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At least 199 records · Page 11

Methanol carbonylation to acetaldehyde on Au particles supported by single-layer MoS 2 grown on silica

Homogenous single-layer MoS 2 films coated with sub-single layer amounts of gold are found to isolate the reaction of methanol with carbon monoxide, the fundamental step toward higher alcohols, from an array of possible surface reactions. Active surfaces were prepared from homogenous single-layer MoS 2 films coated with sub-single layer amounts of gold. These gold atoms formed clusters on the MoS2 surface. A gas mixture of carbon monoxide (CO) and methanol (CH 3 OH) was partially converted to acetaldehyde (CH 3 CHO) under mild process conditions (308 kPa and 393 K). This carbonylation of methanol to a C 2 species is a critical step toward the formation of higher alcohols. Density functional theory modeling of critical steps of the catalytic process identify a viable reaction pathway. Imaging and spectroscopic methods revealed that the single layer of MoS 2 facilitated formation of nanoscale gold islands, which appear to sinter through Ostwald ripening. Here, the formation of acetaldehyde by the catalytic carbonylation of methanol over supported gold clusters is an important step toward realizing controlled production of useful molecules from low carbon-count precursors.

2D catalyst↗

Stereoscopic detection of hot spots in superfluid 4 He (He II) for accelerator-cavity diagnosis

Superconducting radio-frequency (SRF) cavities cooled by superfluid 4He (He II) are building blocks of many modern particle accelerators due to their high quality factor. However, Joule heating from sub-millimeter surface defects on cavities can lead to cavity quenching, which limits the maximum acceleration gradient of the accelerators. Developing a non-contacting detection technology to accurately locate these surface hot spots is the key to improve the performance of SRF cavities and hence the accelerators. In a recent proof-of-concept experiment, we demonstrated that a molecular tagging velocimetry (MTV) technique based on the tracking of a He molecular tracer line created nearby a surface hot spot in He II can be utilized to locate the hot spot. In order to make this technique practically useful, here we describe our further development of a stereoscopic MTV setup for tracking the tracer line’s motion in three-dimensional (3D) space. We simulate a quench spot by applying a transient voltage pulse to a small heater mounted on a substrate plate. Images of the drifted tracer line, taken with two cameras from orthogonal directions, are used to reconstruct the line profile in 3D space. Here, a new algorithm for analyzing the 3D line profile is developed, which incorporates the finite size effect of the heater. We show that the center location of the heater can be reproduced on the substrate surface with an uncertainty of only a few hundred microns, thereby proving the practicability of this method.

43 PARTICLE ACCELERATORS↗

Imaging the Meissner effect in hydride superconductors using quantum sensors

By directly altering microscopic interactions, pressure provides a powerful tuning knob for the exploration of condensed phases and geophysical phenomena. Here, the megabar regime represents an interesting frontier, in which recent discoveries include high-temperature superconductors, as well as structural and valence phase transitions. However, at such high pressures, many conventional measurement techniques fail. Here we demonstrate the ability to perform local magnetometry inside a diamond anvil cell with sub-micron spatial resolution at megabar pressures. Our approach uses a shallow layer of nitrogen-vacancy colour centres implanted directly within the anvil; crucially, we choose a crystal cut compatible with the intrinsic symmetries of the nitrogen-vacancy centre to enable functionality at megabar pressures. We apply our technique to characterize a recently discovered hydride superconductor, CeH 9 . By performing simultaneous magnetometry and electrical transport measurements, we observe the dual signatures of superconductivity: diamagnetism characteristic of the Meissner effect and a sharp drop of the resistance to near zero. By locally mapping both the diamagnetic response and flux trapping, we directly image the geometry of superconducting regions, showing marked inhomogeneities at the micron scale. Our work brings quantum sensing to the megabar frontier and enables the closed-loop optimization of superhydride materials synthesis.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Real-space observation of ergodicity transitions in artificial spin ice

Abstract Ever since its introduction by Ludwig Boltzmann, the ergodic hypothesis became a cornerstone analytical concept of equilibrium thermodynamics and complex dynamic processes. Examples of its relevance range from modeling decision-making processes in brain science to economic predictions. In condensed matter physics, ergodicity remains a concept largely investigated via theoretical and computational models. Here, we demonstrate the direct real-space observation of ergodicity transitions in a vertex-frustrated artificial spin ice. Using synchrotron-based photoemission electron microscopy we record thermally-driven moment fluctuations as a function of temperature, allowing us to directly observe transitions between ergodicity-breaking dynamics to system freezing, standing in contrast to simple trends observed for the temperature-dependent vertex populations, all while the entropy features arise as a function of temperature. These results highlight how a geometrically frustrated system, with thermodynamics strictly adhering to local ice-rule constraints, runs back-and-forth through periods of ergodicity-breaking dynamics. Ergodicity breaking and the emergence of memory is important for emergent computation, particularly in physical reservoir computing. Our work serves as further evidence of how fundamental laws of thermodynamics can be experimentally explored via real-space imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nondestructive microstructural investigation of defects in 4H-SiC epilayers using a multiscale luminescence analysis approach

The development of metal oxide semiconductor field effect transistors (MOSFETs) utilizing epitaxially grown 4H-SiC has accelerated in recent years due to their favorable properties, including a high breakdown field, high saturated electron drift velocity, and good thermal conductivity. However, extended defects in epitaxial 4H-SiC can affect both device yields and operational lifetime. In this work, we demonstrate the importance of a multiscale luminescence characterization approach to studying nondestructively extended defects in epitaxial 4H-SiC semiconducting materials. Multiscale luminescence analysis reveals different aspects of excess charge carrier recombination behavior based on the scale of a particular measurement. Combining measurements of the same extended defect area at different scales tells us more about the essential nature of that defect and its microstructure. Here, we use photoluminescence imaging and cathodoluminescence spectrum imaging to investigate the recombination behavior of several different types of extended defects, including stacking faults, inclusions, and basal plane dislocations. A detailed understanding of the optoelectronic properties of extended defects in epitaxial SiC helps elucidate the microstructure of extended defects and can provide pathways to mitigate detrimental changes during device operation related to their evolution, such as the recombination enhanced dislocation glide effect that affects SiC-based MOSFETs.

3C-inclusion↗

Advances in machine-learning-based sampling motivated by lattice quantum chromodynamics

Sampling from known probability distributions is a ubiquitous task in computational science, underlying calculations in domains from linguistics to biology and physics. Generative machine-learning (ML) models have emerged as a promising tool in this space, building on the success of this approach in applications such as image, text, and audio generation. Often, however, generative tasks in scientific domains have unique structures and features—such as complex symmetries and the requirement of exactness guarantees—that present both challenges and opportunities for ML. This Perspective outlines the advances in ML-based sampling motivated by lattice quantum field theory, in particular for the theory of quantum chromodynamics. Enabling calculations of the structure and interactions of matter from our most fundamental understanding of particle physics, lattice quantum chromodynamics is one of the main consumers of open-science supercomputing worldwide. Here, the design of ML algorithms for this application faces profound challenges, including the necessity of scaling custom ML architectures to the largest supercomputers, but also promises immense benefits, and is spurring a wave of development in ML-based sampling more broadly. In lattice field theory, if this approach can realize its early promise it will be a transformative step towards first-principles physics calculations in particle, nuclear and condensed matter physics that are intractable with traditional approaches.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Discovery of orbital ordering in Bi 2 Sr 2 CaCu 2 O 8+x

The primordial ingredient of cuprate superconductivity is the CuO 2 unit cell. Theories usually concentrate on the intra-atom Coulombic interactions dominating the 3d 9 and 3d 10 configurations of each copper ion. However, if Coulombic interactions also occur between electrons of the 2p 6 orbitals of each planar oxygen atom, spontaneous orbital ordering may split their energy levels. This long-predicted intra-unit-cell symmetry breaking should generate an orbitally ordered phase, for which the charge transfer energy ε separating the 2p 6 and 3d 10 orbitals is distinct for the two oxygen atoms. Here we introduce sublattice-resolved ε(r) imaging to CuO 2 studies and discover intra-unit-cell rotational symmetry breaking of ε(r). Spatially, this state is arranged in disordered Ising domains of orthogonally oriented orbital order bounded by dopant ions, and within whose domain walls low-energy electronic quadrupolar two-level systems occur. Overall, these data reveal a Q = 0 orbitally ordered state that splits the oxygen energy levels by ~50 meV, in underdoped CuO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Artificial spin ice: Paths forward

Artificial spin ice systems are lithographically prepared arrays of interacting nanoscale magnetic moments with collective behavior resulting from the chosen array geometry. These many-body systems are unusual in that their simple constituent elements can be configured to design their interactions with exquisite control. They can then be probed experimentally over a remarkably large range of time scales and length scales, including imaging of the individual moments. The study of artificial spin ice has broadened well beyond the original focus on systems with connection to spin ice and ice models, and now the term is used in reference to many other structures that exhibit a much wider range of physical phenomena. Here in this perspective, we review progress in the field of artificial spin ice since its inception more than a decade ago. We then discuss prospects for future directions – continuing the exploration of nanomagnetism, statistical spin models, and the potential for technological devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Signatures of two-dimensional superconductivity emerging within a three-dimensional host superconductor

Significance We report signatures of a new phenomenon wherein a hidden “interdimensional” order emerges from a bulk three-dimensional superconductor tuned to approach a phase transition to an insulator. Prior electrical transport measurements found that the superconductor–insulator transition of BaPb 1− x Bi x O 3 demonstrated critical scaling behavior but inexplicably required parameters consistent only with two dimensions. Here, we directly image the three-dimensional superconducting state as it approaches an insulating phase and discover that signatures of a two-dimensional granular superconducting phase spontaneously emerge at the transition. Moreover, the properties of this phase precisely match the theory of emergent electronic granularity specific to two-dimensional materials. These findings posit that a three-dimensional superconductor electronically reorganizes itself into a two-dimensional granular superconductor before ultimately transforming to an insulator.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Evolution of ferroelastic domain walls during phase transitions in barium titanate nanoparticles

In this work, ferroelastic domain walls inside BaTiO 3 (BTO) tetragonal nanocrystals are distinguished by Bragg peak position and studied with Bragg coherent x-ray diffraction imaging (BCDI). Convergence-related features of the BCDI method for strongly phased objects are reported. A ferroelastic domain wall inside a BTO crystal has been tracked and imaged across the tetragonal-cubic phase transition and proves to be reversible. The linear relationship of relative displacement between two twin domains with temperature is measured and shows a different slope for heating and cooling, while the tetragonality reproduces well over temperature changes in both directions. An edge dislocation is also observed and found to annihilate when heating the crystal close to the phase transition temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Real Space Imaging of Spin Stripe Domain Fluctuations in a Complex Oxide

Understanding the formation and dynamics of charge and spin-ordered states in low-dimensional transition metal oxide materials is crucial to understanding unconventional high-temperature superconductivity. La 2-x Sr x NiO 4+δ (LSNO) has attracted much attention due to its interesting spin dynamics. Recent x-ray photon correlation spectroscopy studies have revealed slow dynamics of the spin order (SO) stripes in LSNO. Here, we applied resonant soft x-ray ptychography to map the spatial distribution of the SO stripe domain inhomogeneity in real space. The reconstructed images show the SO domains are spatially anisotropic, in agreement with previous diffraction studies. For the SO stripe domains, it is found that the correlation lengths along different directions are strongly coupled in space. Surprisingly, fluctuations were observed in the real space amplitude signal, rather than the phase or position. Overall, we attribute the observed slow dynamics of the stripe domains in LSNO to thermal fluctuations of the SO domain boundaries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Topological Magneto-optics in the Noncoplanar Antiferromagnet Co 1/3 ⁢NbS 2 : Imaging and Writing Chiral Magnetic Domains

Despite its tiny net magnetization, the antiferromagnetic (AFM) van der Waals material Co 1/3 ⁢NbS 2 exhibits a large transverse Hall conductivity 𝜎 𝑥⁢𝑦 even at zero applied magnetic field, which arises, as recently shown, from the topological nature of its noncoplanar “tetrahedral” AFM order. Here, this triple-𝐪 magnetic order can be regarded as the short-length-scale limit of a magnetic skyrmion lattice and has an intrinsic spin chirality. Here, we show, using optical wavelengths spanning the ultraviolet to infrared (400–1000 nm), that magnetic circular dichroism provides an incisive optical probe of the topological AFM order in Co 1/3 ⁢NbS 2 . Measurements as a continuous function of photon energy are directly compared with first-principles calculations, revealing the influence of the underlying quantum geometry on optical conductivity. Leveraging the power and flexibility of optical methods, we use scanning magnetic circular dichroism microscopy to directly image chiral AFM domains and demonstrate writing of chiral AFM domains.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dielectric Resonator Design for Low Power and Low Temperature Microwave Plasma

Waveguide-based microwave plasmas generally operate at high temperatures (2000 - 6000K)[1], making it difficult to directly interface solid materials with the plasma without significant thermal damage. Dielectric microwave resonators (DMRs), long studied for wave-based manipulation of electromagnetic radiation for telecom and optics, can focus radiation to extremely small mode volumes, creating intense localized fields with low-power input.[2] This phenomenon can be used for applications ranging from efficient plasma electronics to near-ambient plasma-materials interactions. Such DMR-based plasmas have been demonstrated a handful of times in the literature, but the majority of research towards this utilize the lowest frequency resonance mode.[3], [4], [5] By carefully controlling the geometry of cylindrical resonators, a variety of electromagnetic modes can be excited. In this work, COMSOL Multiphysics simulations are used to study the electric field enhancement and absorption properties of CaTiO3 DMRs as a function of geometry and excitation frequency. Whereas previous studies have utilized the HEM111 resonance frequency to drive low power plasma excitation, we find that higher order resonance frequencies are more effective at field enhancement and result in less power loss within the dielectric material, hence less wasted heating. The effectiveness of these modes is also geometry dependent and can be computationally optimized for plasma generation. Complementing these computational efforts, we demonstrate a new closed-system reactor design built in a WR-650 waveguide and experimentally demonstrate the formation of atmospheric argon microwave plasma using < 30 W input power on DMR dimers. We observe a shifting resonance frequency as the DMRs heat in response to microwave excitation and develop a Python-based lock-in mechanism to effectively track the DMR resonance over time, leading to stable plasma operation. We use infrared thermal imaging to monitor the temperature of the DMR dimers and surrounding quartz chamber, demonstrating thermal temperatures < 60 degreesC. Finally, we utilize optical emission spectroscopy (OES) to probe the plasma properties as a function of the resonance mode.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Overdriven-detonation states produced by spherically diverging waves

A series of experiments are currently underway at the Detonation Science and Technology group, within Los Alamos National Laboratory, to study the overdriven-detonation states achievable in energetic materials as a result of detonation-wave interactions. A multi-component, energetic-material array was designed to study the amplification of velocity and pressure states produced by spherically diverging detonation waves in pentaerythritol tetranitrate (PETN) output charges. The unique geometry provides a low-jitter, highly controlled series of interactions between three independent-detonation inputs. Streak-camera imaging was performed on the output face of PETN pellets ranging in thickness from 2.5 – 10 mm to characterize the resulting breakout profile. Additionally, photonic Doppler velocimetry (PDV) measurements were collected at the output-pellet surface to determine simultaneity within the system. Detonation-wave velocities upwards of 16 mm/µs were measured, as compared to a steady-state detonation velocity of 7.9 mm/µs for the PETN pressing density investigated. Finally, additional experiments are being conducted to measure the pressure amplification generated at key areas of interaction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Layer-Dependent Magnetism and Spin Fluctuations in Atomically Thin van der Waals Magnet CrPS 4

van der Waals (vdW) magnets, an emerging family of two-dimensional (2D) materials, have received tremendous attention due to their rich fundamental physics and significant potential for cutting-edge technological applications. In contrast to the conventional bulk counterparts, vdW magnets exhibit significant tunability of local material properties, such as stacking engineered interlayer coupling and layer-number dependent magnetic and electronic interactions, which promise to deliver previously unavailable merits to develop multifunctional microelectronic devices. As a further ingredient of this emerging topic, here we report nanoscale quantum sensing and imaging of atomically thin vdW magnet chromium thiophosphate CrPS 4 , revealing its characteristic layer-dependent 2D static magnetism and dynamic spin fluctuations. We also show a large tunneling magnetoresistance in CrPS 4 -based spin filter vdW heterostructures. Here, the excellent material stability, robust strategy against environmental degradation, in combination with tailored magnetic properties highlight the potential of CrPS 4 in developing state-of-the-art 2D spintronic devices for next-generation information technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Deep learning of interface structures from simulated 4D STEM data: cation intermixing vs. roughening ∗

Abstract Interface structures in complex oxides remain an active area of condensed matter physics research, largely enabled by recent advances in scanning transmission electron microscopy (STEM). Yet the nature of the STEM contrast in which the structure is projected along the given direction precludes separation of possible structural models. Here, we utilize deep convolutional neural networks (DCNN) trained on simulated 4D STEM datasets to predict structural descriptors of interfaces. We focus on the widely studied interface between LaAlO 3 and SrTiO 3 , using dynamical diffraction theory and leveraging high performance computing to simulate thousands of possible 4D STEM datasets to train the DCNN to learn properties of the underlying structures on which the simulations are based. We test the DCNN on simulated data and show that it is possible (with >95% accuracy) to identify a physically rough from a chemically diffuse interface and create a DCNN regression model to predict step positions. We quantify the applicability of the model to different thicknesses and the transferability of the approach. The method shown here is general and can be applied for any inverse imaging problem where forward models are present.

42 ENGINEERING↗

Evidence for chiral superconductivity on a silicon surface

Tin adatoms on a Si(111) substrate with a one-third monolayer coverage form a two-dimensional triangular lattice with one unpaired electron per site. These electrons order into an antiferromagnetic Mott-insulating state, but doping the Sn layer with holes creates a two-dimensional conductor that becomes superconducting at low temperatures. Although the pairing symmetry of the superconducting state is currently unknown, the combination of repulsive interactions and frustration inherent in the triangular adatom lattice opens up the possibility of a chiral order parameter. Here we study the superconducting state of Sn/Si(111) using scanning tunneling microscopy, scanning tunneling spectroscopy and quasiparticle interference imaging. Here we find evidence for a doping-dependent superconducting critical temperature with a fully gapped order parameter, the presence of time-reversal symmetry breaking and a strong enhancement in zero-bias conductance near the edges of the superconducting domains. Although each individual piece of evidence could have a more mundane interpretation, our combined results suggest the possibility that Sn/Si(111) is an unconventional chiral d-wave superconductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Compositional Control on Shale Pore Structure Characteristics across a Maturation Gradient: Insights from the Devonian New Albany Shale and Marcellus Shale in the Eastern United States

The pore structure characteristics of shales are controlled by their mineralogical and organic matter (OM) composition. However, the contributions by different components in shales at varying thermal maturities remain poorly understood. In this study, Devonian New Albany Shale and Marcellus Shale samples spanning a thermal maturity from marginally mature (vitrinite reflectance R o 0.55%) to post-mature (R o 2.41 %) were selected to study the control of composition on the pore structure properties of shales at different stages of thermal maturation. Scanning electron microscope (SEM) imaging was used to examine pore types in shales, and low-pressure N 2 and CO 2 adsorption analyses were used to quantitatively characterize the mesopore and micropore characteristics of bulk shales and major components in shales. The results show that matrix-associated pores including interparticle pores between silt-sized mineral grains, phyllosilicate framework pores, and intraparticle pores within mineral grains exist in all samples but become less common with increasing maturity, which is likely caused by elevated compaction, cementation, and occlusion with bitumen. Secondary organic pores were not observed under SEM at marginal maturity but were detected in the condensate–wet gas and dry gas windows, with more organic pores in the dry gas window. At marginal maturity, OM has large amounts of mesopores and micropores as demonstrated by low-pressure N 2 and CO 2 adsorption analyses of OM isolated from shales, even though no OM-hosted pores were observed under SEM. With increasing thermal maturity, the mesopore and micropore specific surface area of OM increase and make greater contributions to the pore structure properties of bulk shales. The mesopore and micropore properties of shales are controlled by OM content and maturity as well as by clay mineral type and content, and they can be estimated from the contribution of each component at different stages of thermal maturation. In conclusion, accurate evaluation of the pore volume and SSA of shales will have important implications for assessing gas adsorption and transport in shales.

03 NATURAL GAS↗