapping mechanisms in CZT and CZTS that act to degrade detector performance, while the demonstration of these combined microscopy techniques provides a new analytical tool that can be utilized for further optimization of the detector performance for these semiconducting compounds.

36 MATERIALS SCIENCE

A metastable pentagonal 2D material synthesized by symmetry-driven epitaxy

Most two-dimensional (2D) materials experimentally studied so far have hexagons as their building blocks. Only a few exceptions, such as PdSe 2 , are lower in energy in pentagonal phases and exhibit pentagons as building blocks. Although theory has predicted a large number of pentagonal 2D materials, many of these are metastable and their experimental realization is difficult. Here, in this paper, we report the successful synthesis of a metastable pentagonal 2D material, monolayer pentagonal PdTe 2 , by symmetry-driven epitaxy. Scanning tunnelling microscopy and complementary spectroscopy measurements are used to characterize this material, which demonstrates well-ordered low-symmetry atomic arrangements and is stabilized by lattice matching with the underlying Pd(100) substrate. Theoretical calculations, along with angle-resolved photoemission spectroscopy, reveal monolayer pentagonal PdTe 2 to be a semiconductor with an indirect bandgap of 1.05 eV. Our work opens an avenue for the synthesis of pentagon-based 2D materials and gives opportunities to explore their applications such as multifunctional nanoelectronics.

interfaces

Nanoscale Quantum Imaging of Field-Free Deterministic Switching of a Chiral Antiferromagnet

Recently, unconventional spin-orbit torques (SOTs) with tunable spin generation have opened new pathways for designing novel magnetization control for cutting-edge spintronics innovations. A leading research thrust is to develop field-free deterministic magnetization switching for implementing scalable and energy favorable magnetic recording and storage, which have been demonstrated in conventional ferromagnetic and antiferromagnetic material systems. Here, in this work, we extend this advanced magnetization control strategy to chiral antiferromagnet Mn 3 ⁢Sn using spin currents with out-of-plane canted polarization generated from low-symmetry van der Waals (vdW) material WTe 2 . Numerical calculations suggest that dampinglike SOT of spins injected perpendicular to the kagome plane of Mn 3⁢ Sn serves as a driving force to rotate the chiral magnetic order, while the fieldlike SOT of spin currents with polarization parallel to the kagome plane provides the bipolar deterministicity to the magnetic switching in the absence of an external magnetic field. We further introduce scanning quantum microscopy to visualize nanoscale evolutions of Mn 3 ⁢Sn magnetic domains during the field-free switching process, corroborating the exceptionally large magnetic switching ratio up to 90%. Our results highlight the opportunities provided by hybrid SOT material platforms consisting of noncollinear antiferromagnets and low-symmetry vdW spin source materials for developing next-generation spintronic logic devices.

2-dimesional systems

Origin of reduced efficiency in GaN-based micro-LEDs studied by scanning near-field optical microscopy

The quantum efficiency of micro-light emitting diodes (micro-LEDs) is lower than that of large area LEDs. This efficiency reduction is typically attributed to the nonradiative Shockley–Read–Hall recombination at the surface defects and current leakage through the sidewall region without a clear distinction between these effects. In this work, we attempt to find out which of these phenomena is most critical for the reduced efficiency of micro-LEDs. This has been done by mapping electroluminescence (EL) and photoluminescence (PL) and measuring PL dynamics in blue GaN micro-LEDs fabricated by dry etching. It has been found that in the as-etched device, the EL intensity is much lower than in devices with KOH etching and atomic layer deposition of SiO 2 . This effect is especially pronounced close to the sidewalls. On the other hand, PL decay times are similar in as-etched and passivated devices, both in their center and at the sidewalls. This allows concluding that the main mechanism of the reduced efficiency of micro-LEDs fabricated by dry etching is the current leakage in the sidewall region and not the nonradiative recombination. The KOH etching has been found to be the most efficient means to eliminate the current leakage.

36 MATERIALS SCIENCE

Quantifying Twist Angles in Cuprate Heterostructures with Anisotropic Raman Signatures

Artificially engineered twisted van der Waals (vdW) heterostructures have unlocked new pathways for exploring emergent quantum phenomena and strongly correlated electronic states. Many of these phenomena are highly sensitive to the twist angle, which can be deliberately tuned to tailor the interlayer interactions. This makes the twist angle a critical tunable parameter, emphasizing the need for precise control and accurate characterization during device fabrication. In particular, twisted cuprate heterostructures based on Bi 2 Sr 2 CaCu 2 O 8 + x (BSCCO) have demonstrated angle-dependent superconducting properties, positioning the twist angle as a key tunable parameter. However, the twisted interface is highly unstable under ambient conditions and vulnerable to damage from conventional characterization tools such as electron microscopy or scanning probe techniques. In this work, a fully non-invasive, polarization-resolved Raman spectroscopy approach is introduced for determining twist angles in artificially stacked BSCCO heterostructures. By analyzing twist-dependent anisotropic vibrational Raman modes, particularly utilizing the out-of-plane A 1g vibrational mode of Bi/Sr at ≈116 cm −1 , clear optical fingerprints of the rotational misalignment between cuprate layers are identified. The high-resolution confocal Raman setup, equipped with polarization control and RayShield filtering down to 10 cm −1 , allows for reliable and reproducible measurements without compromising the material's structural integrity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Direct Exfoliation of Nanoribbons from Bulk van der Waals Crystals

Confinement of monolayers into quasi-1D atomically thin nanoribbons could lead to novel quantum phenomena beyond those achieved in their bulk and monolayer counterparts. However, current experimental availability of nanoribbon species beyond graphene is limited to bottom-up synthesis or lithographic patterning. Here, in this study, a versatile and direct approach is introduced to exfoliate bulk van der Waals crystals as nanoribbons. Akin to the Scotch tape exfoliation method for producing monolayers, this technique provides convenient access to a wide range of nanoribbons derived from their corresponding bulk crystals, including MoS 2 , WS 2 , MoSe 2 , WSe 2 , MoTe 2 , WTe 2 , ReS 2 , and hBN. The nanoribbons are predominantly monolayer, single-crystalline, parallel-aligned, flat, and exhibit high aspect ratios. The role of confinement, strain, and edge configuration of these nanoribbons is observed in their electrical, magnetic, and optical properties. This versatile exfoliation technique provides a universal route for producing a variety of nanoribbon materials and supports the study of their fundamental properties and potential applications.

2D materials

Evidence of a distinct collective mode in Kagome superconductors

The collective modes of the superconducting order parameter fluctuation can provide key insights into the nature of the superconductor. Recently, a family of superconductors has emerged in non-magnetic kagome materials AV 3 Sb 5 (A = K, Rb, Cs), exhibiting fertile emergent phenomenology. However, the collective behaviors of Cooper pairs have not been studied. Here, we report a distinct collective mode in CsV 3-x Ta x Sb 5 using scanning tunneling microscope/spectroscopy. The spectral line-shape is well-described by one isotropic and one anisotropic superconducting gap, and a bosonic mode due to electron-mode coupling. With increasing x, the two gaps move closer in energy, merge into two isotropic gaps of equal amplitude, and then increase synchronously. The mode energy decreases monotonically to well below 2Δ and survives even after the charge density wave order is suppressed. We propose the interpretation of this collective mode as Leggett mode between different superconducting components or the Bardasis-Schrieffer mode due to a subleading superconducting component.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Dynamic control and quantification of active sites on ceria for CO activation and hydrogenation

Ceria (CeO 2 ) is a widely used oxide catalyst, yet the nature of its active sites remains elusive. This study combines model and powder catalyst studies to elucidate the structure-activity relationships in ceria-catalyzed CO activation and hydrogenation. Well-defined ceria clusters are synthesized on planar CeO 2 (111) and exhibit dynamic and tunable ranges of Ce coordination numbers, which enhance their interaction with CO. Reduced ceria clusters (e.g., Ce 3 O 3 ) bind CO strongly and facilitate its dissociation, while near-stoichiometric clusters (e.g., Ce 3 O 7 ) adsorb CO weakly and promote oxidation via carbonate formation. Unlike planar ceria surfaces, supported ceria clusters exhibit dynamic properties and enhanced catalytic activity, that mimic those of powder ceria catalysts. Insight from model studies provide a method to quantify active sites on powder ceria and guide further optimization of ceria catalysts for syngas conversion. This work marks a leap toward model-guided catalyst design and highlights the importance of site-specific catalysis.

03 NATURAL GAS

Integration of scanning probe microscope with high-performance computing: Fixed-policy and reward-driven workflows implementation

The rapid development of computation power and machine learning algorithms has paved the way for automating scientific discovery with a scanning probe microscope (SPM). The key elements toward operationalization of the automated SPM are the interface to enable SPM control from Python codes, availability of high computing power, and development of workflows for scientific discovery. Here, we build a Python interface library that enables controlling an SPM from either a local computer or a remote high-performance computer, which satisfies the high computation power need of machine learning algorithms in autonomous workflows. We further introduce a general platform to abstract the operations of SPM in scientific discovery into fixed-policy or reward-driven workflows. Furthermore, our work provides a full infrastructure to build automated SPM workflows for both routine operations and autonomous scientific discovery with machine learning.

47 OTHER INSTRUMENTATION

Properties of V-defect injectors in long wavelength GaN LEDs studied by near-field electro- and photoluminescence

The efficiency of multiple quantum well (QW) light emitting diodes (LEDs) to a large degree depends on uniformity of hole distribution between the QWs. Typically, transport between the QWs takes place via carrier capture into and thermionic emission out of the QWs. In InGaN/GaN QWs, the thermionic hole transport is hindered by the high quantum confinement and polarization barriers. To overcome this drawback, hole injection through semipolar QWs located at sidewalls of V-defects had been proposed. However, in the case of the V-defect injection, strong lateral emission variations take place. In this work, we explore the nature of these variations and the impact of the V-defects on the emission spectra and carrier dynamics. The study was performed by mapping electroluminescence (EL) and photoluminescence (PL) with a scanning near-field optical microscope in LEDs that contain a deeper well that can only be populated by holes through the V-defects. Applying different excitation schemes (electrical injection and optical excitation in the far- and near-field), we have shown that the EL intensity variations are caused by the lateral nonuniformity of the hole injection. We have also found that, in biased structures, the PL intensity and decay time in the V-defect regions are only moderately lower that in the V-defect-free regions thus showing no evidence of an efficient Shockley-–Read–Hall recombination. In the V-defect regions, the emission spectra experience a red shift and increased broadening, which suggests an increase of the In content and well width in the polar QWs close to the V-defects.

Electroluminescence

Impact of threading dislocations on the V-defect assisted lateral carrier injection and recombination in InGaN quantum well LEDs

The nonuniform hole distribution between InGaN quantum wells (QWs) of light emitting diodes (LEDs) has a negative impact on LED efficiency. The uniformity can be increased by using lateral hole injection through sidewalls of V-defects, which form at threading dislocations. However, the inherent coupling between the V-defects and dislocations might affect efficiency of the hole injection and nonradiative recombination. In this work, we have tested the possible impact of the dislocations on the injection and recombination by means of scanning near-field electroluminescence and photoluminescence spectroscopy on single green-emitting InGaN QW LEDs containing large (∼0.5 μm) V-defects. The measurements have not provided any evidence of a lower hole injection efficiency or enhanced nonradiative recombination at the dislocations located at the V-defect facets or their apexes. This shows that large V-defects are excellent volumetric injectors for long wavelength InGaN LEDs. Furthermore, it was established that V-defects are preferential hole injectors even in single quantum well devices. Compared to vertical injection, the V-defect injection allows lowering the operating voltage, which should contribute to an enhanced wall plug efficiency.

42 ENGINEERING

Nanoscale Imaging of Magnetotransport around a Circular 𝑝−𝑛 Junction in Graphene

Magnetoresistance studies of 2D systems are often shaped by the motion of electrons that occupy spatially confined wave functions, such as topological edge modes and disorder-induced bound states. Directly probing how such states form and behave in situ , under applied currents, provides a clear way of connecting microscopic physics to the macroscopic transport response. Here, in this Letter, scanning tunneling potentiometry is used to probe the local, current-induced electrochemical potential of carriers in graphene near circular 𝑝−𝑛 junctions in an out-of-plane magnetic field ranging from 0 to 1.4 T. These measurements provide detailed information about the motion of carriers at the nanometer scale, revealing how it evolves with increasing field. The electrochemical potential displays distinct patterns, such as dipoles, spirals, and concentric disks in weak, moderate, and high fields, respectively. The size and orientation of these patterns can be used to understand how local carrier dynamics change in different transport regimes as well as to directly extract physical parameters such as the electron mean free path and cyclotron diameter.

36 MATERIALS SCIENCE

Anomalous Superfluid Density in a Disordered Charge-Density-Wave Material: Pd-Intercalated ErTe 3

We image local superfluid density in single crystals of Pd-intercalated ErTe 3 below the superconducting critical temperature T c , well below the onset temperature T CDW of (disordered) charge-density-wave order. We find no detectable inhomogeneities on micron scales. Furthermore, we observe a rapid increase of the superfluid density below T c , deviating from the behavior expected in a conventional Bardeen-Cooper-Schrieffer superconductor, and show that the temperature dependence is qualitatively consistent with a combination of quantum and thermal phase fluctuations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Ultra-Low Disorder Graphene Quantum Dot-Based Spin Qubits for Cyber Secure Fossil Energy Infrastructure (Final Technical Report)

The overarching goal of the proposed project is to demonstrate the feasibility of creating ultralow local disorder graphene quantum dots (GQDs)-based high-speed, high-fidelity spin quantum bits (qubits) for extremely cyber-secure coal energy plants of the future. Despite their inherent benefits, the coherence times in the state-of-the-art GQD qubits are still low primarily due to the local disorder in GQD devices generated during lithographic fabrication of GQDs. Hence, the focus of this research is to prepare ultralow disorder GQDs (e.g., edge roughness ~0.5nm) and evaluate the low temperature (~mK) charge/spin transport characteristics of the engineered GQD qubit platform. To achieve minimal disorder in GQD qubits, we employ a novel approach that combines nanotomy (novel GQD fabrication technique developed by the PI) and scanning probe microscopy-atomic oxidation lithography (SPM-AOL).

20 FOSSIL-FUELED POWER PLANTS

Two-Dimensional Silk Crystal Films as Matrix Layer for High-Performance Microelectronics

This study explores a bio-inspired approach for memristive devices by combining Keggin-type polyoxometalates (POMs)-[SiW 12 O 40 ] 4 (POM-T) and [PW 12 O 40 ] 3 (POM-P), with silk fibroin (SF) to create 2D SF–POM layers on highly ordered pyrolytic graphite (HOPG) as resistive switching layers for memristors. We propose that the ordered SF layer template 0D POMs facilitate the formation of conductive filaments, thereby enhancing the variability of the manufactured memristors. AFM analysis revealed that both SF and SF–POM layers shared similar morphologies, while SF–POM–T formed larger aggregates, likely due to the stronger acidity of POM-T, which probably caused SF to aggregate and alter its secondary structure. Scanning Kelvin probe microscopy (SKPM) revealed that POMs reduced the contact potential difference of HOPG, resulting in lower work functions. Compared to an SF device, the SF–POM–P device showed improved memristive behavior, with a larger current gap and good repeatability over multiple sweeps; whereas the SF–POM–T device did not exhibit memristor activity, likely due to acidity-induced disruption of the SF template’s order and CF formation. More importantly, SF–POM–P devices also demonstrated programmable memristive states. Finally, combining simulation-driven memristor modeling, we showcase a co-design workflow for advancing bioinspired memristors through new materials design, synthesis, and device modeling and development.

36 MATERIALS SCIENCE

Hierarchical domain structures in buckled ferroelectric free sheets

Flat elastic sheets tend to display wrinkles and folds. From pieces of clothing down to two-dimensional crystals, these corrugations appear in response to strain generated by sheet compression or stretching, thermal or mechanical mismatch with other elastic layers, or surface tension. Extensively studied in metals, polymers and, — more recently — in van der Waals exfoliated layers, with the advent of thin single crystal freestanding films of complex oxides, researchers are now paying attention to novel microstructural effects induced by bending ferroelectric-ferroelastics, where polarization is strongly coupled to lattice deformation. Here we show that wrinkle undulations in BaTiO3 sheets bonded to a viscoelastic substrate transform into a buckle delamination geometry when transferred onto a rigid substrate. Using spatially resolved techniques at different scales (Raman, scanning probe and electron microscopy), we show how these delaminations in the free BaTiO3 sheets display a self-organization of ferroelastic domains along the buckle profile that strongly differs from the more studied sinusoidal wrinkle geometry. Moreover, we disclose the hierarchical distribution of a secondary set of domains induced by the misalignment of these folding structures from the preferred in-plane crystallographic orientations. Our results disclose the relevance of the morphology and orientation of buckling instabilities in ferroelectric free sheets, for the stabilization of different domain structures, pointing to new routes for domain engineering of ferroelectrics in flexible oxide sheets.

36 MATERIALS SCIENCE

Room-temperature spin injection across a chiral perovskite/III–V interface

Spin accumulation in semiconductor structures at room temperature and without magnetic fields is key to enable a broader range of optoelectronic functionality. Current efforts are limited owing to inherent inefficiencies associated with spin injection across semiconductor interfaces. Here we demonstrate spin injection across chiral halide perovskite/III-V interfaces achieving spin accumulation in a standard semiconductor III-V (Al x Ga 1-x ) 0.5 In 0.5 P multiple quantum well light-emitting diode. The spin accumulation in the multiple quantum well is detected through emission of circularly polarized light with a degree of polarization of up to 15 ± 4%. The chiral perovskite/III-V interface was characterized with X-ray photoelectron spectroscopy, cross-sectional scanning Kelvin probe force microscopy and cross-sectional transmission electron microscopy imaging, showing a clean semiconductor/semiconductor interface at which the Fermi level can equilibrate. Finally, these findings demonstrate that chiral perovskite semiconductors can transform well-developed semiconductor platforms into ones that can also control spin.

14 SOLAR ENERGY

Correlations Between In-Line X-ray Diffraction Data and In-Field Critical Current of Long, 4-μm Thick Film REBCO Tapes Made by Advanced MOCVD

REBa 2 Cu 3 O 7-δ (REBCO, RE = rare earth) tapes with high critical current can be very impactful in high magnetic field applications at low temperatures and power applications at high temperatures. A pilot-scale Advanced Metal Organic Chemical Vapor Deposition (MOCVD) method was used to fabricate 50-m-long, 4+μm-thick REBCO tape in a single pass. Critical currents 3.3x that of commercial HTS tapes were achieved at 20 K, 12 T in these 50-m-long tapes. An in-line 2D X-ray Diffraction (XRD) system has been used to assess the quality of the long tapes in real-time, during manufacturing. The key peaks of REBCO, REO, and BZO phases were identified and utilized for tape quality analysis. Furthermore, a 20-m tape made by Advanced MOCVD was tested over its entire length by reel-to-reel (R2R) scanning Hall-probe microscopy (SHPM) at 65 K, 0.25 T, 2 T, and 4 T. 4-mm-wide strands of Advanced MOCVD tapes showed mean critical currents at 65 K of 530 A, 200 A, and 104 A at 0.25 T, 2 T, and 4 T respectively. The combined use of in-line and offline characterization techniques provides a reliable approach for assessing long REBCO tapes during manufacturing, serving as an effective feedback source for quality control in scaled-up REBCO tape deposition processes. This advancement contributes to the production of longer and more uniform high-performance REBCO tapes for large-scale, high-field superconducting applications

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND