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Physics Condensed Matter Materials Science

cond-mat.mtrl-sci Watch Materials Science

Thursday 18 June

Materials Science

Breaking symmetry to create a parallel-plate varactor dielectric with unparalleled microwave performance

Florian Bergmann, Matthew R. Barone, Zishen Tian et al. (+24 more)

Voltage-tunable capacitors (varactors) are key to microwave circuits. Tunable dielectric varactors outperform competing technologies in almost every relevant metric but usually suffer from high dielectric loss. In contrast, Ruddlesden-Popper (RPs) dielectric thin films have remarkably low microwave loss. Unfortunately, their crystallographic symmetry has until recently dictated an in-plane device structure, precluding the favorable out-of-plane parallel-plate varactor design for minimized size and maximized electric field in the tunable dielectric. Guided by theory, we report RPs akin to the widely studied tunable microwave dielectric BaxSr1-xTiO3. Assembling these same atoms into the first RP phase with broken out-of-plane symmetry, we achieve a low-loss, out-of-plane tunable dielectric thin film. The highest performing film, (ATiO3)nAO film with A = Ba0.45Sr0.55 and n = 8, unlocks a tenfold improvement in the figure of merit for out-of-plane tunable dielectrics at 10 GHz, paving the way for a new generation of tunable monolithic microwave integrated circuits.
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All authors Florian Bergmann, Matthew R. Barone, Zishen Tian, Aiden Ross, Gerhard H. Olsen, Meagan C. Papac, Samuel Freed, Bryan T. Bosworth, Nicholas R. Jungwirth, Eric J. Marksz, Tomasz Karpisz, Noah Schnitzer, Lopa Bhatt, David A. Muller, Dylan Sotir, Akash Surampalli, Veronica Goian, Christelle Kadlec, Stanislav Kamba, Asher Hansen, Nathan Rongitsch, Dmitri A. Tenne, Ichiro Takeuchi, Long-Qing Chen, Lane W. Martin, Nathan D. Orloff, Darrell G. Schlom

Materials Science

Effective masses, Burstein-Moss shift, and bandgap renormalization in degenerate Al-doped ZnO from broadband ellipsometry and Hall measurements

S. Mishra, L. A. Enrique, D. Cespedes et al. (+7 more)

A comprehensive methodology is developed to extract electron and hole effective masses in degenerate semiconductors through a simultaneous global fit of carrier concentration dependence of bandgap and plasma energy, explicitly incorporating band nonparabolicity. Broadband spectroscopic ellipsometry combined with Hall effect analyses enables accurate determination of the bandgap, plasma energy and carrier concentrations. The dielectric function of sputtered Al-doped ZnO thin films are modeled in the fundamental absorption region using an Elliott based model with overlapping excitonic transitions and Urbach tails, while free carrier absorption is described by a modified sernelius formula. Wide carrier concentrations are achieved via controlled deposition and post-annealing, revealing changes in electron effective masses and deviations from parabolic dispersion. Two nonparabolic models are compared, Pisarkiewicz, assuming spherically symmetric band with a step-function approximation of the Fermi-Dirac distribution and Nilsson, incorporating thermal and impurity effects. The latter is shown to capture accurately band nonparabolicity, yielding effective masses and nonparabolicity parameter consistent with bandgap evolution. This approach quantitatively separates Burstein-Moss shift and bandgap renormalization, reproducing carrier dependent bandgap shifts across a wide concentration range. Neglecting valence band contributions introduces systematic bias. Bandgap renormalization is further evaluated using plasmon pole and random phase approximations, underscoring the importance of many-body screening. This framework also enables determination of the Mott critical concentration and the fundamental absorption edge onset. Collectively, these results establish a reliable methodology for extracting band-structure parameters and bandgap shifts, extendable to other transparent conducting oxides.
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All authors S. Mishra, L. A. Enrique, D. Cespedes, E. Perez, E. Serquen, F. Bravo, P. Llontop, F. Ruske, L. Korte, J. A. Guerra

Materials Science

Tunable Flat Bands and magnetism in Triangulene-based Superatomic Graphene

Wenya Zhai, Tingfeng Zhang, Fengkun Chen et al. (+8 more)

Superatomic graphene platforms host a rich portfolio of flat-band-driven exotic quantum properties, yet their experimental realization remains challenging. Here, we report the bottom-up on-surface synthesis of superatomic graphene using phosphorus-doped triangulene as building blocks. Scanning tunneling microscopy and spectroscopy measurements resolve the well-defined honeycomb lattice of as-fabricated superatomic graphene and demonstrate the characteristic Dirac band and flat band electronic structures. Density functional theory calculations reveal that the flat bands originate from the in-plane p$_x,_y$-like frontier orbitals of the phosphorus-doped triangulene units, leading to intrinsic half-metallic behavior. Furthermore, oxygen functionalization of the molecular precursor enables deterministic modulation of the electronic structure and magnetic ordering. This work establishes a general platform for designing correlated quantum materials with tunable flat band properties.
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All authors Wenya Zhai, Tingfeng Zhang, Fengkun Chen, Xiuqin Lu, Yunlong Xia, Zengfu Ou, Ye Chen, Donghui Guo, Meifang Zhu, Zhengfei Wang, Jingcheng Li

Materials Science

Exciton Transport in Disordered Perovskite Nanocrystal Solids

Simon Solari, Enrique Arévalo Rodríguez, Antonella Cutrupi et al. (+6 more)

Solution-processed thin films of colloidal lead halide perovskite (LHP) nanocrystals (NCs) show great potential for the implementation into optoelectronic devices such as light-emitting diodes (LEDs), lasers, and solar cells. However, these hybrid LHP NC solids exhibit non-negligible size and shape polydispersity, which introduces both structural and energetic disorder. Here, we resolve the exciton dynamics in space, time, and energy to elucidate the impact of different forms of disorder (structural and energetic) on exciton transport. We show that the disorder depends sensitively on the length of the alkylamine ligand used in the synthesis. While shorter alkyl chain lengths lead to high polydispersity, longer alkyl chains lead to more monodispersed and smaller particles where quantum confinement becomes more pronounced and, consequently, lead to increased energetic disorder. Strikingly, we find that exciton transport is less efficient in NC solids with long alkyl chain ligands, despite having a significantly more monodisperse ensemble. This demonstrates that energetic disorder, rather than structural disorder, is the dominant factor for predicting exciton transport within these materials. These findings reveal the critical role of ligand engineering in designing high-performance optoelectronic devices based on hybrid LHP NCs, providing new insights into energy transport dynamics in disordered systems and highlighting the versatility of these materials for advanced photonic and optoelectronic applications.
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All authors Simon Solari, Enrique Arévalo Rodríguez, Antonella Cutrupi, Amalia Coro, Marc Meléndez, Alicia De Andrés, Almudena Torres-Pardo, Beatriz H. Juárez, Ferry Prins

Materials Science

Anomalous magneto-optical response at $\mathrm{RuO_2 / WSe_2}$ van der Waals interface

Muhammad Hassan Shaikh, Abhijith Puthiya Veettil, Collin Maurtua et al. (+9 more)

Ruthenium dioxide ($\mathrm{RuO_2}$) has been proposed as an altermagnetic candidate, although its magnetic ground state remains controversial. Here, we probe weak interfacial magnetic states at the surface of (001)-oriented $\mathrm{RuO_2}$ films using the magnetic proximity effect (MPE) in a van der Waals heterostructure consisting of monolayer tungsten diselenide ($\mathrm{WSe_2}$) atop $\mathrm{RuO_2}$. Temperature-dependent magneto-optical spectroscopy reveals an anomalous excitonic energy shift and a deviation from conventional Varshni behavior below 55 K that are absent in an encapsulated $\mathrm{WSe_2}$ control sample. The anomalous shift reverses sign upon field cooling with opposite magnetic field polarity, indicating a magnetic origin. Polarization-resolved measurements further show a nearly field-independent and fluctuating valley splitting in $\mathrm{WSe_2 / RuO_2}$ in strong contrast to the conventional linear Zeeman splitting observed in the control bare $\mathrm{WSe_2}$ sample. These results suggest that the valley states are governed predominantly by interfacial exchange fields associated with weak surface magnetic states in $\mathrm{RuO_2}$, which do not produce a conventional linear Zeeman response within the applied magnetic field range. Importantly, this approach enables direct optical probing of emergent surface magnetism without introducing an additional ferromagnetic layer, positioning MPE-based optical probing as a tool for investigating weak surface magnetism and offering new possibilities for studying magnetic materials with controversial magnetic states.
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All authors Muhammad Hassan Shaikh, Abhijith Puthiya Veettil, Collin Maurtua, Dai Q. Ho, Subhash Bhatt, David T. Plouff, Malitha Gulawita, Kenji Watanabe, Takashi Taniguchi, John Q. Xiao, Anderson Janotti, Chitraleema Chakraborty

Materials Science

On representation of macroscopic crack in periodic fine-scale discrete mechanical models

Jan Raisinger and Jan Eliáš

In multiscale modeling of heterogeneous softening materials, boundary conditions (BC) in the fine-scale model strongly influence the strain localization pattern and the macroscopic response. For rectilinear models (e.g., squares or cubes), standard Periodic BCs produce artificially ductile behavior with excessive energy dissipation when the localization band inclination does not match the periodicity directions. Recently proposed Tessellation and Percolation-path-aligned BCs promise to address this by adapting the periodicity frame to align with the evolving localization bands. Alternatively, spherical/circular models provide an orientation independent response by design. Unfortunately, the standard Periodic BCs do not allow development of proper localization band crossing spherical model's boundaries. A recently proposed modification addresses this by adding a displacement jump to the spherical periodic BCs. This study evaluates the applicability of these novel BCs to a mesoscale discrete particle model of concrete. Two-dimensional square and circular models under uniaxial tension with different loading directions are analyzed, with the selected approaches extended to three-dimensional cube models. Results show that Percolation-path-aligned BCs exhibit major shortcomings: they can lead to multiple localization bands due to uneven straining of the two boundary sections and their weakly constrained section can be prone to spurious strain localization. In contrast, Tessellation BCs consistently yield a well-defined localization band, whose length is determined solely by the model geometry, making it straightforward to account for in post-processing. Periodic boundary conditions augmented with a displacement jump applied to a circular model sometimes incorrect produce crack patterns similar to those under the standard Periodic BCs.
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Materials Science

Large spin splitting at ferromagnetic surfaces of bulk antiferromagnets

William A. Schaarman and Sophie F. Weber

We use density functional theory and model Hamiltonians to reveal large spin splitting of bands localized at ferromagnetic surfaces of bulk antiferromagnets (AFMs). There is great interest in material platforms combining the robustness and ultrafast dynamics of AFMs with large, functional spin splitting which is often restricted to ferromagnets (FMs). Here, we show that a subset of AFM surfaces which have symmetry-allowed magnetization can host large spin splitting via bulk degeneracy lifting of sublattice-resolved exchange splittings. We find that the spin splitting is maximized for two ferromagnetic surface motifs: terminations with single uncompensated magnetic sublattices, and two-sublattice surfaces whose sublattices are magnetically compensated in the bulk, but acquire distinct crystal field environments via surface truncation. The latter case can yield FM-like spin splitting magnitudes while also having small uncompensated magnetization. We confirm these predictions with first-principles calculations of $\mathrm{Cr_2O_3}$ and $\mathrm{FeF_2}$, finding splittings as large as $1~\mathrm{eV}$ depending on the surface in question. Our findings point to intrinsic surface symmetry breaking as a route to large, functional spin splitting in an expanded range of AFM materials.
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Materials Science · Cross-listed from cond-mat.mes-hall

Electric-field-driven magnetic switching and tightly bound interlayer excitons in bilayer CrSBr

Xiubin Li, Yu Sun, Xuanji Wang et al. (+8 more)

Electric field control of magnetic order in two-dimensional (2D) van der Waals magnets is a central goal for low-power spin-based technologies. In the ambient-stable antiferromagnet CrSBr, strong magnetic anisotropy and robust exciton-spin coupling provide a favorable platform, yet deterministic electric field control of its magnetic phases has not been achieved. Here we demonstrate electric-field-driven reversible switching between antiferromagnetic and ferromagnetic states in dual-gated bilayer CrSBr without intentional carrier doping. In parallel, photoluminescence measurements resolve a tightly bound interlayer exciton with an intrinsic dipole moment of only ~1 e angstrom. The electric field dependence of the magnetic phase transition reveals two coexisting mechanisms: a linear magnetoelectric effect in the antiferromagnetic state and an electric-field-modulated interlayer exchange coupling. Their interplay accounts for the asymmetric evolution of the critical magnetic field. Our results establish bilayer CrSBr as a promising 2D material for electrically controlled spin-optoelectronic functionalities.
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All authors Xiubin Li, Yu Sun, Xuanji Wang, Chunyan Wang, Kenji Watanabe, Takashi Taniguchi, Sheng Liu, Ting Yu, Liang Li, Tao Zhang, Jing Li

Materials Science

Hartree-Fock Limit for Energies in Solids

Jānis Užulis and Andris Gulans

This study establishes a route to the Hartree–Fock (HF) limit for molecules and solids within the linearized augmented plane wave (LAPW) framework. We remove current limitations of the standard LAPW approach to nonlocal exchange by constructing radial basis functions and core orbitals consistently with the HF Hamiltonian. The presented method yields total energies of molecules and solids with a precision of a few $\mu$Ha, and we use it to provide reference data for 14 semiconductors and insulators. For the systems considered in this study, the standard approach based on (semi)local potentials for constructing radial basis functions and core orbitals remains highly precise for practical relative energies, including molecular and solid-state formation energies and Si self-interstitial defect formation energies. More broadly, the results provide stringent all-electron benchmarks for basis-set and pseudopotential assessment, improve error control in hybrid-functional calculations within LAPW, and open the way to X-ray spectroscopy simulations within LAPW based directly on hybrid-functional core orbitals.
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Materials Science

Terahertz frequency upconversion by coherently driving charge dynamics in the InSb/CdTe heterostructure

Pai Peng, Mingxiang Pan, Jiuming Liu et al. (+10 more)

We investigate terahertz (THz) harmonic generation in the InSb/CdTe heterostructure, demonstrating, for the first time, efficient in-plane magnetic field-induced second-harmonic generation (SHG). We also achieve significant third-harmonic generation (THG), rivalling Dirac materials such as graphene and Cd3As2. Our theoretical analysis identifies the primary SHG mechanism as the orbital-Zeeman correction to Drude conductivity, while the dominant THG contribution also shows Drude-like behavior. The results provide a general route to efficient THz harmonic generation in high mobility materials.
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All authors Pai Peng, Mingxiang Pan, Jiuming Liu, Yi Yang, Lei Wang, Hao Lin, Zehao Hu, Jianlin Luo, Tao Dong, Xufeng Kou, Xinbo Wang, Huaqing Huang, Luyi Yang

Materials Science · Cross-listed from cond-mat.soft

Constraint-Limited Tube Orientation of Entangled Polymers in Oscillatory Shear Deformation

Dario Nichetti and Alessio Zaccone

We develop a molecularly motivated description of the nonlinear index (NLI) in oscillatory shear deformation of entangled polymers. The central assumption is that the shear component of the tube-orientation tensor cannot grow without bound. Convective constraint release (CCR), chain stretch, and tube dilation progressively reduce the number and lifetime of orientational constraints, but the maximum shear alignment of a tube segment is geometrically limited by $S_{xy}\leq 1/2$. This motivates a constraint-limited orientation closure in which the NLI first grows approximately with strain amplitude and then approaches the limiting value $\mathrm{NLI}_{\max}=3$ asymptotically rather than through an artificial cutoff. The same framework yields a molecular expression for the characteristic half-saturation strain $\gamma_s$, defined by $\mathrm{NLI}(\gamma_s)=3/2$, in terms of the entanglement number, oscillation frequency, and a critical number of remaining orientational constraints. We further derive architecture-dependent expressions for the nonlinear onset strain $\gamma_c$ for linear, sparsely long-chain-branched, and more regularly branched polymers. The resulting framework provides a compact bridge between Fourier harmonic analysis, CCR-based tube dynamics, and the progressive loss of orientational memory in highly deformed entangled polymer liquids.
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Materials Science

Quantitative prediction of excitons in lattice-mismatched van der Waals heterostructures

Jakob Kjærulff Svaneborg, Mikkel Ohm Sauer, Amalie Helena Svaneborg et al. (+1 more)

Accurate modeling of dielectric screening in van der Waals (vdW) heterostructures is essential for predicting photonic and optoelectronic properties - yet conventional first-principles methods are often hindered by incommensurate lattices and prohibitive computational costs. In this work, we introduce the microscopic Quantum Electrostatic Heterostructure (mQEH) method. mQEH employs a hierarchical and systematically improvable basis set to describe potentials and induced densities, eliminating the need for arbitrary geometric cutoffs and ensuring accurate screening descriptions at all length scales. The mQEH method is combined with a layer projected Bethe-Salpeter Equation (BSE) to enable calculations of optical spectra of experimentally relevant lattice-mismatched vdW heterostructures. Applying the mQEH-BSE framework to a series of transition-metal dichalcogenide (TMD) heterobilayers, we obtain absorption spectra and momentum-indirect exciton energies in excellent agreement with experiment. The framework provides a computationally efficient route to predictive modeling and design of vdW heterostructures with tailored optical properties.
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All authors Jakob Kjærulff Svaneborg, Mikkel Ohm Sauer, Amalie Helena Svaneborg, Kristian Sommer Thygesen

Materials Science

Interplay of Altermagnetism and Coupled Quasi-Altermagnetic states in Sliding Two-dimensional Square Lattice

Bhautik R Dhori, Deepak Upadhyay and Prafulla K Jha

The emergence of non-relativistic spin splitting (NRSS) in altermagnetic systems has introduced a new paradigm in antiferromagnets with vanishing net magnetization. Although sliding-induced valley-polarized phases have recently been demonstrated in two-dimensional altermagnets, the observed valley-polarized state represents only a partial manifestation of altermagnetism, and a comprehensive classification based on spinsplitting characteristics remains lacking. Here, using first-principles calculations, general stacking theory, and spin-Laue symmetry analysis, we propose a coupled quasialtermagnetic state representing a distinct subclass of altermagnetism, in which reversible type-IV NRSS is controlled through interlayer sliding. Accordingly, the sliding-induced phases are classified into two categories: altermagnetic and quasi-altermagnetic states. We establish a direct correspondence between reciprocal-space spin splitting and real-space switching between the two quasi-altermagnetic states. Importantly, the spin-polarized bands in these states remain spin split at {\Gamma} point even in the absence of spin-orbit coupling (SOC), distinguishing them within the proposed classification framework. To demonstrate the interplay between altermagnetic and quasi-altermagnetic states, we investigate the two-dimensional Lieb-lattice material Mn2WS4 and its Janus derivative Mn2WS2Se2, analysing how changes in the local environment influence the different magnetic phases. Importantly, the underlying mechanism is broadly applicable to a wide class of twodimensional square-lattice systems. We further investigate the effects of SOC, focusing on spin texture and transport signatures in coupled quasi-altermagnetic states.
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Materials Science

Strain- and Electric-Field-Tunable Valley Polarization in Mo0.75V0.25Te2(Mo3VTe8) for Valleytronic Application

Md. Mostaqul Islam, Vivek Chowdhury, Md. Nure-Alam-Dipu et al. (+1 more)

Valley polarization in 2D TMDs is promising for low-power valleytronic and spin-valley information processing, but time-reversal symmetry in pristine nonmagnetic TMDs keeps the K+ and K- valleys degenerate, limiting device applications. In this work, we investigated the structural stability, electronic properties, and tunable valley polarization of V-alloyed MoTe2 monolayer, Mo0.75V0.25Te2, using first-principles density functional theory (DFT) calculations. Substitutional alloying of MoTe2 with V introduced magnetic exchange interaction, which, together with spin-orbit coupling (SOC), lifted the valley degeneracy at the unequal valleys. The alloyed structure was found to be energetically and dynamically stable due to the absence of imaginary phonon modes. In pristine MoTe2, SOC produced spin splittings of 34.0 meV and 218.9 meV in the conduction bands and valence bands, respectively, but no valley polarization was observed. In contrast, Mo0.75V0.25Te2 exhibited spontaneous valley polarization of 37.3 meV in the conduction band and 78.2 meV in the valence band. The valley polarization was further enhanced by external electric fields and biaxial strain. A transverse electric field along the crystal c axis produced the maximum valley splitting of 132.8 meV in the valence band, whereas biaxial tensile strain increased the valence band valley splitting up to 160.8 meV. The maximum conduction band valley splitting reached 54.4 meV under 2% biaxial compressive strain. These results demonstrated that V alloying, combined with electric-field and strain engineering, provides an effective strategy for achieving large and tunable valley polarization in MoTe2. Thus, Mo0.75V0.25Te2 can be considered a promising 2D platform for tunable valleytronic device applications, such as transistors and sensors.
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All authors Md. Mostaqul Islam, Vivek Chowdhury, Md. Nure-Alam-Dipu, Ahmed Zubair

Materials Science

MinSurf: resolving the atomic-scale stability landscape of mineral surfaces

Fengzijun Pan, Zhoulin Liu, Pingyang Zhang et al. (+4 more)

Mineral surfaces govern interfacial reactivity in carbon mineralization, geo-energy storage, contaminant immobilization, heterogeneous catalysis and electrochemical interface engineering. Yet atomistic simulations often rely on commonly used facets or facet-level stability criteria, while distinct atomic terminations of the same crystallographic orientation are rarely resolved systematically because experimental characterization and density functional theory (DFT) calculations remain costly across large surface spaces. Here we present MinSurf, a high-throughput framework that resolves mineral surface selection as a surface-energy and morphology problem. MinSurf integrates surface enumeration, DFT labelling, machine-learning interatomic potentials and Wulff construction to predict stable terminations, surface-energy landscapes and equilibrium crystal morphologies. Applied to ten representative minerals, MinSurfSet comprises 764 surface slabs, with 90 corresponding oriented unit cells constructed as bulk references for surface-energy evaluation. The resulting MinNEP model predicts DFT surface energies with a mean absolute error of 0.0119 eV per Angstrom squared and achieves an overall acceleration of 1.14 x 10^4 relative to DFT. MinNEP preserves the DFT-derived morphology-determining surface-energy hierarchy and reproduces the dominant Wulff-exposed facets, while X-ray diffraction provides an independent crystallographic consistency check for alpha-quartz benchmark. By linking atomic terminations, surface energies and equilibrium morphologies, MinSurf provides reproducible and physically representative surface models for high-throughput simulations of mineral interfaces across energy, environmental and advanced inorganic materials.
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All authors Fengzijun Pan, Zhoulin Liu, Pingyang Zhang, Jiaqiu Xu, Zepeng Fan, Dawei Wang, Jianzhong Pei

Materials Science

Thickness-Dependent Interlayer Coupling and Semiconductor-to-Semimetal Crossover in Arsenene Multilayers

Jeonghwan Ahn, Seoung-Hun Kang and Jaron T. Krogel

Interlayer interactions in layered materials are often assumed to transfer from the bilayer to the bulk, but this assumption can fail when chemically active out-of-plane orbitals participate in bonding. We combine diffusion quantum Monte Carlo (DMC) and density functional theory (DFT) to determine how interlayer coupling evolves in arsenene multilayers. DMC shows that bulk gray arsenic is compact, whereas the corresponding few-layer structures remain at substantially larger interlayer separations despite sharing the same nominal A$_{1}$B$_{-1}$ adjacent-layer registry. Registry alone therefore does not determine the bonding regime; thickness and coordination reshape the interlayer interaction. Among the tested functionals, SCAN+rVV10 most closely reproduces DMC equilibrium separations and stacking energetics. Using the DMC-benchmarked SCAN+rVV10 calculations, we predict a thickness-driven stacking sequence from A$_{1}$A$_{1}$ to A$_{1}$B$_{1}$ and finally bulk-like A$_{1}$B$_{-1}$. The structural crossover coincides with a stacking-dependent DFT band-gap collapse driven by enhanced interlayer As p$_{z}$ hybridization.
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Materials Science

Enhanced electronic correlations and altermagnetic ground state of two-dimensional CsCr3Sb5 monolayers

Z. H. Guan, Z. L. Peng, W. Z. Zhuo et al. (+8 more)

Recently, layered corrected kagome metal CsCr3Sb5 have garnered significant attention attributed to its flat bands near the Fermi level (EF) and altermagnetic ground state [ Yi Liu et al., Nature 632, 1032 (2024)]. However, the van Hove singularities (vHSs) in bulk CsCr3Sb5 are far away from the EF, while an effective modulation of VHS toward the EF is essential for exploring intriguing electron transport properties. In this work, using first-principles calculations, we investigate electronic structures of two-dimensional (2D) Cr3Sb5 and CsCr3Sb5 monolayers which may be mechanically exfoliated from bulk materials. Notably, it is revealed that both flat bands and vHSs simultaneously reside in close proximity to the EF in Cr3Sb5 monolayer, signifying enhanced electronic correlations. Importantly, a tensile strain further shifts the incipient flat bands and vHSs of two monolayers simultaneously to the vicinity of the EF, suggesting strain tunable electronic correlations and concomitant quantum effects. Furthermore, altermagnetic ground state is also revealed due to retained mirror symmetry between two sublattices in these two monolayers. Thus, this work advances understanding and modulations of electronic properties of 2D CsCr3Sb5 monolayers, strengthening their great potential for exploring unconventional quantum phenomena and altermagnetism.
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All authors Z. H. Guan, Z. L. Peng, W. Z. Zhuo, G. Tian, Z. P. Hou, D. Y. Chen, Z. Fan, X. B. Lu, X. S. Gao, M. H. Qin, J. M. Liu

Materials Science

HEACalculator: An Open-Source Python Tool for Thermodynamic Property Calculation and Solid Solution Prediction in High-Entropy Alloys

Doğuhan Sar{\i}türk, Yunus Eren Kalay and Raymundo Arróyave

High-entropy alloys (HEAs) have attracted sustained interest since their introduction by Cantor et al. and Yeh et al. because multi-principal-element compositions can exhibit unusual combinations of strength, thermal stability, and functional performance. A recurring problem in HEA design is determining whether a candidate composition is likely to form a single-phase solid solution or instead separate into multiple phases or intermetallic compounds. That question sits early in the alloy-design workflow because it shapes which compositions require further thermodynamic analysis, synthesis, and experimental validation. HEACalculator is an open-source Python package for calculating thermodynamic and structural descriptors used in HEA research and for evaluating published solid-solution formation rules in a single place. It computes sixteen commonly used quantities, including mixing enthalpy, configurational entropy, valence electron concentration, Hume-Rothery electron-to-atom ratio, atomic size mismatch, electronegativity mismatch, and derived stability parameters such as Omega, Lambda, and Phi, and it evaluates eight published prediction criteria. The package combines a curated elemental and binary-interaction dataset with three access modes: a command-line interface (CLI), a desktop graphical user interface (GUI), and a Python application programming interface (API) for programmatic use in notebooks and screening workflows.
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Wednesday 17 June

Materials Science · Cross-listed from physics.chem-ph

LLM-Guided Test-Time Discovery of Quantum-Chemical Approximation Algorithms

Masaya Hagai, Yuta Suzuki, Tomoya Murata et al. (+2 more)

Quantum chemistry simulations underpin modern materials discovery, yet their impact is limited by steep computational cost and dependence on fixed approximation schemes. Foundation models, such as machine-learned interatomic potentials, have accelerated parts of this workflow, but their reliance on large-scale pretraining restricts adaptability at the frontier of chemical space, where methodological innovation and sparse data are the norm. Agentic AI systems can automate existing simulation pipelines, yet they remain constrained by the predefined tools and algorithms they orchestrate. In response, we introduce LADeQ, an LLM-guided workflow that discovers, implements, and benchmarks candidate approximation algorithms at test-time within existing quantum chemistry codes. Rather than selecting from a predefined repertoire, LADeQ constructs candidate approximation schemes on demand, drawing on techniques from disciplines such as spatial statistics, circuit simulation, and kernel methods that have had little prior presence in electronic-structure theory. Because it builds on an out-of-the-box language model, LADeQ requires no task-specific pretraining or curated data, and the resulting implementations are transparent and inspectable, with explicitly traceable approximation errors that enable principled control of accuracy–efficiency trade-offs. We show that LADeQ accelerates coupled cluster singles and doubles (CCSD) and configuration interaction singles and doubles (CISD) calculations while keeping correlation-energy errors within user-specified tolerances, demonstrating autonomous, objective-driven discovery of approximation algorithms inside existing electronic-structure solvers.
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All authors Masaya Hagai, Yuta Suzuki, Tomoya Murata, Shuhei Kurita, Masaki Adachi

Materials Science

Coordination-Sensitive Nanoscale Analysis of Defect-Driven Phase Transformation in Si-Doped (AlXGa1-X)2O3

Shaon Das, Jith Sarker, Christopher Chae et al. (+5 more)

Defect-driven phase instability critically influences the structural reliability of ultrawide bandgap oxides, yet direct nanoscale metrics linking local chemistry to structural transformation remain limited. Here, we introduce a coordination-sensitive atom probe tomography framework that quantitatively resolves reductions in local cation coordination and links them directly to defect-driven phase transformation. Using Si-doped beta-(AlxGa1-x)2O3 heterostructures with controlled Al composition (6-17%) and doping levels (10^17-10^20 cm^-3), we show that gamma-phase inclusions emerge exclusively under the combined conditions of elevated Al content and heavy Si doping. Two-dimensional compositional mapping reveals pronounced lateral Al/Ga inhomogeneity in these regions, while nearest-neighbor and radial distribution analyses quantitatively resolve a significant reduction in first-shell Ga coordination, consistent with local cation deficiency. Correlative scanning transmission electron microscopy confirms that these coordination-depleted regions coincide spatially with gamma-phase inclusions. Density functional theory further supports this mechanism, demonstrating that Al incorporation reduces monoclinic lattice stability and, in conjunction with donor-induced vacancy formation, facilitates vacancy-mediated cation rearrangement and coordination collapse. Together, these results establish coordination loss as a measurable nanoscale signature directly linked to defect-driven phase instability. This framework provides a generalizable approach for probing defect-driven phase instability in doped and alloyed ultrawide bandgap semiconductors.
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All authors Shaon Das, Jith Sarker, Christopher Chae, Lingyu Meng, Joel B. Varley, Hongping Zhao, Jinwoo Hwang, Baishakhi Mazumder

Materials Science

Charge-state control of carbon-related optical absorption in AlN

Helen C. Robinson, Daniil Danilin, Md Shafiqul Islam Mollik et al. (+5 more)

Sub-bandgap optical absorption in AlN between 2 eV and 4 eV is widely observed, but its microscopic origin remains contested. Using photo-induced electron paramagnetic resonance (photo-EPR) and optical absorption spectroscopy on the same samples, we demonstrate a correlation between this absorption band and the neutral charge state of substitutional carbon on the nitrogen site (C$_N$). Hybrid functional calculations of the optical absorption spectra show that a transition involving C$_N$ and the valence band occurs near 3.3 eV, which agrees well with a peak identified within the measured optical absorption between 2 eV and 4 eV. This conclusion requires the combined ability to manipulate the charge state of carbon using photo-EPR and to use first-principles calculations of the absorption line shape that account for the dispersion of the valence band and the energy dependence of the optical matrix elements.
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All authors Helen C. Robinson, Daniil Danilin, Md Shafiqul Islam Mollik, Darshana Wickramaratne, John L. Lyons, Vladimir Fedorov, Sergey Mirov, M.E. Zvanut

Materials Science

Deposition and Growth of the AlCoCuFeNi High-Entropy Alloy Thin Film: Molecular Dynamics Simulation

Oleksandr I. Kushnerov, Valerij F. Bashev and Sergey I. Ryabtsev

The growth of a thin film of a high-entropy AlCoCuFeNi alloy on a silicon (100) substrate was studied using molecular dynamics modeling. The simulation was carried out using the embedded atom model to describe the interactions among Al, Co, Cu, Ni, and Fe atoms. The interaction between Al, Co, Cu, Fe, Ni atoms and the Si substrate was modeled using the Lennard-Jones potential, while the interaction between silicon atoms was described using the Stillinger-Weber potential. The total simulation time was 50 ns. It was found that small clusters were formed at the first stage of deposition and that crystallization started after approximately 5 ns of simulation, when the characteristic cluster size was about 2 nm. At the end of the simulation, after 50 ns of modeling, the simulated film contained face-centered cubic, body-centered cubic, hexagonal close-packed, and amorphous phases. Analysis of the radial distribution function made it possible to determine nearest-neighbor distances and estimate the lattice parameters of these phases.
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Materials Science · Cross-listed from cond-mat.mes-hall

Optical spin injection in graphane and fluorographene

Angélica Marina López-Martínez, César Castillo-Quevedo, Cesar Camas-Flores et al. (+2 more)

We theoretically investigate the optical spin-injection response in different stoichiometric configurations of graphane and fluorographene using density functional theory. Our goal is to determine which configuration yields the strongest degree of spin polarization. The results show that the fluorographene zigzag configuration yields the best degree of spin polarization response (${\cal DSP}^{\mathrm{z}}$), with 98% spin polarized electrons at the band edge and over a wide range of excitation photon energies. In contrast, other graphane and fluorographene configurations achieve a ${\cal DSP}^{\mathrm{z}}$ of roughly 83–100%, but only within a limited photon-excitation energy range. In structures with low spin-orbit coupling, the degree of spin polarization is close to 100% over a wide range of photon energies. For higher spin-orbit coupling, this strong response appears, but only in a narrow photon energy region. Additionally, under the band-resolved decomposition scheme, the contributions of different band-to-band transitions to the ${\cal DSP}^{\mathrm{z}}$ spectrum are identified by summing only the selected valence and conduction bands. Our findings show that almost the entire ${\cal DSP}^{\mathrm{z}}$ spectrum of the fluorographene zigzag configuration comes from transitions that involve only the top valence band, which is a mixture of C–p and F–p states.
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All authors Angélica Marina López-Martínez, César Castillo-Quevedo, Cesar Camas-Flores, Analila Luna-Valenzuela, Jose Luis Cabellos

Materials Science · Cross-listed from math.NA

Moreau-Yosida-based Kohn-Sham Inversion for Periodic Systems

Vebjørn H. Bakkestuen, Michael F. Herbst, Vegard Falmår et al. (+2 more)

Density-potential inversion for periodic systems within Moreau-Yosida-regularised density-functional theory is investigated, both theoretically and numerically. We develop the framework in a periodic homogeneous Sobolev space and use it to recover the exchange-correlation potential of Kohn-Sham theory through a limiting procedure. A key analytical ingredient is the proof of lower semicontinuity of the non-interacting kinetic-energy functional in the chosen topology. The proximal mapping, together with its algorithmic evaluation, plays a central role in the resulting inversion scheme. Numerical experiments illustrate the performance and properties of the method for both the Kohn-Sham and Gross-Pitaevskii equations.
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All authors Vebjørn H. Bakkestuen, Michael F. Herbst, Vegard Falmår, Markus Penz, Andre Laestadius

Materials Science

Spin point group symmetry and classification of non-relativistic spin splitting in non-collinear magnetic structures: Identification of high-order spin splitting types (l=5,7, and 9)

Luis Elcoro, Jesus Etxebarria, J. Manuel Perez-Mato et al. (+1 more)

A comprehensive study of the possible types of non-relativistic spin splitting of electronic bands in coplanar and non-coplanar magnetic structures is presented on the basis of spin-group theory. First, we tabulate all non-equivalent spin point groups (SpPGs) which can be expressed as a direct product of a nontrivial part and a spin-only group limited to be the intrinsic (trivial) one, or augmented by the time-reversal (TR) operation. This tabulation, which includes the listing of symmetry operations for 1249 nonequivalent SpPGs, is now available as an online database SPGENPOS in the Bilbao Crystallographic Server (BCS). This extends previous enumerations, in which the possible presence of TR in the magnetic point group was not taken into account, thus overlooking the full SpPG symmetry associated with the numerous magnetic structures which have a magnetic space group of type IV. For each of the listed coplanar and non-coplanar SpPGs, the spin-splitting that is symmetry allowed is analyzed in detail using the program STENSOR also in the BCS. Except for the SpPGs that include the operation 1', i.e., the combined operation of TR and space inversion, all other coplanar and non-coplanar SpPGs allow spin splitting at some order in a power expansion of the electron wave vector components. We find that, depending on the SpPG, spin-splitting terms can appear with the lowest-order monomials ranging from l=0 to 9, with the exception of l=8. This contrasts with the collinear case, where the lowest order is not higher than l=6, and where TR forbids any spin splitting. For the newly identified spin textures with powers l=5, 7, and 9, which are possible in some noncentrosymmetric SpPGs, the functional form of the spin splitting in terms of the components of the crystal momentum is given. One example of a real material, LaMnAu5, showing l=5 spin splitting is identified.
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All authors Luis Elcoro, Jesus Etxebarria, J. Manuel Perez-Mato, Emre S. Tasci

Materials Science

Direct large-area observation of subsurface plastic activity in conditioned copper electrodes

Yinon Ashkenazy, Inna Popov, Victoria M. Bjelland et al. (+2 more)

High-field conditioning is the process by which radio-frequency structures in particle accelerators and other high-gradient devices reach their operating fields, yet the underlying physical mechanism remains an open question. Models and indirect measurements point to subsurface dislocation dynamics, but large-area structural measurements have been missing. We present electron backscatter diffraction measurements spanning millimeter-scale regions on a copper cathode conditioned at pulsed direct-current fields up to $\sim$80~MV/m in a sloped-anode geometry, which imposes a known gradient of field exposure across a single electrode. Across nine regions of interest spanning this exposure range, the mean intragrain misorientation of field-exposed regions exceeds that of unexposed references by $\sim$75%; the difference is reproduced by three independent misorientation metrics and confirmed by Kolmogorov–Smirnov tests. To our knowledge, this is the first large-area observation of structural differences between conditioned and unconditioned regions of a high-field electrode. The misorientation separates into three tiers (high-field center and edge, low-field periphery, and unexposed reference) that match the spatial profile of the conditioning-state variable $E_S$ predicted by Monte Carlo simulations. These observations point to the evolving subsurface dislocation population as a candidate physical basis of conditioning.
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All authors Yinon Ashkenazy, Inna Popov, Victoria M. Bjelland, William L. Millar, Walter Wuensch

Materials Science

AdsMind: A Physics-Grounded Multi-Agent System for Self-Correcting Discovery of Adsorption Configurations on Heterogeneous Catalyst Surfaces

Zongmin Zhang, Yuyang Lou, Bowen Zhang et al. (+6 more)

Identifying the lowest-energy surface-adsorbate configuration is critical for modeling heterogeneous catalysis, yet exhaustive exploration with ab initio calculations is computationally prohibitive. Machine-learning force fields (MLFFs) accelerate structural relaxation but leave the search over the vast configurational space a major bottleneck, and open-loop large language model (LLM) agents lack a physics-grounded feedback mechanism to correct erroneous initial guesses. We propose AdsMind (Adsorption configuration discovery with Machine intelligence and relaxation feedback), a closed-loop multi-agent framework that enables autonomous error correction through MLFF relaxation feedback. Across four LLM backends, AdsMind achieves consistently high search reliability, with success rates of 100% and 98.8% on the benchmarks AA20 and OCD-GMAE62. Relative to its single-pass (1-Shot) ablation it reduces cross-backend energy dispersion, and it uses only 4.11 and 4.67 MLFF relaxations per case, respectively – an approximately 14-fold reduction over heuristic enumeration baselines. Density functional theory (DFT) validation using VASP/PBE on six representative AA20 systems shows that the reported open-loop Adsorb-Agent outputs exhibit qualitative adsorption-energy sign errors for molecular adsorbates, whereas AdsMind preserves the correct sign in all tested cases with closer quantitative agreement. AdsMind thus delivers reliability, self-reflection, and interpretability simultaneously, supporting more DFT-informed autonomous chemistry workflows.
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All authors Zongmin Zhang, Yuyang Lou, Bowen Zhang, Junwu Chen, Ryo Kuroki, Xuan Vu Nguyen, Edvin Fako, Lixue Cheng, Philippe Schwaller

Materials Science

Controllable Growth and Characterization of {\alpha}- and {\beta}-phase MnSe by Chemical Vapor Deposition

Jennifer E. DeMell, Elias Kallon, Michael Pedowitz et al. (+3 more)

Manganese selenide (MnSe) is a promising air-stable two-dimensional magnetic semiconductor for which theory predicts robust ferromagnetism in monolayers with Curie temperatures approaching 250 K. However, the crystallographic phases and magnetic properties of thin-film MnSe grown by scalable methods remain poorly understood. Here, we demonstrate the controllable growth of ${\alpha}$- and ${\beta}$-phase MnSe on C-face sapphire using a three-zone chemical vapor deposition process with elemental Se and ${MnCl_{2}}$ precursors in an $Ar/{H_{2}}$ atmosphere. Using Raman spectroscopy, atomic force microscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy, we show that our process yields phase-pure ${\alpha}$-MnSe nanorods and ${\beta}$-MnSe triangular flakes with lateral sizes up to 20 ${\mu}m$ and thicknesses of 15-30 nm. Low-temperature photoluminescence of the ${\beta}$-phase films reveals a bandgap of approximately 2.0 eV. Systematic variation of growth parameters shows that precursor vapor pressure, rather than ${H_{2}}$ partial pressure, is the dominant factor controlling lateral flake size. Vibrating-sample magnetometry measurements reveal a $N{\'e}el$ temperature of 53 K in the ${\beta}$-phase films, providing clear evidence of antiferromagnetism in the multilayer regime and establishing MnSe as a tunable platform for 2D spintronic and optoelectronic devices.
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All authors Jennifer E. DeMell, Elias Kallon, Michael Pedowitz, Jimmy C. Kostakidis, Ihteyaz Aqaeed Avash, Kevin M. Daniels

Materials Science · Cross-listed from physics.optics

Equivariant Graph Neural Networks Improve Optical Spectra Prediction for Materials Screening

Kasper Helverskov Petersen, François R J Cornet, Martin Ovesen et al. (+3 more)

Scalable prediction of optical spectra is a critical component of high-throughput materials screening for optoelectronic applications such as solar cells. Existing surrogate models are trained on spectra computed from lower levels of theory or rely on rotation-invariant scalar features, limiting their geometric expressiveness. We explore the use of equivariant graph neural networks for optical spectra prediction, adapting GotenNet to this task and evaluating it on multiple datasets including a recently published collection of 10,533 structures with spectra computed at the level of the random phase approximation (RPA). The proposed model outperforms the current state of the art, with the largest gains in the 0-8 eV range and on predicting the static real permittivity, both of particular relevance for thin-film optics.
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All authors Kasper Helverskov Petersen, François R J Cornet, Martin Ovesen, Mikkel Jordahn, Kristian S. Thygesen, Mikkel N. Schmidt

Materials Science

Generalized deformation potential and machine-learning approaches for electron-phonon coupling and thermoelectric transport in semiconductors

Ransell D'Souza and Ivana Savic

The ability to compute electron-phonon coupling from first principles, using density functional perturbation theory and interpolation techniques, has enabled predictive calculations of electronic transport coefficients in crystalline materials. However, these methods are still computationally expensive. Here we present two inexpensive methods to obtain thermoelectric transport properties of semiconductors using a small number of electron-phonon matrix elements calculated from first principles. The first method combines models for coupling of electrons with different phonon modes whose parameters are obtained from $\sim 10$ matrix elements per electronic band and phonon mode calculated from first principles. Within this method, we formulate the acoustic deformation potential model for arbitrary crystal symmetries and band extrema locations. The second method uses machine learning to interpolate $\sim 100$ electron-phonon matrix elements per electronic band and phonon mode on dense reciprocal space grids in the parts of the Brillouin zone relevant for transport. We apply both methods to two-dimensional MoS$_2$ and show very good agreement with the state-of-the-art method. The calculated thermoelectric properties also agree well with experiments. We find that the machine-learning method is more accurate and straightforward to implement compared to the model approach.
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