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At least 19 records

Multioutput Convolutional Neural Network for Improved Parameter Extraction in Time-Resolved Electrostatic Force Microscopy Data

Time-resolved scanning probe microscopy methods, like time-resolved electrostatic force microscopy (trEFM), enable imaging of dynamic processes ranging from ion motion in batteries to electronic dynamics in microstructured thin film semiconductors for solar cells. Reconstructing the underlying physical dynamics from these techniques can be challenging due to the interplay of cantilever physics with the actual transient kinetics of interest in the resulting signal. Previously, quantitative trEFM used empirical calibration of the cantilever or feed-forward neural networks trained on simulated data to extract the physical dynamics of interest. Both these approaches are limited by interpreting the underlying signal as a single exponential function, which serves as an approximation but does not adequately reflect many realistic systems. Here, we present a multi-branched, multi-output convolutional neural network (CNN) that uses the trEFM signal in addition to the physical cantilever parameters as input. The trained CNN accurately extracts parameters describing both single-exponential and bi-exponential underlying functions, and more accurately reconstructs real experimental data in the presence of noise. This article demonstrates an application of physics-informed machine learning to complex signal processing tasks, enabling more efficient and accurate analysis of trEFM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing the atomic dynamics of ultrafast melting with femtosecond electron diffraction

Melting is an every-day phase transition that is determined by thermodynamic parameters like temperature and pressure. In contrast, ultra-fast melting is governed by the microscopic response to a rapid energy input and, thus, can reveal the strength and dynamics of atomic bonds as well as the energy flow rate to the lattice. Accurately describing these processes remains challenging and requires detailed insights into transient states encountered. Here, we present data from femtosecond electron diffraction measurements that capture the structural evolution of copper during the ultrafast solid-to-liquid phase transformations. At absorbed energy densities 2-4 times the melting threshold, melting begins at the surface slightly below the nominal melting point followed by rapid homogeneous melting throughout the volume. Molecular dynamics simulations reproduce these observations and reveal a weak electron-lattice energy transfer rate for the given experimental conditions. Both simulations and experiments show no indications of rapid lattice collapse when its temperature surpasses proposed limits of superheating, providing evidence that the inherent dynamics limits the speed of disordering in ultrafast melting of metals.

FOS: Physical sciences↗

Keldysh tuning of photoluminescence in a lead halide perovskite crystal

In 1964, Keldysh laid the groundwork for strong-field physics in atomic, molecular, and solid-state systems by delineating a ubiquitous transition from multiphoton absorption to quantum electron tunneling under intense AC driving forces. While both processes in semiconductors can generate carriers and result in photon emission through electron-hole recombination, the low quantum yields in most materials have hindered direct observation of the Keldysh crossover. Leveraging the large quantum yields of photoluminescence in lead halide perovskites, we show that we can not only induce bright light emission from extreme sub-bandgap light excitation but also distinguish between photon-induced and electric-field-induced processes. Our results are rationalized by the Landau-Dykhne formalism, providing insights into the non-equilibrium dynamics of strong-field light-matter interactions. These findings open new avenues for light upconversion and sub-bandgap photon detection, highlighting the potential of lead halide perovskites in advanced optoelectronic applications.

FOS: Physical sciences↗

Prediction of L⁢i 3 ⁢F⁡e 8 ⁢B 8 compound with rapid one-dimensional ion diffusion channels

Using a computational crystal structure search in the Li-Fe-B ternary system, we predict a stable phase of L⁢i 3 ⁢F⁡e 8 ⁢B 8 , featuring 1D channels that enable rapid Li-ion transport. Ab initio molecular dynamics simulations show that the Li-ion diffusion coefficient in L⁢i 3 ⁢F⁡e 8⁢ B 8 surpasses that of common electrode and conductive additive materials by several orders of magnitude. The high diffusion in L⁢i 3 ⁢F⁡e 8 ⁢B 8 can be explained by the Frenkel–Kontorova model, which describes an incommensurate state between the Li diffusion chain and the periodic potential field caused by the FeB backbone structure. The favorable lithium-ion diffusivity and mechanical properties of L⁢i 3 ⁢F⁡e 8 ⁢B 8 make it a promising conductive additive for battery materials. Furthermore, an external magnetic field can further manipulate the properties of this material due to its predicted itinerant ferromagnetism, which also offers a platform for exploring spin-dependent phenomena.

1-dimensional systems↗

Distinguishing Thermal Fluctuations from Polaron Formation in Halide Perovskites

Recent angle-resolved photoelectron spectroscopy (ARPES) measurements of the hole effective mass in CsPbBr$_3$ revealed an enhancement of $\sim$50 % compared to the bare mass computed from first principles for CsPbBr$_3$ at $T = 0 K$. This large enhancement was interpreted as evidence of polaron formation. Employing accurate finite-temperature first-principles calculations, we show that the calculated hole effective mass of CsPbBr$_3$ at $T = 300 K$ can explain experimental results without invoking polarons. Thermal fluctuations are particularly strong in halide perovskites compared to conventional semiconductors such as Si and GaAs, and cannot be ignored when comparing with experiment. We not only resolve the debate on polaron formation in halide perovskites, but also demonstrate the general importance of including thermal fluctuations in first-principles calculations for strongly anharmonic materials.

36 MATERIALS SCIENCE↗

Tuning of altermagnetism by strain

For all collinear altermagnets, we sort out piezomagnetic free-energy invariants allowed in the nonrelativistic limit and relativistic piezomagnetic invariants bilinear in the Néel vector $\mathbf{L}$ and magnetization $\mathbf{M}$, which include strain-induced Dzyaloshinskii-Moriya interaction. The symmetry-allowed responses are fully determined by the nonrelativistic spin Laue group. In the nonrelativistic limit, two distinct mechanisms are discussed: the band-filling mechanism, which exists in metals and is illustrated using the simple two-dimensional Lieb lattice model, and the temperature-dependent exchange-driven mechanism, which is illustrated using first-principles calculations for transition-metal fluorides. The leading second-order nonrelativistic term in the strain-induced magnetization is also obtained for CrSb. Piezomagnetism due to the strain-induced Dzyaloshinskii-Moriya interaction is calculated from first principles for transition-metal fluorides, MnTe, and CrSb. Finally, we discuss triplet superconducting correlations supported by altermagnets and protected by inversion rather than time-reversal symmetry. We apply the nonrelativistic classification of Cooper pairs to describe the interplay between strain and superconductivity in the two-dimensional Lieb lattice and in bulk rutile structures. Here, we show that triplet superconductivity is, on average, unitary in an unstrained altermagnet, but becomes non-unitary under piezomagnetically active strain.

FOS: Physical sciences↗

Surface preparation method for investigating the three-dimensional electronic structure of perovskite nickelates

The investigation of the electronic structures on perovskite oxides using surface-sensitive spectroscopy techniques is often hindered by their “uncleavable” nature, typically requiring expensive and complex in situ experimental setups that integrate the capabilities of sample synthesis and spectroscopy measurement under ultrahigh vacuum condition. Here, we address this challenge by developing an ozone-annealing process that yields atomically flat surfaces on perovskite oxide thin films, making them suitable for high-resolution angle-resolved photoemission spectroscopy measurements. Using this method, we present a three-dimensional electronic structure study of Nd 1−𝑥 ⁢Sr 𝑥 ⁢NiO 3 (𝑥=0 and 0.175) thin films with unprecedented accuracy. The experimentally determined low-energy fermiology exhibits quantitative agreements with two-band tight-binding simulations, which is further validated by first-principles calculations considering the material's actual crystal structure. This work provides an accessible approach for ex situ ARPES measurements on perovskite oxides and other strongly correlated oxides, including the recently discovered high-𝑇 c nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measuring the Burgers vector of dislocations with dark-field X-ray microscopy

The subsurface dynamics of dislocations are essential to many properties of bulk crystalline materials. However, it is challenging to characterize a bulk crystal by conventional transmission electron microscopy (TEM) due to the limited penetration depth of electrons. A novel X-ray imaging technique – dark-field X-ray microscopy (DFXM) – was developed to image hierarchical dislocation structures in bulk crystals. While today's DFXM can effectively map the line structures of dislocations, it is still challenging to quantify the Burgers vectors, the key characterization governing the dislocation behaviors. Here, we extend the 'invisibility criterion' formalism from the TEM theory to the geometrical-optics model of DFXM and demonstrate the consistency between DFXM and dark-field TEM using multi-diffraction-peak imaging for a single edge dislocation. Due to the practical difficulty of multi-peak DFXM experiments, we further study how the Burgers vector effect is encoded for a single-peak DFXM experiment. Using the geometrical-optics DFXM simulation, we explore the asymmetry of rocking tilt scans at different rolling tilts and develop a new method to characterize the Burgers vector. The conclusions of this study advance our understanding of the use of DFXM in characterizing individual dislocations, enabling the connection from bulk DFXM imaging to dislocation mechanics.

36 MATERIALS SCIENCE↗

Discovery of spontaneous mesoscopic strain waves in nematic domains using dark-field x-ray microscopy

Electronic nematic order arises when correlated electrons spontaneously break the rotational symmetry of a crystal lattice. When electronic nematic order couples bilinearly to symmetry-breaking lattice strain, both appear together at a single ferroelastic phase transition, producing structural twin domains with distinct orientations of the nematic director. While the effects of applied strain on these domains are well established, the intrinsic behavior of spontaneous subdomain strain fields has remained unexplored. Here, we report the discovery of spontaneous mesoscopic strain waves within individual nematic domains of an iron-based superconductor, observed using dark-field x-ray microscopy (DFXM). Using this advanced full-field imaging technique, we visualize subdomain strain modulations emerging concurrently with nematic order. Elastic compatibility relations governing inhomogeneous strains provide a natural mechanism for the strain waves. Our findings reveal a broadly relevant form of strain self-organization and position DFXM as a powerful probe of the local interplay between lattice strain and electronic order.

36 MATERIALS SCIENCE↗

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic lengthscales. Our results provide direct evidence that ultrafast excitation of LaTe$_3$ leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

FOS: Physical sciences↗

Uniaxial stress effect on the electronic structure of quantum materials

Uniaxial stress has proven to be a powerful experimental tuning parameter for effectively controlling lattice, charge, orbital, and spin degrees of freedom in quantum materials. In addition, its ability to manipulate the symmetry of materials has garnered significant attention. Recent technical progress to combine uniaxial stress cells with quantum oscillation and angle-resolved photoemission techniques allowed to study the electronic structure as function of uniaxial stress. This review provides an overview on experimental advancements in methods and examines studies on diverse quantum materials, encompassing the semimetal WTe2, the unconventional superconductor Sr2RuO4, Fe-based superconductors, and topological materials.

FOS: Physical sciences↗

Reexamining Circular Dichroism in Photoemission From a Topological Insulator

The orbital angular momentum (OAM) of electron states is an essential ingredient for topological and quantum geometric quantities in solids. For example, Dirac surface states with helical spin- and orbital-angular momenta are a hallmark of a 3D topological insulator. Angle-resolved photoemission spectroscopy (ARPES) with variable circular light polarization, known as circular dichroism (CD), has been assumed to be a direct probe of OAM and, by proxy, of the Berry curvature of electronic bands in energy- and momentum-space. Indeed, topological surface states have been shown to exhibit angle-dependent CD (CDAD), and more broadly, CD is often interpreted as evidence of spin-orbit coupling. Meanwhile, it is well-established that CD originates from the photoemission matrix elements, which can have extrinsic contributions related to the experimental geometry and the inherently broken inversion symmetry at the sample surface. Therefore, it is important to broadly examine CD-ARPES to determine the scenarios in which it provides a robust probe of intrinsic material physics. We performed CD-ARPES on the canonical topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$ over a wide range of incident photon energies. Not only do we observe angle-dependent CD in the surface states, as expected, but we also find CD of a similar magnitude in virtually all bulk bands. Since OAM is forbidden by inversion symmetry in the bulk, we conclude this originates from symmetry-breaking in the photoemission process. Comparison with theoretical calculations supports this view and suggests that $\textit{hidden}$ OAM - localized to atomic sites within each unit cell - contributes significantly. Additional effects, including inter-atomic interference and final-state resonances, are responsible for the rapid variation of the CDAD signal with photon energy.

FOS: Physical sciences↗

Electronic structure of compressively strained thin film La$_2$PrNi$_2$O$_7$

The discovery of superconductivity in the bulk nickelates under high pressure is a major advance in physics. The recent observation of superconductivity at ambient pressure in compressively strained bilayer nickelate thin films has now enabled direct characterization of the superconducting phase through angle resolved photoemission spectroscopy (ARPES). Here we present an in-situ ARPES study of compressively strained La$_2$PrNi$_2$O$_7$ films grown by oxide molecular beam epitaxy, and the ozone treated counterparts with an onset T$_c$ of 40 K, supplemented with results from pulsed laser deposition films with similar T$_c$. We resolve a systematic strain-driven electronic band shift with respect to that of bulk crystals, in qualitative agreement with density functional theory (DFT) calculations. However, the strongly renormalized flat 3$d_{z2}$ band shifts a factor of 5-10 smaller than anticipated by DFT. Furthermore, it stays ~70 meV below the Fermi level, contradicting the expectation that superconductivity results from the high density of states of this band at the Fermi level. We also observed a non-trivial k$_z$ dispersion of the cuprate-like 3$d_{x2-y2}$ band. Combined with results from both X-ray diffraction and DFT, we suggest that the strained films are under ~5 GPa effective pressure, considerably larger than the naïve expectation from the DFT relaxed structure. Finally, the ~70 meV energy position is intriguingly close to the collective mode coupling more prominently seen in thin films, in the energy range of both oxygen related phonons and the maximum of the spin excitation spectrum.

FOS: Physical sciences↗

Magnetization Dependent In-plane Anomalous Hall Effect in a Low-dimensional System

Anomalous Hall Effect (AHE) response in magnetic systems is typically proportional to an out-of-plane magnetization component because of the restriction imposed by system symmetries, which demands that the magnetization, applied electric field, and induced Hall current are mutually orthogonal to each other. Here, we report experimental realization of an unconventional form of AHE in a low-dimensional heterostructure, wherein the Hall response is not only proportional to the out-of-plane magnetization component but also to the in-plane magnetization component. By interfacing a low-symmetry topological semimetal (TaIrTe4) with the ferromagnetic insulator (Cr2Ge2Te6), we create a low-dimensional magnetic system, where only one mirror symmetry is preserved. We show that as long as the magnetization has a finite component in the mirror plane, this last mirror symmetry is broken, allowing the emergence of an AHE signal proportional to in-plane magnetization. Our experiments, conducted on multiple devices, reveal a gate-voltage-dependent AHE response, suggesting that the underlying mechanisms responsible for the Hall effect in our system can be tuned via electrostatic gating. A minimal microscopic model constrained by the symmetry of the heterostructure shows that both interfacial spin-orbit coupling and time-reversal symmetry breaking via the exchange interaction from magnetization are responsible for the emergence of the in-plane AHE. Our work highlights the importance of system symmetries and exchange interaction in low-dimensional heterostructures for designing novel and tunable Hall effects in layered quantum systems.

FOS: Physical sciences↗

Second-order microscopic nonlinear susceptibility in a centrosymmetric material: application to imaging valence electron motion

We report measurements of phase-matched nonlinear x-ray and optical sum-frequency generation from single-crystal silicon using sub-resonant 0.95 eV laser pulses and 9.5 keV hard x-ray pulses from the LCLS free-electron laser. The sum-frequency signal appears as energy and momentum sidebands to the elastic Bragg peak. It is proportional to the magnitude squared of the relevant temporal and spatial Fourier components of the optically induced microscopic charges/currents. We measure the first- and second-order sideband to the 220 Bragg peak and find that the efficiency is maximized when the applied field is along the reciprocal lattice vector. For an optical intensity of $\sim10^{12} \text{W}/\text{cm}^2$, we measure peak efficiencies of $3\times 10^{-7}$ and $3\times 10^{-10}$ for the first and second-order sideband respectively (relative to the elastic Bragg peak). The first-order sideband is consistent with induced microscopic currents along the applied electric field (consistent with an isotropic response). The second-order sideband depends nontrivially on the optical field orientation and is consistent with an anisotropic response originating from induced charges along the bonds with C$_{3v}$ site symmetry. The results agree well with first-principles Bloch-Floquet calculations.

FOS: Physical sciences↗

Glassy interphases reinforce elastomeric nanocomposites by enhancing percolation-driven volume expansion under strain

For nearly a century, introduction of nanoparticles to elastomers has yielded extraordinarily tough nanocomposites that are critical to technologies from actuators to tires. The mechanisms by which this reinforcement occurs have nevertheless remained a central open question in material science. One widely debated hypothesis posits that strong interactions between polymer and particles induce "glassy bridges" that cement particles into a cohesive percolating network that resists elongation. Here, molecular dynamics simulations show that glassy particle shells do not primarily provide elongational cohesion. Instead, they amplify an underlying mechanism wherein competition between filler and elastomer networks causes the elastomer's volume to increase on deformation. This induces contributions from the elastomer's bulk modulus, which is of order 1000 times larger than its Young's modulus. These findings establish a unified understanding of low-strain reinforcement in filled elastomers as emanating from volumetric competition between coexisting particulate and elastomeric networks. This reframes and unifies our understanding of low-strain reinforcement, provides a clear-cut diagnostic for the presence of glassy bridging, and offers a new design principle for tough elastomeric nanocomposites.

Computational Physics (physics.comp-ph)↗

Synthesis of epitaxial TaO$_2$ thin films on Al$_2$O$_3$ by suboxide molecular-beam epitaxy and thermal laser epitaxy

Tantalum dioxide (TaO2) is a metastable tantalum compound. Here, we report the epitaxial stabilization of TaO2 on Al2O3 (1-102) (r-plane sapphire) substrates using suboxide molecular-beam epitaxy (MBE) and thermal laser epitaxy (TLE), demonstrating single-oriented, monodomain growth of anisotropically strained thin films. Microstructural investigation is performed using synchrotron X-ray diffraction and scanning transmission electron microscopy. The tetravalent oxidation state of tantalum is confirmed using X-ray absorption and photoemission spectroscopy as well as electron energy-loss spectroscopy. Optical properties are investigated via spectroscopic ellipsometry and reveal a 0.3 eV Mott gap of the tantalum 5d electrons. Density-functional theory and group theoretical arguments are used to evaluate the limited stability of the rutile phase and reveal the potential to unlock a hidden metal-insulator transition concomitant with a structural phase transition to a distorted rutile phase, akin to NbO2. Our work expands the understanding of tantalum oxides and paves the way for their integration into next-generation electronic and photonic devices.

FOS: Physical sciences↗

Ab Initio Many Body Quantum Embedding and Local Correlation in Crystalline Materials using Interpolative Separable Density Fitting

We present an efficient implementation of ab initio many-body quantum embedding and local correlation methods for infinite periodic systems through translational symmetry adapted interpolative separable density fitting, an approach which reduces the scaling of the calculations to only linear with the number of k-points. Employing this methodology, we compute correlated ground-state coupled cluster energies within density matrix embedding and local natural orbital correlation frameworks for both weakly and strongly correlated solids, using up to 1000 k-points. By extrapolating the local correlation domains and k-point sampling we further obtain estimates of the full coupled cluster with singles, doubles, and perturbative triples ground-state energies in the thermodynamic limit.

Chemical Physics (physics.chem-ph)↗