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The Raman active G mode in graphene exhibits strong coupling to electrons, yet the comprehensive treatment of this interaction in the calculation of its temperature-dependent Raman spectrum remains incomplete. In this study, we calculate the temperature dependence of the G mode frequency and linewidth, and successfully explain the experimental trend, by accounting for the contributions arising from the first-order electron-phonon coupling, electron-mediated phonon-phonon coupling, and standard lattice anharmonicity. The generality of our approach enables its broad applicability to study phonon dynamics in materials where both electron-phonon coupling and anharmonicity are important., Comment: 14 pages, 7 figures, SI included in "anc" folder

We have studied theoretically the specific heat of a large number of non-frustrated magnetic structures described by the Heisenberg model for systems with total angular momentum $J=7/2$, which corresponds to the 4f$^7$ configuration of Gd$^{+3}$ and Eu$^{+2}$. For a given critical temperature (controlled by the magnitude of the exchange interactions) we find that to a large accuracy, the specific heat is controlled by two parameters: the effective number of neighbors (which controls the importance of quantum fluctuations) and the axial anisotropy. Using these two parameters we fit the specific heat of four Gd compounds and two Eu compounds obtaining a remarkable agreement. Another Gd compound has been fitted previously. Our work opens the possibility of describing the specific heat of non-frustrated 4f$^7$ systems within a general framework., Comment: 20 pages, 6 figures

Ruthenium metal and its oxide stand out for their exceptional catalytic activity, stability in Oxygen Evolution Reactions (OER) and electrical conductivity, making them indispensable in electronics and electrocatalysis. In this study, atomic layer deposition (ALD) was used to synthesize ruthenium thin films, and the subsequent annealing of deposited ruthenium films at different elevated temperatures resulted in a progressive phase transformation from ruthenium metal to ruthenium dioxide (RuO2). The films were systematically characterized using atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and Raman spectroscopy. XPS was carried out with both soft X-rays from a lab-based instrument and tender X-rays from the synchrotron. The different probing depths of the techniques revealed the gradual transformation of Ru to RuO2 from the top surface as the annealing temperature was increased. The water adsorption behavior of the films was also assessed using ambient pressure XPS (APXPS) at different water vapor pressures. The influence of annealing conditions on the films affinity for water and tendency for water dissociation was analyzed to seek an initial understanding of the surface chemistry relevant to electrochemical water splitting.

Scanning probe microscopy (SPM) is a powerful technique for mapping nanoscale surface properties through tip-sample interactions. Thermal scanning-probe lithography (tSPL) is an advanced SPM variant that uses a silicon tip on a heated cantilever to sculpt and measure polymer films with nanometer precision. The surfaces produced by tSPL-smooth topographic landscapes-allow mathematically defined contours to be fabricated on the nanoscale, enabling sophisticated functionalities for photonic, electronic, chemical, and biological technologies. Evaluating the physical effects of a landscape requires fitting arbitrary mathematical functions to SPM datasets, however, this capability does not exist in standard analysis programs. Here, we provide an open-source software package (FunFit) to fit analytical functions to SPM data and develop a fabrication and characterization protocol based on this analysis. We demonstrate the benefit of this approach by patterning periodic and quasiperiodic landscapes in a polymer resist with tSPL, which we transfer to hexagonal boron nitride (hBN) flakes with high fidelity via reactive-ion etching. The topographic landscapes in polymers and hBN are measured with tSPL and atomic force microscopy (AFM), respectively. Within the FunFit program, the datasets are corrected for artefacts, fit with analytical functions, and compared, providing critical feedback on the fabrication procedure. Beyond application to tSPL, this protocol can improve analysis, reproducibility, and process development for a broad range of SPM experiments. The protocol can be performed within a working day by an inexperienced user, where fabrication and characterization take a few hours and software analysis takes a few minutes.

We employ ultrabroadband terahertz (THz) spectroscopy to expose the high-frequency transport properties of Dirac fermions in monolayer graphene. By controlling the carrier concentration via tunable electrical gating, both equilibrium and transient optical conductivities are obtained for a range of Fermi levels. The frequency-dependent equilibrium response is determined through a combination of time-domain THz and Fourier-transform infrared spectroscopy for energies up to the near-infrared, which also provides a measure of the gate-voltage dependent Fermi level. Transient changes in the real and imaginary parts of the graphene conductivity are electro-optically resolved for frequencies up to 15 THz after near-infrared femtosecond excitation, both at the charge-neutral point and for higher electrostatic-doping levels. Modeling of the THz response provides insight into changes of the carrier spectral weights and scattering rates, and reveals an additional broad-frequency ($\approx$ 8 THz) component to the photo-induced response, which we attribute to the zero-momentum mode of quantum-critical transport observed here in large-area CVD graphene.

Hard X-ray angle-resolved photoemission spectroscopy reveals significant alterations in the valence band states of EuPd$_2$Si$_2$ at a temperature $T_V$, where the Eu ions undergo a temperature-induced valence crossover from a magnetic Eu$^{2+}$ state to a low-temperature valence-fluctuating state. The introduction of small amounts of Au on Pd lattice sites and Ge on Si sites, respectively, results in a decrease in $T_V$ and the emergence of an antiferromagnetic state at low temperatures without valence fluctuations. It has been proposed that the boundary between AFM order and valence crossover represents a first-order phase transition associated with a specific type of second-order critical end point. In this scenario, strong coupling effects between fluctuating charge, spin, and lattice degrees of freedom are to be expected. In the case of EuPd$_2$(Si$_{1-x}$Ge$_x$)$_2$ with x=0.13, which is situated close to the critical end point, a splitting of conduction band states and the emergence of flat bands with one-dimensional character have been observed. A comparison with ab initio theory demonstrates a high degree of correlation with experimental findings, particularly in regard to the bands situated in proximity to the critical end point., Comment: 9 pages, 9 figures

Topological magnons give rise to possibilities for engineering novel spintronics devices with critical applications in quantum information and computation, due to its symmetry-protected robustness and low dissipation. However, to make reliable and systematic predictions about material realization of topological magnons has been a major challenge, due to the lack of neutron scattering data for most materials. In this work, we significantly advance the symmetry-based approach for identifying topological magnons through developing a fully automated algorithm, utilizing the theory of symmetry indicators, that enables a highly efficient and large-scale search for candidate materials hosting field-induced topological magnons. This progress not only streamlines the discovery process but also expands the scope of materials exploration beyond previous manual or traditional methods, offering a powerful tool for uncovering novel topological phases in magnetic systems. Performing a large-scale search over all 1649 magnetic materials in Bilbao Crystallographic Server with a commensurate magnetic order, we discover 387 candidate materials for topological magnons, significantly expanding the pool of topological magnon materials. We further discuss examples and experimental accessibility of the candidate materials, shedding light on future experimental realizations of topological magnons in magnetic materials., Comment: Main text: 30 pages with 2 tables + 12 figures. Supplementary materials: 945 pages with 900+ tables and 460+ figures

CMOS-based microelectronics are limited to ~150{\deg}C and therefore not suitable for the extreme high temperatures in aerospace, energy, and space applications. While wide bandgap semiconductors can provide high-temperature logic, nonvolatile memory devices at high temperatures have been challenging. In this work, we develop a nonvolatile electrochemical memory cell that stores and retains analog and digital information at temperatures as high as 600 {\deg}C. Through correlative electron microscopy, we show that this high-temperature information retention is a result of composition phase separation between the oxidized and reduced forms of amorphous tantalum oxide. This result demonstrates a memory concept that is resilient at extreme temperatures and reveals phase separation as the principal mechanism that enables nonvolatile information storage in these electrochemical memory cells., Comment: 19 pages, 4 figures

Bismuth has been shown to be topological in its different allotropes and compounds, with one of the most notable examples being the Bi-Sb alloy, the first 3D topological insulator ever discovered. In this paper we explore two-dimensional alloys of Bi and Sb, both crystalline and amorphous, to determine the critical concentrations that render the alloys topological. For the amorphous alloy, we determine the effect of structural disorder on its topological properties, remarkably observing a trivial to topological transition as disorder increases. The alloys are modelled using a Slater-Koster tight-binding model and the topological behaviour is assessed through the entanglement spectrum together with artificial neural networks. Additionally, we perform electronic transport calculations with results compatible with those of the entanglement spectrum, which, furthermore, reveal an insulator to metal transition in the highly disordered regime.

Magnetoelectric materials displaying strong magnetically induced polarization have attracted considerable interest due to their potential applications in spintronics and various fast electrically controlled magnetic devices. CaMn$_7$O$_{12}$ (CMO) stands out for its giant spin-induced ferroelectric polarization. However, the origin of the induced electric polarization in CMO remains highly controversial and continues to be a subject of ongoing debate. In this paper, through room temperature X-ray powder diffraction (XRPD), temperature-dependent magnetic susceptibility, and thermally stimulated depolarizing current (TSDC) measurements, we provide experimental evidence for a route to tune the magnetically induced polarization by modifying the exchange-striction in CMO via Sr-doping. Our findings demonstrate that the large and broad current peaks observed near the first magnetic phase transition ($T_N1 \sim 90$ K) indicate polarization contributions from both thermally stimulated depolarization current (TSDC) and intrinsic magnetically induced electric polarization. We suggest that this reduction in induced electric polarization in CMO originates from the increase in the Mn$^{3+}$ -- O -- Mn$^{4+}$ bond angle due to Sr$^{2+}$ doping, weakening the exchange-striction interaction. Meanwhile, the Dzyaloshinskii-Moriya (DM) effect determines the direction of the induced electric polarization. Our result sheds light on understanding the intriguing giant-induced polarization in CMO and similar compounds with complex magnetic structures.

This paper explores the mechanical behaviour of the composite materials used in modern lithium-ion battery electrodes. These contain relatively high modulus active particle inclusions within a two-component matrix of liquid electrolyte which penetrates the pore space within a viscoelastic polymer binder. Deformations are driven by a combination of (i) swelling/contraction of the electrode particles in response to lithium insertion/extraction, (ii) swelling of the binder as it absorbs electrolyte, (iii) external loading and (iv) flow of the electrolyte within the pores. We derive the macroscale response of the composite using systematic multiple scales homomgenisation by exploiting the disparity in lengthscales associated with the size of an electrode particle and the electrode as a whole. The resulting effective model accurately replicates the behaviour of the original model (as is demonstrated by a series of relevant case studies) but, crucially, is markedly {simpler and hence} cheaper to solve. This is significant practical value because it facilitates low-cost, realistic computations of the mechanical states of battery electrodes, thereby allowing model-assisted development of battery designs that are better able to withstand the mechanical abuse encountered in practice and ultimately paving the way for longer-lasting batteries., Comment: 46 pages, 19 figures

Perfect circular dichroism has been observed in the Raman scattering by the optical phonons in single chiral domain NiCo2TeO6 crystals. The selection rules for the optical phonons are determined by the combination of the chiral structure C and the electric polarization P along the c-axis. These two symmetry operations are equivalent to the ferroaxial order (C dot P) = A, so the observed optical phonons are referred to as "ferroaxial". For a given Raman scattering geometry the observed effect may also be described as a complete non-reciprocal propagation of the optical phonons, whose preferable vector direction is determined by the sign of C dot P. The combination of Raman scattering and polarization plane rotation of the transmitted white light allows for identification of the direction of electric polarization P in mono domain chiral crystals.

Ni particle coarsening is a primary degradation mechanism in Ni/YSZ solid oxide cells, limiting the lifespan of these devices. In this study, we demonstrate the use of Scanning 3D X-ray diffraction (S3DXRD) with an unprecedented spatial resolution of 100 nm, to monitor the microstructural evolution within the 3D volume of a solid oxide cell subjected to ex situ heat treatment. Unlike conventional tomography, S3DXRD combines crystallographic information with spatial maps, enabling precise identification of grain boundaries and the determination of local curvature changes in the Ni microstructure. Our study reveals that the Ni phase undergoes significant structural changes during annealing, driven by grain growth. This transformation is characterized by a reduction in local curvature, particularly in regions where grains disappear. We observe that the disappearing grains are the smallest grains in the size distribution and are often located near pores. As a result, the most notable reduction in local curvature occurs at the Ni-pore interface. The quantitative characterization of polycrystalline microstructural evolution in Ni/YSZ system provides new insights into the mechanisms of Ni particle coarsening in SOC devices, potentially guiding strategies to enhance the long-term stability of SOC devices.

Magneto-transport measurements of Pr$_4$Ni$_3$O$_{10}$ single crystals performed under externally applied pressures up to 73 GPa in diamond anvil cells with either KBr or Nujol oil as pressure media yield signatures of superconductivity with a maximum onset temperature of approximately 31 K. True zero resistance was not observed, consistent with a non-percolating superconducting volume fraction. Magnetization measurements provided corroborating evidence of superconductivity, with a pressure-dependent diamagnetic signal occurring below the onset temperature, and an estimate from the absolute value of the susceptibility suggests a superconducting volume fraction on the order of 10%. We observe sample-to-sample variations in the magnitude and pressure dependence of Tc as well as a dependence on the configuration of electrical contacts on a given sample. Possible causes of this behavior may be significant inhomogeneities in the pressure and/or damage to the samples induced by the pressure media as well as inhomogeneities in the crystals themselves. The results imply that our as-grown Pr$_4$Ni$_3$O$_{10}$ single crystals are not bulk superconductors but that there is a minority structure present within the crystals that is indeed superconducting.

The electrical response of ferroelectric domain walls is often influenced by their geometry underneath the sample surface. Tomographic imaging in these material systems has therefore become increasingly important for its ability to correlate the surface-level functional response with subsurface domain microstructure. In this context, AFM-based tomography emerges as a compelling choice because of its simplicity, high resolution and robust contrast mechanism. However, to date, the technique has been implemented in a limited number of ferroelectric materials, typically to depths of a few hundred nanometers or on relatively soft materials, resulting in an unclear understanding of its capabilities and limitations. In this work, AFM tomography is carried out in YbMnO3, mapping its complex domain microstructure up to a depth of around 1.8 um along with its current pathways. A model is presented, describing the impact of interconnected domain walls within the network, which act as current dividers and codetermine how currents distribute. Finally, challenges such as tip-blunting and subsurface amorphisation are identified through TEM studies, and strategies to address them are also put forward. This study highlights the potential of AFM tomography and could spur interest within the ferroics community for its use in the investigation of similar material systems.

Cu$_2$OSeO$_3$ is a multiferroic insulating chiral magnet which exhibits various magnetic orderings at different conditions. The positions of these magnetic phase transitions are known to be sensitive to chemical substitution. Here, we present a universality class analysis of the Cu$_2$OSe$_{1-x}$Te$_x$O$_3$ with $(0\leq x \leq 0.1)$. Tellurium is a non-magnetic ion which, upon substitution into the selenium positions of the structure, applies a positive chemical pressure and expands the crystal lattice. Our SANS and magnetometry data indicate that Te inclusion lowers the paramagnetic to helical ordering temperature and the critical field required for the conical to field polarised phase transition. By using the Heat-map Modified Iteration Method that evaluates critical behaviour on both sides of the transition, we show that the Heisenberg to Ising universality class transition of the initial ordering is robust to internal chemical pressure. Additionally, we attribute the decreases with doping in both critical temperature and critical field to be due to decreases in the strength of the Dzyaloshinskii-Moriya and Symmetric Exchange Interactions., Comment: 21 pages and 9 figures (Manuscript)

In this article, we present results of our recent work of epitaxially-grown aluminum (epi-Al) on antimonide heterostructures, where the epi-Al thin film is grown at either room temperature or below zero $^o$C. A sharp superconducting transition at $T \sim 1.3$ K is observed in these epi-Al films, and the critical magnetic field follows the BCS (Bardeen-Cooper-Schrieffer) model. We further show that supercurrent states are achieved in Josephson junctions fabricated in the epi-Al/antimonide heterostructures with mobility $\mu \sim 1.0 \times 10^6$ cm$^2$/Vs, making these heterostructures a promising platform for the exploration of Josephson junction effects for quantum microelectronics applications, and the realization of robust topological superconducting states that potentially allow the realization of intrinsically fault-tolerant qubits and quantum gates.

Direct numerical simulations of mechanical metamaterials are prohibitively expensive due to the separation of scales between the lattice and the macrostructural size. Hence, multiscale continuum analysis plays a pivotal role in the computational modeling of metastructures at macroscopic scales. In the present work, we assess the continuum limit of mechanical metamaterials via homogenized models derived rigorously from variational methods. It is shown through multiple examples that micropolar-type effective energies, derived naturally from analysis, properly capture the kinematics of discrete lattices in two and three dimensions. Moreover, the convergence of the discrete energy to the continuum limit is shown numerically. We provide open-source computational implementations for all examples, including both discrete and homogenized models., Comment: Accepted version

The determination of mechanical properties such as the Young's modulus provides an important means to compare classical molecular dynamics simulations with materials. In this respect, ultra-thin materials hold several challenges: their volume is ambiguous, and different methods to determine a stress-strain relation deliver different result in particular for disordered systems. Using the example of carbon nanomembranes we show that stress-strain simulations following experimental setups deliver correct results if adjusted carefully., Comment: 21 pages, 8 figures

Excitons dominate the optoelectronic response of many materials. Depending on the timescale and host material, excitons can exhibit free diffusion, phonon-limited diffusion, or polaronic diffusion, and exciton transport often limits the efficiency of optoelectronic devices such as solar cells or photodetectors. We demonstrate that topological excitons exhibit enhanced diffusion in all transport regimes. Appealing to notions of quantum geometry, we find that topological excitons are generically larger and more dispersive than their trivial counterparts, promoting their diffusion. We apply this general theory to a range of organic polyacene semiconductors, and show that exciton transport increases four-fold when topological excitons are present. We also propose that non-uniform electric fields can be used to directly probe the quantum metric of excitons, providing an experimental window into a basic geometric feature of quantum states. Our results provide a new avenue to enhance exciton transport and reveal that the mathematical ideas of topology and quantum geometry can be important ingredients in designing next-generation optoelectronic technologies.

Fabrication of semiconductor heterostructures is now so precise that metrology has become a key challenge for progress in science and applications. It is now relatively straightforward to characterize classic III-V and group IV heterostructures consisting of slabs of different semiconductor alloys with thicknesses of $\sim$5 nm and greater using sophisticated tools such as X-ray diffraction, high energy X-ray photoemission spectroscopy, and secondary ion mass spectrometry. However, profiling thin layers with nm or sub-nm thickness, e.g. atomically thin dopant layers ($\delta$-layers), of impurities required for modulation doping and spin-based quantum and classical information technologies is more challenging. Here, we present theory and experiment showing how resonant-contrast X-ray reflectometry meets this challenge. The technique takes advantage of the change in the scattering factor of atoms as their core level resonances are scanned by varying the X-ray energy. We demonstrate the capability of the resulting element-selective, non-destructive profilometry for single arsenic $\delta$-layers within silicon, and show that the sub-nm electronic thickness of the $\delta$-layers corresponds to sub-nm chemical thickness. In combination with X-ray fluorescence imaging, this enables non-destructive three-dimensional characterization of nano-structured quantum devices. Due to the strong resonances at soft X-ray wavelengths, the technique is also ideally suited to characterize layered quantum materials, such as cuprates or the topical infinite-layer nickelates.

Scanning tunneling potentiometry (STP) is used to probe the local, current-induced electrochemical potential of carriers in graphene near circular electrostatic barriers in an out-of-plane magnetic field ranging from 0 to 1.4 T. These measurements provide nanometer-resolved information about the local motion of carriers, revealing significant changes in carrier dynamics with increasing field strength. At low magnetic fields the electrochemical potential displays a spiral-like pattern, while at high fields it exhibits distinct changes at particular radii. We show that the observed behavior indicates a transition from diffusive to ballistic transport. Additionally, the sharp changes in the measured potential profile at high fields result from the `spirograph' motion of carriers, which creates a local enhancement of the Hall field one cyclotron diameter away from the semiclassical turning point near the electrostatic barrier., Comment: 18 pages, 6 figures

Josephson junction field-effect transistors (JJFETs) have recently re-emerged as promising candidates for superconducting computing. For JJFETs to perform Boolean logic operations, the so-called gain factor $\alpha_{R}$ must be larger than 1. In a conventional JJFET made with a classical channel material, due to a gradual dependence of superconducting critical current on the gate bias, $\alpha_{R}$ is much smaller than 1. In this Letter, we propose a new device structure of quantum enhanced JJFETs in a zero-energy-gap InAs/GaSb heterostructure. We demonstrate that, due to an excitonic insulator quantum phase transition in this zero-gap heterostructure, the superconducting critical current displays a sharp transition as a function of gate bias, and the deduced gain factor $\alpha_{R}$ ~ 0.06 is more than 50 times that (~ 0.001) reported in a classical JJFET. Further optimization may allow achieving a gain factor larger than 1 for logic applications.

In this study, we identify EuCd2X2 (for X = P, As, Sb) as a series of magnetic semiconductors. We examine how the band gap of the series responds to X changing from phosphorus (P), to arsenic (As), and finally antimony (Sb). We characterize the samples using electronic transport and magnetization measurements. Based on infrared spectroscopy, we find that the band gap reduces progressively from 1.23 eV in EuCd2P2, to 0.77 eV in EuCd2As2, and finally 0.52 eV in EuCd2Sb2. In a magnetic field, all three systems show a strong response and their band gaps decrease at 4 K. This decrease is non-monotonic as we change X. It is strongest in the phosphorous compound and weakest in the antimony compound. For all the three compositions, EuCd2X2 remains a semiconductor up to the highest magnetic field applied (16 T).

The capture of photoexcited hot electrons in semiconductors before they lose their excess energy to cooling is a long-standing goal in photon energy conversion. Semiconductor nanocrystals have large electron energy spacings that are expected to slow down electron relaxation by phonon emission, but hot electrons in photoexcited nanocrystals nevertheless cool rapidly by energy transfer to holes. This makes the intrinsic phonon-bottleneck limited electron lifetime in nanocrystals elusive. We used a combination of theory and experiments to probe the hot electron dynamics of negatively charged Cadmium Sulfide (CdS) colloidal quantum dots (QDs) in the absence of holes. Experiments found that these hot electrons cooled on a 100 ps timescale. Theoretical simulations predicted that pure phonon-bottleneck limited electron cooling occurs on a similar timescale. This similarity suggests that the experimental measurements reflect the upper limit on hot electron lifetimes in these CdS QDs and the lower limit on the rates of processes that can harvest those hot electrons.

In the superionic phase of silver iodide, we observe a distorted tetragonal structure characterized by symmetry breaking in the cation distribution. This phase competes with the well known bcc phase, with a symmetric cation distribution at an energetic cost of only a few meV/atom. The small energy difference suggests that these competing structures may both be thermally accessible near the superionic transition temperature. We also find that the distribution of silver ions depends on the low-temperature parent polymorph, with memory persisting in the superionic phase on the nanosecond time scales accessible in our simulations. Furthermore, simulations on the order 100ns reveal that even at temperatures where the bcc phase is stable, significant fluctuations toward the tetragonal lattice structure remain. Our results are consistent with many "anomalous" experimental observations and offer a molecular mechanism for the "memory effect" in silver iodide.

Erbium ions in crystals show considerable promise for the technologies that will form the backbone of future networked quantum information technology. Despite advances in leveraging erbium's fibre-compatible infrared transition for classical and quantum applications, the transitions are, in general, not well understood. We present detailed absorption and laser site-selective spectroscopy of the C$_{\rm 3v}$(O$^{2-}$) centre in CaF$_2$:Er$^{3+}$ as an interesting erbium site case study. The $^{4}$I$_{15/2}$Z$_1 \rightarrow {^{4}}$I$_{13/2}$Y$_1$ transition has a low-temperature inhomogeneous linewidth of 1 GHz with hyperfine structure observable from the $^{167}$Er isotope. A parametrized crystal-field Hamiltonian is fitted to 34 energy levels and the two ground state magnetic splitting factors. The wavefunctions are used to perform a transition intensity analysis and electric-dipole parameters are fitted to absorption oscillator strengths. Simulated spectra for the $^{4}$I$_{11/2}\rightarrow {^{4}}$I$_{15/2}$ and $^{4}$I$_{13/2} \rightarrow {^{4}}$I$_{15/2}$ inter-multiplet transitions are in excellent agreement with the experimentally measured spectra. The $^{4}$I$_{13/2}$ excited state lifetime is 25.0\,ms and the intensity calculation is in excellent agreement with this value.

Strain engineering is a powerful tool routinely used to control and enhance properties such as ferroelectricity, magnetic ordering, or metal-insulator transitions. Epitaxial strain in thin films allows manipulation of in-plane lattice parameters, achieving strain values generally up to 4\%, and above in some specific cases. In polycrystalline films, which are more suitable for functional applications due to their lower fabrication costs, strains above 1% often cause cracking. This poses challenges for functional property tuning by strain engineering. Helium implantation has been shown to induce negative pressure through interstitial implantation, which increases the unit cell volume and allows for continuous strain tuning with the implanted dose in epitaxial monocrystalline films. However, there have been no studies on the transferability of helium implantation as a strain-engineering technique to polycrystalline films. Here, we demonstrate the technique's applicability for strain engineering beyond epitaxial monocrystalline samples. Helium implantation can trigger an unprecedented lattice parameter expansion of up to 3.2% in polycrystalline BiFeO3 films without causing structural cracks. The film maintains stable ferroelectric properties with doses up to 1E15 He/cm2. This finding underscores the potential of helium implantation in strain engineering polycrystalline materials, enabling cost-effective and versatile applications., Comment: 6 pages, 4 Figures

Solid-state single-photon emitters provide a versatile platform for exploring quantum technologies such as optically connected quantum networks. A key challenge is to ensure optical coherence and spectral stability of the emitters. Here, we introduce a high-bandwidth `check-probe' scheme to quantitatively measure (laser-induced) spectral diffusion and ionisation rates, as well as homogeneous linewidths. We demonstrate these methods on single V2 centers in commercially available bulk-grown 4H-silicon carbide. Despite observing significant spectral diffusion under laser illumination ($\gtrsim$ GHz/s), the optical transitions are narrow ($\sim$35 MHz), and remain stable in the dark ($\gtrsim$1 s). Through Landau-Zener-St\"uckelberg interferometry, we determine the optical coherence to be near-lifetime limited ($T_2 = 16.4(4)$ ns), hinting at the potential for using bulk-grown materials for developing quantum technologies. These results advance our understanding of spectral diffusion of quantum emitters in semiconductor materials, and may have applications for studying charge dynamics across other platforms.

Bismuth antimony alloys (Bi$_x$Sb$_{1-x}$) provide a tuneable materials platform to study topological transport and spin-polarized surface states resulting from the nontrivial bulk electronic structure. In the two-dimensional limit, it is a suitable system to study the quantum spin Hall effect. In this work we grow epitaxial, single orientation thin films of Bi$_x$Sb$_{1-x}$ on an InSb(111)B substrate down to two bilayers where hybridization effects should gap out the topological surface states. Supported by a tight-binding model, spin- and angle-resolved photoemission spectroscopy data shows pockets at the Fermi level from the topological surface states disappear as the bulk gap increases from confinement. Evidence for a gap opening in the topological surface states is shown in the ultrathin limit. Finally, we observe spin-polarization approaching unity from the topological surface states in 10 bilayer films. The growth and characterization of ultrathin Bi$_x$Sb$_{1-x}$ alloys suggest ultrathin films of this material system can be used to study two-dimensional topological physics as well as applications such as topological devices, low power electronics, and spintronics., Comment: 7 pages, 4 figures

Ionising radiation interactions in matter can trigger a cascade of processes that underpin long-lived damage in the medium. To date, however, a lack of suitable methodologies has precluded our ability to understand the role that material nanostructure plays in this cascade. Here, we use transient photoabsorption to track the lifetime of free electrons (t_c) in bulk and nanostructured SiO2 (aerogel) irradiated by picosecond-scale (10^-12 s) bursts of X-rays and protons from a laser-driven accelerator. Optical streaking reveals a sharp increase in t_c from < 1 ps to > 50 ps over a narrow average density (p_av) range spanning the expected phonon-fracton crossover in aerogels. Numerical modelling suggests that this discontinuity can be understood by a quenching of rapid, phonon-assisted recovery in irradiated nanostructured SiO_2. This is shown to lead to an extended period of enhanced energy density in the excited electron population. Overall, these results open a direct route to tracking how low-level processes in complex systems can underpin macroscopically observed phenomena and, importantly, the conditions that permit them to emerge.

We have investigated the magnetic diffuse scattering of isostructural $S$ = 5/2 fcc antiferromagnets Ba$_2$MnTeO$_6$ and Ba$_2$MnWO$_6$ using polarized neutrons. Both materials display short-range correlated magnetism above their respective magnetic ordering temperatures of 20 K and 8 K. The spin correlations were analysed using a Reverse Monte Carlo approach. For Ba$_2$MnTeO$_6$, we find antiferromagnetic nearest-neighbor correlations along with ferromagnetic next-nearest neighbor correlations directly linked to the Type I order below $T_N$. For Ba$_2$MnWO$_6$, both the nearest-neighbor and next-nearest-neighbor spin correlations are antiferromagnetic in the paramagnetic state. The short-range spin correlations persist up to $T$ = 7$T_N$. The magnetic diffuse scattering was also fitted using Onsager reaction-field theory allowing us to evaluate the magnetic interactions in these materials. We obtained $J_1$ = -3.25(3) K and $J_2$ = 0.41(2) K for Ba$_2$MnTeO$_6$ and $J_1$ = -1.08(1) K and $J_2$ = -0.88(1) K for Ba$_2$MnWO$_6$. These interactions are comparable to previous results from inelastic neutron scattering experiments below $T_N$, which highlights the potential of the Onsager approach for the analysis of magnetic interactions., Comment: 21+4 pages, 5+3 figures

The tetragonal $4f$-electron intermetallic ErB$_4$ is characterized by strong Ising anisotropy along the tetragonal $c$ axis. The magnetic moments on the erbium sites can be mapped onto a Shastry-Sutherland (SSL) lattice resulting in geometrical frustration. At zero magnetic field ErB$_4$ exhibits collinear columnar antiferromagnetic (CAFM) order below $T_\text{N} = 15.4$ K. In the presence of a magnetic field parallel to the $c$ axis, ErB$_4$ exhibits a plateau at $1/2$ of the saturation magnetization $M_\text{S}$, which arises at a spin flip transition at $H_1$ $=$ 1.9 T. Fractional magnetization plateaus and other exotic spin phases are a well-established characteristic feature of frustrated spin systems. Monte Carlo simulations propose that ErB$_4$ is an ideal candidate to feature a spin supersolid phase in close vicinity of $H_1$ between the CAFM and $M/M_\text{S}=1/2$ plateau (HP) phase. Here we combine single-crystal neutron diffraction and inelastic neutron scattering to study the magnetic phase diagram and the crystal electric field (CEF) ground state of ErB$_4$. Our measurements as a function of magnetic field find no signature of the spin supersolid phase but allow us to determine the magnetic structure of the HP phase to be of the uuud type consistent with an Ising material. The magnetic moment $\mu_{\mathrm{CEF}}$ $=$ 8.96 $\mu_B$ expected from the CEF configuration determined by our inelastic neutron scattering measurements is also consistent with the ordered moment observed in neutron diffraction showing that the moments are fully ordered and close to the Er$^{3+}$ free ion moment (9.6 $\mu_B$).

Introducing superconductivity in topological materials can lead to innovative electronic phases and device functionalities. Here, we present a new strategy for quantum engineering of superconducting junctions in moire materials through direct, on-chip, and fully encapsulated 2D crystal growth. We achieve robust and designable superconductivity in Pd-metalized twisted bilayer molybdenum ditelluride (MoTe2) and observe anomalous superconducting effects in high-quality junctions across ~ 20 moire cells. Surprisingly, the junction develops enhanced, instead of weakened, superconducting behaviors, exhibiting fluctuations to a higher critical magnetic field compared to its adjacent Pd7MoTe2 superconductor. Additionally, the critical current further exhibits a striking V-shaped minimum at zero magnetic field. These features are unexpected in conventional Josephson junctions and indeed absent in junctions of natural bilayer MoTe2 created using the same approach. We discuss implications of these observations, including the possible formation of mixed even- and odd-parity superconductivity at the moire junctions. Our results also demonstrate a pathway to engineer and investigate superconductivity in fractional Chern insulators., Comment: 25 pages, 5 main article figures and 10 supplementary figures

We investigate the impact of introducing a local cavity within the center of a topological chain, revealing profound effects on the system's quantum states. Notably, the cavity induces a scissor-like effect that bisects the chain, liberating Majorana zero modes (MZMs) within the bulk. Our results demonstrate that this setup enables the observation of non-trivial fusion rules and braiding -- key signatures of non-Abelian anyons -- facilitated by the spatially selective ultra-strong coupling of the cavity photon field. These MZM characteristics can be directly probed through fermionic parity readouts and photon Berry phases, respectively. Furthermore, by leveraging the symmetry properties of fermion modes within a two-site cavity, we propose a novel method for generating MZM-polariton Schr\"odinger cat states. Our findings present a significant advancement in the control of topological quantum systems, offering new avenues for both fundamental research and potential quantum computing applications., Comment: Main text: 6 pages, 5 Figures, Supplemental Material: 8 pages, 5 Figures

Exchange bias (EB) is a fundamental phenomenon in widespread information technologies. However, a comprehensive understanding of its microscopic origin remains a great challenge. One key issue in the debate is the role of frustration and disorder in the EB mechanism, which motivates the exploration of the EB effect in spin glass (SG) systems. Here,in the SG state of Cr-doped Hund's metal CsFe2As2, we discover a giant EB effect with a maximum bias field of ~ 2 Tesla, which is almost two orders of magnitude larger than that of traditional alloy SGs. Our results indicate that the giant EB effect should originate from the exchange interactions at the natural boundaries between the tunable ferromagnetic-like (FM) regions around Cr dopants and the SG matrix, via which the FM spins are strongly pinned by the frozen spins in the SG matrix. In addition, the temperature-dependent and cooling-field-dependent EB behaviors could be interpreted well by the SG model with frustrated FM/SG boundaries, which provides an intuitive and explicit understanding of the impact of glassy parameters on the EB effect. All these results suggest that the correlated metals are promising directions for exploring the EB effect in the SG state., Comment: 17 pages, 5 figures,Supplementary information available on request

The Pauli exclusion principle combined with interactions between fermions is a unifying basic mechanism that can give rise to quantum phases with spin order in diverse physical systems. Transition-metal ferromagnets, with isotropic ordering respecting crystallographic rotation symmetries and with a net magnetization, are a relatively common manifestation of this mechanism, leading to numerous practical applications, e.g., in spintronic information technologies. In contrast, superfluid $^3$He has been a unique and fragile manifestation, in which the spin-ordered phase is anisotropic, breaking the real-space rotation symmetries, and has zero net magnetization. The recently discovered altermagnets share the spin-ordered anisotropic zero-magnetization nature of superfluid $^3$He. Yet, altermagnets appear to be even more abundant than ferromagnets, can be robust, and are projected to offer superior scalability for spintronics compared to ferromagnets. Our Perspective revisits the decades of research of the spin-ordered anisotropic zero-magnetization phases including, besides superfluid $^3$He, also theoretically conceived counterparts in nematic electronic liquid-crystal phases. While all sharing the same extraordinary character of symmetry breaking, we highlight the distinctions in microscopic physics which set altermagnets apart and enable their robust and abundant material realizations., Comment: 12 pages, 4 figures

On-surface chemistry has emerged as a key technique for designing novel low-dimensional materials, enabling precise manipulation of their electronic and magnetic properties at the atomic scale. It also proves highly effective for the fabrication of heterostructures. Leveraging these benefits, herein, we perform a first principles study of the magnetic proximity effect (MPE) in a heterostructure formed by a monolayer of the two-dimensional carbon allotrope biphenylene network (BPN) deposited on the surface of the above-room-temperature ferrimagnet yttrium iron garnet (YIG). Our results reveal strong hybridization between BPN orbitals and YIG surface states, resulting in non-homogeneous electron transfer and robust MPE. The proposed methodology accurately describes YIG magnetic interactions, allowing us to study the tuning effects of BPN on the magnetic properties of the substrate for the first time. Additionally, we explore the impact of van der Waals (vdW) distance at the interface, finding enhanced spin splitting up to 30% under external pressure. These findings highlight a promising strategy for inducing spin polarization in BPN without chemical modifications, opening new possibilities for BPN-based spintronic devices through the creation of heterostructures with magnetic materials.

We present the first calculations of the inelastic part of the dynamical structure factor (DSF) for warm dense matter (WDM) using Time-Dependent Orbital-Free Density Functional Theory (TD-OF-DFT) and Mixed-Stochastic-Deterministic (mixed) Kohn Sham TD-DFT (KS TD-DFT). WDM is an intermediate phase of matter found in planetary cores and laser-driven experiments, where the accurate calculation of the DSF is critical for interpreting X-ray Thomson scattering (XRTS) measurements. Traditional TD-DFT methods, while highly accurate, are computationally expensive, motivating the exploration of TD-OF-DFT and mixed TD-KS-DFT as more efficient alternatives. We applied these methods to experimentally measured WDM systems, including solid-density aluminum and beryllium, compressed beryllium, and carbon-hydrogen mixtures. Our results show that TD-OF-DFT requires a dynamical kinetic energy potential in order to qualitatively capture the plasmon response. Additionally, it struggles with capturing bound electron contributions and accurately modeling plasmon dynamics without the inclusion of a dynamic kinetic energy potential. In contrast, mixed TD-KS-DFT offers greater accuracy in distinguishing bound and free electron effects, aligning well with experimental data, though at a higher computational cost. This study highlights the trade-offs between computational efficiency and accuracy, demonstrating that TD-OF-DFT remains a valuable tool for rapid scans of parameter space, while mixed TD-KS-DFT should be preferred for high-fidelity simulations. Our findings provide insight into the future development of DFT methods for WDM and suggest potential improvements for TD-OF-DFT.

Interface-type resistive switching (RS) devices with lower operation current and more reliable switching repeatability exhibits great potential in the applications for data storage devices and ultra-low-energy computing. However, the working mechanism of such interface-type RS devices are much less studied compared to that of the filament-type devices, which hinders the design and application of the novel interface-type devices. In this work, we fabricate a metal/TiOx/TiN/Si (001) thin film memristor by using a one-step pulsed laser deposition. In situ transmission electron microscopy (TEM) imaging and current-voltage (I-V) characteristic demonstrate that the device is switched between high resistive state (HRS) and low resistive state (LRS) in a bipolar fashion with sweeping the applied positive and negative voltages. In situ scanning transmission electron microscopy (STEM) experiments with electron energy loss spectroscopy (EELS) reveal that the charged defects (such as oxygen vacancies) can migrate along the intrinsic grain boundaries of TiOx insulating phase under electric field without forming obvious conductive filaments, resulting in the modulation of Schottky barriers at the metal/semiconductor interfaces. The fundamental insights gained from this study presents a novel perspective on RS processes and opens up new technological opportunities for fabricating ultra-low-energy nitride-based memristive devices.

There is an important difference between piezoelectric polymer films and solid crystals for the application to piezoelectric generators. In the case of polymers, the optimal piezoelectric response imposes {\it a large bending regime}. Starting from the linear Curie's constitutive equations, we develop an analytical model under the assumption of the large bending regime resulting from bulge testing configuration. This model shows a specific non-linear piezoelectric response, that follows a power $2/3$ of the mechanical excitation. The piezoelectric voltage and the corresponding power are then studied experimentally as a function of the angular frequency $\omega$ of the mechanical excitation, the load resistance $R$, and the thickness of the film $\ell$. The experimental results carried out on piezoelectric PVDF films validate the model., Comment: The following article has been accepted by Journal of Applied Physics. After it is published, it will be found at https://pubs.aip.org/aip/jap

A quantitative measure of symmetry breaking is introduced that allows the quantification of which symmetries are most strongly broken due to the introduction of some kind of defect in a perfect structure. The method uses a statistical approach based on the Jensen-Shannon divergence. The measure is calculated by comparing the transformed atomic density function with its original. Software code is presented that carries the calculations out numerically using Monte Carlo methods. The behavior of this symmetry breaking measure is tested for various cases including finite size crystallites (where the surfaces break the crystallographic symmetry), atomic displacements from high symmetry positions, and collective motions of atoms due to rotations of rigid octahedra. The approach provides a powerful tool for assessing local symmetry breaking and offers new insights that can help researchers understand how different structural distortions affect different symmetry operations., Comment: 25 pages, 15 figures

The term sample dependence describes the troublesome tendency of nominally equivalent samples to exhibit different physical properties. High entropy oxides (HEOs) are a class of materials where sample dependence has the potential to be particularly profound due to their inherent chemical complexity. In this work, we prepare a spinel HEO of identical nominal composition by five distinct methods, spanning a range of thermodynamic and kinetic conditions: solid state, high pressure, hydrothermal, molten salt, and combustion syntheses. By structurally characterizing these five samples across all length scales with a variety of x-ray methods, we find that while the average structure is unaltered, the samples vary significantly in their local structures and their microstructures. The most profound differences are observed at intermediate length scales, both in terms of crystallite morphology and cation homogeneity. As revealed by x-ray fluorescence microscopy ideal cation homogeneity is achieved only in the case of combustion synthesis. These structural differences in turn significantly alter the observed functional properties, which we demonstrate via characterization of their magnetic response. While ferrimagnetic order is retained across all five samples, the sharpness of the transition, the size of the saturated moment, and the coercivity all show marked variations with synthesis method. We conclude that the chemical flexibility inherent to HEOs is complemented by strong synthesis method dependence, providing another axis along which to optimize these materials for a wide range of applications., Comment: 14 pages, 5 figures

We explore the impact of introducing IIIA-group element Ga in place of IIB-group element Zn in binary intermetallic GdZn on its magnetic and magnetocaloric properties, as well as explicate the modified electronic band structure of the compound. The magnetic transition temperature of the compound decreases with the increase of Ga concentration in GdZn1-xGax (x = 0-0.1) while the crystal structure (CsCl-prototype) and lattice parameters remain unchanged. Our detailed analysis of magnetization and magnetocaloric data conclusively proves that long-ranged magnetic ordering exists in the sample, despite the magnetic interaction considerably weakening with the increase of Ga. The experimental data is rationalized using both theoretical machine learning model and first-principle density functional theory.The electronic band structure of GdZn is manifested with some unusual complex features which gradually diminish with Ga doping and conventional sinusoidal feature of Ruderman-Kittel-Kasuya- Yosida (RKKY)-type interactions also disappears. A mean-field theory model is developed and can successfully describe the overall magnetocaloric behavior of the GdZn1-xGax series of samples

Efficient hybrid DFT simulations of solid state materials would be extremely beneficial for computational chemistry and materials science, but is presently bottlenecked by difficulties in computing Hartree-Fock (HF) exchange with plane wave orbital bases. We present a GPU-accelerated, Gaussian orbital based integral algorithm for systems with periodic boundary conditions, which takes advantage of Ewald summation to efficiently compute electrostatic interactions. We have implemented this approach into the TeraChem software package within the $\Gamma$ point approximation, enabling simulation of unit cells with hundreds or thousands of atoms at the HF or hybrid DFT level on a single GPU card. Our implementation readily parallelizes over multiple GPUs and paves the road to accurate simulation of the properties and dynamics of extended materials in both the ground and excited states.

Polarized Raman spectra of piezoelectric bismuth germanate single crystal were recorded using vortex light in order to verify the predicted symmetry selection rules for Raman scattering of photons with nonzero orbital angular momentum. At first, the phonon spectrum is fully characterized by the infrared reflectivity and Raman scattering with ordinary light. Then, vortex light Raman spectra were compared with the ordinary ones, but no influence of the orbital momentum on the Raman spectra of Bi$_4$Ge$_3$O$_{12}$ was observed. In particular, we experimentally negate the theoretical prediction that Raman scattering using vortex light can yield frequencies of the silent optic modes of Bi$_4$Ge$_3$O$_{12}$. We also have not seen evidence for the predicted symmetry-lowering of the Raman scattering tensors of $E$ modes. We propose that the orbital momentum effects are inaccessible to the ordinary Raman spectroscopy experiments because of the tiny magnitudes of typical phonon coherence lengths., Comment: 6 pages, 6 figures

The synthesis of inorganic crystalline materials is essential for modern technology, especially in quantum materials development. However, designing efficient synthesis workflows remains a significant challenge due to the precise experimental conditions and extensive trial and error. Here, we present a framework using large language models (LLMs) to predict synthesis pathways for inorganic materials, including quantum materials. Our framework contains three models: LHS2RHS, predicting products from reactants; RHS2LHS, predicting reactants from products; and TGT2CEQ, generating full chemical equations for target compounds. Fine-tuned on a text-mined synthesis database, our model raises accuracy from under 40% with pretrained models, to under 80% using conventional fine-tuning, and further to around 90% with our proposed generalized Tanimoto similarity, while maintaining robust to additional synthesis steps. Our model further demonstrates comparable performance across materials with varying degrees of quantumness quantified using quantum weight, indicating that LLMs offer a powerful tool to predict balanced chemical equations for quantum materials discovery., Comment: 66 pages total, 6 main figures + 3 supplementary figures

Dielectric metasurfaces that combine high-index materials with optical nonlinearities are widely recognized for their potential in various quantum and classical nanophotonic applications. However, the fabrication of high-quality metasurfaces poses significant material-dependent challenges, as their designs are often susceptible to disorder, defects, and scattering losses, which are particularly prone to occur at the edges of nanostructured features. Additionally, the choice of the material platforms featuring second-order optical nonlinearities, $\chi^{(2)}$, is limited to broken-inversion symmetry crystals such as GaAs, GaP, LiNbO$_3$, and various bulk van der Waals materials, including GaSe and NbOCl$_2$. Here, we use a combination of top-down lithography and anisotropic wet etching of a specially stacked van der Waals crystal -- 3R-MoS$_2$, which exhibits both a high refractive index and exceptional $\chi^{(2)}$ nonlinearity, to produce metasurfaces consisting of perfect equilateral triangle nanoholes with atomically precise zigzag edges. Due to the geometry of the triangle, the etching process is accompanied by a transition from an in-plane $C_4$ symmetric structure to a broken-in-plane symmetry configuration, thereby allowing for the realization of the quasi-bound-state-in-the-continuum (q-BIC) concept. The resulting ultrathin metasurface ($\sim$ 20-25 nm) demonstrates a remarkable enhancement in second-harmonic generation (SHG) -- over three orders of magnitude at specific wavelengths and linear polarization directions compared to a host flake.

Hydrogen in its metallic form is the most common material in our solar system, found under the extreme pressure and temperature conditions found in giant planets. Such conditions are inaccessible to experiment and consequently, theoretical work has typically led experiment. Many remarkable properties are proposed for metallic hydrogen, which is expected to exist in solid form down to low temperatures. Relevant here is that solid metallic hydrogen is not expected to have a close-packed structure, even at extreme pressures. The predicted crystal structure has a packing fraction of only 0.44 compared with 0.74 for fcc. Alloying with other metallic elements can form compounds with atomic hydrogen and much reduced metallization pressure. Here, we investigate the possible solid solubility of a representative range of elements (Be, B, Mg, S, Fe, La) in metallic atomic hydrogen near 500GPa. Zero point energy is highly significant in all cases. The metallic elements Be, Mg, Fe, and La have a well-defined clathrate-style first neighbour shell at 300K, while the non-metallic B and S have more open arrangements. All the elements considered are soluble, in sites substituting for more than one hydrogen atom. The solid solubility of such a wide range of ambient bonding types: simple metals, covalent materials, transition metals, lanthanides, which gives a strong indication that most elements will dissolve in solid metallic hydrogen., Comment: 7 pages, 4 figures, submitted to Physical Review Letters

Janus transition metal-dichalcogenide (JTMD) materials have attracted a great deal of attention due to their remarkable physical properties arising from the two-dimensional geometry and the breakdown of the out-of-plane symmetry. Using first-principles density functional theory, we investigated the phase stability, strain-enhanced phase stability, and superconductivity of Janus WSeH and WSH. In addition, we investigated the contribution of the phonon linewidths from the phonon energy spectrum responsible for the superconductivity, and the electron-phonon coupling as a function of phonon wave vectors and modes. Previous work has examined hexagonal 2H and tetragonal 1T structures, but we found that neither is a ground state structure. The metastable 2H phase of WSeH is dynamically stable with Tc around 11.60K, similar to WSH. Compressive biaxial strain - the 2D equivalent of pressure - can stabilize the 1T structures of WSeH and WSH with Tc around 9.23K and 10.52K, respectively., Comment: 13 pages, 15 figures, to be published in Physical Review B