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Physics Condensed Matter Materials Science

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Tuesday 17 February

Materials Science

Ligand Mediated Magnetic Coupling Across Metamagnetic Transitions in CrPS4

Giuseppe Buccoliero, Rachel Nickel, Roberto Sant et al. (+8 more)

Chromium thiophosphate (CrPS4) is a long-known material: a layered semiconducting antiferromagnet. Its recently discovered gate-tunable metamagnetic phase transitions, the remarkable positive and oscillating magnetoresistance as a tunnel barrier, and its Fano-resonance luminescence, elusive among the multitude of Cr3+ compounds, call for revisiting the understanding of its electronic structure, especially regarding how it relates to magnetic order. Here, we employ X-ray magnetic circular dichroism, implemented in both absorption and resonant inelastic X-ray spectroscopies, together with quantum many-body calculations, to unveil the role of metal-ligand covalency in mediating the metamagnetic transitions in CrPS4, using crystal-field and charge-transfer excitations as fingerprints of the evolving magnetic order. We reveal the role of extended superexchange paths involving P and S atoms, coupling interactions between the Cr spins across the different magnetic phases: antiferromagnetic, canted, and ferromagnetic. Our results elucidate the electronic states involved in these phases and provide prescriptions for engineering the metamagnetic phase diagram of CrPS4.
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All authors Giuseppe Buccoliero, Rachel Nickel, Roberto Sant, Marli dos Reis Cantarino, Andrei Rogalev, Nathan J. Yutronkie, Tristan Riccardi, Daniel A. Chaney, Kurt Kummer, Johann Coraux, Nicholas B. Brookes

Materials Science

Twist-induced Out-of-plane Ferroelectricity in Bilayer Hafnia

Jian Huang, Gwan Yeong Jung, Pravan Omprakash et al. (+6 more)

Ferroelectric HfO2 is a promising candidate for next-generation memory devices due to its CMOS compatibility and ability to retain polarization at nanometer scales. However, the polar orthorhombic phase (Pca2_1) responsible for ferroelectricity is metastable and requires extrinsic stabilization, which makes it challenging for integration with silicon. We predict that bilayer 1T-HfO2 can exhibit robust and switchable out-of-plane (OOP) polarization arising from stacking-induced symmetry breaking. Using first-principles density functional theory, we predict that monolayer 1T-HfO2 can be cleaved from the (111) surface of cubic hafnia, and the monolayer is dynamically stable. When two aligned monolayers are twisted to form a moiré superlattice, it breaks the interlayer symmetry and allows the emergence of bistable OOP polarization. At a twist angle of 7.34o, the system exhibits a net polarization of ~16 {\mu}C/cm2. This sizeable polarization is due to the large polar displacements concentrated in AB stacking domains. Importantly, this polarization can be reversibly switched via interlayer sliding with a low energy barrier (~8 meV/formula unit) and comparable low coercive field (~0.2 V/nm), offering electric-field tunability. These findings establish twisted bilayer 1T-HfO2 as a scalable and robust 2D ferroelectric platform, enabling new pathways for integrating ferroelectric functionality into atomically thin memory and logic devices.
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All authors Jian Huang, Gwan Yeong Jung, Pravan Omprakash, Guodong Ren, Xin Li, Du Li, Xiaoshan Xu, Li Yang, Rohan Mishra

Materials Science · Cross-listed from cs.LG

MolCrystalFlow: Molecular Crystal Structure Prediction via Flow Matching

Cheng Zeng, Harry W. Sullivan, Thomas Egg et al. (+8 more)

Molecular crystal structure prediction represents a grand challenge in computational chemistry due to large sizes of constituent molecules and complex intra- and intermolecular interactions. While generative modeling has revolutionized structure discovery for molecules, inorganic solids, and metal-organic frameworks, extending such approaches to fully periodic molecular crystals is still elusive. Here, we present MolCrystalFlow, a flow-based generative model for molecular crystal structure prediction. The framework disentangles intramolecular complexity from intermolecular packing by embedding molecules as rigid bodies and jointly learning the lattice matrix, molecular orientations, and centroid positions. Centroids and orientations are represented on their native Riemannian manifolds, allowing geodesic flow construction and graph neural network operations that respects geometric symmetries. We benchmark our model against a state-of-the-art generative model (MOFFlow) for large-size periodic crystals and a rule-based structure generation method (Genarris) on two open-source molecular crystal datasets. MolCrystalFlow outperforms MOFFlow while achieving competitive performance against Genarris. We also demonstrate an integration of MolCrystalFlow model with universal machine learning potential to accelerate molecular crystal structure prediction, paving the way for data-driven generative discovery of molecular crystals.
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All authors Cheng Zeng, Harry W. Sullivan, Thomas Egg, Maya M. Martirossyan, Philipp Höllmer, Jirui Jin, Richard G. Hennig, Adrian Roitberg, Stefano Martiniani, Ellad B. Tadmor, Mingjie Liu

Materials Science · Cross-listed from cond-mat.str-el

Zero Indirect Band Gap and Flat Bands in a Niobium Oxyiodide Cluster Material

Jan Beitlberger, Mario Martin, Marcus Scheele et al. (+4 more)

Explorative chemistry in a reaction system composed of NbI$_4$, Li$_2$(CN$_2$), and Li$_2$O has led to the discovery of a number of niobium oxyiodide cluster compounds. During this reaction, the formation of solid phases was detected alongside with gaseous phases, resulting in a range of products with cluster cores of varying shapes. After several niobium oxyiodide cluster compounds have already been identified within this reaction system, two additional compounds, Nb$_6$O$_3$I$_{15}$ and Nb$_{11}$O$_6$I$_{24}$, are discovered and structurally characterized by single-crystal X-ray diffraction. Both structures are based on the butterfly-shaped, oxygen-capped niobium cluster [Nb$_4$O], which is extended to larger cluster fragments. The [Nb$_4$O] cluster core in Nb$_6$O$_3$I$_{15}$is extended by two [NbO] units to form a three-dimensional framework, and Nb$_{11}$O$_6$I$_{24}$ contains two connected [Nb$_4$O] units, which form chiral units within an antiferrochiral hexagonal packing of strings. The striking string-like character of Nb$_{11}$O$_6$I$_{24}$ was investigated in terms of its electronic structure and properties. DFT calculations showed Nb$_{11}$O$_6$I$_{24}$ to possess a zero indirect band gap, with a pair of 3-dimensional flat bands surrounding the Fermi level. These unusual features of the electronic band structure suggest the presence of strongly correlated inter-cluster singlet electron states, arising from the helical shape of the clusters, the hexagonal packing of the strings, and the delocalized nature of cluster electron wavefunctions.
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All authors Jan Beitlberger, Mario Martin, Marcus Scheele, Marek Matas, Carl P. Romao, Markus Ströbele, H.-Jürgen Meyer

Materials Science

Stochastic Modeling of Anisotropic Strength Surfaces from Atomistic Simulations

Alexander Bonacci, John Dolbow and Johann Guilleminot

This work develops a unified framework for inferring, representing, and statistically characterizing an anisotropic strength surface directly from molecular dynamics data. Large-scale tensile loading simulations are used to generate failure data across all principal stress ratios and loading orientations, facilitated by a data-driven mapping between imposed strain-rate tensors and resulting stresses. The orientation-dependent strength surface is then represented using a constrained parametric formulation in which the surface parameters vary smoothly with loading angle through a low-dimensional functional encoding. To deploy the framework, we specifically consider the case of monocrystalline graphene, which is a prototypical two-dimensional material that has been extensively characterized, both experimentally and computationally, in the literature. For defective graphene, multiple random realizations of vacancy defect distributions are used to construct a stochastic ensemble of angular strength surfaces. Because each anisotropic strength surface requires substantial atomistic sampling to construct, the resulting ensemble is inherently limited in size, motivating the use of compact encoding, dimensionality reduction, and probabilistic modeling to characterize strength variability. Dimensionality reduction via Principal Component Analysis reveals a condensed latent representation of the fitted, encoded surfaces, where a Gaussian mixture model is employed to capture defect-induced variability, including rare outlier behaviors arising from clustered vacancy defects. Sampling from this probabilistic model enables the generation of new, physically admissible strength surfaces and the construction of confidence intervals in both parameter space and stress space. (Abstract shortened to meet arXiv limits.)
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Materials Science · Cross-listed from cond-mat.supr-con

Uniaxial stress enhanced anisotropic magnetoresistance and superconductivity in the kagome superconductor LaRu$_{3}$Si$_{2}$

P. Král, V. Sazgari, Yongheng Ge et al. (+10 more)

Elucidating the role of the kagome electronic structure in determining the various quantum ground states is of fundamental importance. In this work, we employ in-plane uniaxial stress as a tuning parameter to probe the electronic structure and its impact on the superconducting and normal-state properties of the kagome superconductor LaRu$_{3}$Si$_{2}$, combining magnetotransport measurements with first-principles calculations. We identify a pronounced anisotropy in both the upper critical field and the normal-state magnetoresistance, indicating strong electronic anisotropy despite the three-dimensional crystal structure. Furthermore, we find that the superconducting transition temperature $T_{\rm c}$ increases under in-plane stress applied within the kagome plane, although the enhancement is modest, reaching approximately 0.3 K at 0.6 GPa. Furthermore, the absolute magnetoresistance exhibits a pronounced increase from about 22${\%}$ at zero stress to 35${\%}$ at 0.6 GPa, indicating a substantial modification of the normal state above $T_{\rm c}$. Previous studies have reported time-reversal-symmetry (TRS) breaking below a temperature scale that coincides with the onset of magnetoresistance. The simultaneous enhancement of both $T_{\rm c}$ and magnetoresistance under stress therefore suggests a positive correlation between superconductivity and normal-state electronic and magnetic properties in LaRu$_{3}$Si$_{2}$. Detailed calculations demonstrate that stress-induced changes in $T_{\rm c}$ arise from the joint evolution of the total density of states and the flat band, whereas the large magnetoresistance enhancement is dominated by the stress-driven downward shift of the Ru $dz^{2}$ kagome flat band.
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All authors P. Král, V. Sazgari, Yongheng Ge, O. Gerguri, M. Spitaler, J.N. Graham, H. Nakamura, M. Bartkowiak, S. Nakatsuji, H. Luetkens, G. Simutis, Gang Xu, Z. Guguchia

Materials Science

A fully differentiable framework for training proxy Exchange Correlation Functionals for periodic systems

Rakshit Kumar Singh, Aryan Amit Barsainyan and Bharath Ramsundar

Density Functional Theory (DFT) is widely used for first-principles simulations in chemistry and materials science, but its computational cost remains a key limitation for large systems. Motivated by recent advances in ML-based exchange-correlation (XC) functionals, this paper introduces a differentiable framework that integrates machine learning models into density functional theory (DFT) for solids and other periodic systems. The framework defines a clean API for neural network models that can act as drop in replacements for conventional exchange-correlation (XC) functionals and enables gradients to flow through the full self-consistent DFT workflow. The framework is implemented in Python using a PyTorch backend, making it fully differentiable and easy to use with standard deep learning tools. We integrate the implementation with the DeepChem library to promote the reuse of established models and to lower the barrier for experimentation. In initial benchmarks against established electronic structure packages (GPAW and PySCF), our models achieve relative errors on the order of 5-10%.
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Materials Science

Three-Dimensional Optical-Electrical Simulation of Cs2AgBiBr6 Double Perovskite Solar Cells

Md Shanian Moed, Adnan Amin Siddiquee and Md Tashfiq Bin Kashem

Despite significant advances in lead-free perovskite photovoltaics, achieving a balance among environmental safety and high optoelectronic performance remains challenging. The inorganic double perovskite Cs2AgBiBr6 has emerged as a promising candidate owing to its robust three-dimensional crystal structure and suitable visible-range bandgap. However, best power conversion efficiencies (PCEs) for Cs2AgBiBr6 solar cells reported so far - 6.37% experimentally and 27.78% in numerical studies - remain below the theoretical performance potential, largely due to suboptimal charge transport layers, and interface-related recombination losses. Here, we address this gap using a 3D finite-element method (FEM) implemented in COMSOL Multiphysics, which couples optical simulations with semiconductor drift-diffusion transport. To our knowledge, this work represents the first comprehensive 3D FEM-based study of a double halide perovskite solar cell. Screening of 25 electron transport layer (ETL)-hole transport layer (HTL) combinations identifies CeO2 and P3HT as the optimal ETL and HTL respectively. Device performance is further analyzed through systematic variation of layer thicknesses, doping concentrations and defect densities within the FTO/CeO2/Cs2AgBiBr6/P3HT/Au architecture. Under optimized parameters, the simulated device achieves a PCE of 31.76%, representing the theoretical upper bound predicted by the model. Overall, this work demonstrates 3D physics-based device engineering as a decisive pathway for overcoming efficiency bottlenecks in lead-free double perovskite photovoltaics.
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Materials Science

Revealing 3D Strain and Carbide Architectures in Additively Manufactured Ni Superalloys

James A. D. Ball, David M. Collins, Yuanbo T. Tang et al. (+4 more)

Fast directional solidification during Laser Additive Manufacturing (LAM) produces a complex microstructure in nickel-based superalloys, comprising columnar grains with cellular sub-grain structures and carbides. Using non-destructive Scanning 3D X-ray Diffraction (S3DXRD), we reveal spatially complex orientation and intergranular strain relationships that couple strongly to processing-induced cellular sub-grain networks and a primary cubic metal carbide (MC) phase. We have examined 3D orientation and elastic strain tensor fields across 82 $\gamma$ grains together with the spatial distribution of over 37,000 MC carbides in an ABD-900AM alloy sample manufactured by the Directed Energy Deposition (DED) LAM process. Carbides are spatially associated with the cellular sub-grain network with a weak but present orientation relationship with their parent $\gamma$ grains. The MC carbides, known to be Ti, Ta and Nb rich, form in regions of high solute segregation, resulting in a significant volumetric lattice parameter patterning in the associated $\gamma$ phase regions. These chemically distinct solute-rich regions possess a higher associated elastic modulus compared to intercellular regions and determine the local residual stress patterning. These results provide the first non-destructive 3D study of the relationship between rapid solidification-induced segregation, deformation heterogeneity and carbide architectures in an additively manufactured Ni-based superalloy. The insights provide crucial detail to rationalise LAM process parameter optimisation and the coupled spatially governed structural performance.
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All authors James A. D. Ball, David M. Collins, Yuanbo T. Tang, Jonathan P. Wright, Can Yildirim, Julia Richter, Yunhui Chen

Materials Science

Planar Structures of Medium-Sized Gold Clusters Become Ground States upon Ionization

Mohammad Ismaeil Safa, Ehsan Rahmatizad Khajehpasha and Stefan Goedecker

This study investigates the structural stability of ionized gold clusters of sizes ranging from 22 to 100 atoms, contrasting compact, cage and planar structures. While it is well known that neutral clusters in the upper part of this size range predominantly favor compact structures, our results reveal that positively ionized gold clusters exhibit structural transitions in which planar structures become energetically preferred once the charge is sufficiently large. In addition, we study the finite-temperature stability of the structures and find that thermodynamic effects further stabilize planar configurations relative to their compact counterparts. To explore the potential energy surface, we use the Minima Hopping algorithm combined with a machine-learned potential. Since the machine-learned potential does not apply to ionized clusters, we introduce a charge-correction term to incorporate Coulomb interactions and charge screening.
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Materials Science

Neel temperature and helical spin order of altermagnetic RuO2

Markus Meinert

The magnetic groundstate of RuO$_2$ remains controversial, with experimental evidence for a nonmagnetic groundstate of ideal bulk material and indications of a magnetic state in strained thin films. Here, I investigate the Néel temperature of the (hypothetical) altermagnetic state of bulk RuO$_2$, stabilized via the DFT$+U$ technique, by mapping on a Heisenberg Hamiltonian. The Néel temperature scales monotonously with the magnetic moment up to the point where a large $+U$ term opens a band gap and turns RuO$_2$ semiconducting. The maximum Néel temperature obtained by this procedure is 408\,K at $U=3$\,eV, and much smaller values for smaller $U$. A reciprocal-space eigenvalue analysis reveals a helimagnetic groundstate of the spin model due to intra-sublattice antiferromagnetic coupling. This situation resembles the isostructural $\beta$-MnO$_2$, which is a prototype helimagnet. Further comparison with calculations on CrO$_2$ and altermagnetic MnF$_2$ taking $U$ as an adjustable parameter supports the validity of the spin model analysis.
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Materials Science

Reactive Coarse Grained Force Field for Metal-Organic Frameworks applied to Modeling ZIF-8 Self-Assembly

Sangita Mondal, Cecilia M. S. Alvares and Rocio Semino

Decoding the self-assembly mechanism of metal-organic frameworks is a crucial step in reducing trial-and-error tests in their synthesis protocols. Atomistic simulations have proven essential in revealing molecular-level features of MOF nucleation, but they still exhibit limitations in the simulation setups due to size constraints (inability of reaching realistic concentrations or exploring non-stoichiometric metal:ligand ratios). In this contribution, we develop a methodology to derive reactive coarse grained force fields based on multiscale coarse graining methods. We apply our novel methodology to the case of the archetypal zeolitic-imidazolate framework ZIF-8. Our coarse grained force field, which we call nb-CG-ZIF-FF, does not contain any explicit connectivity information, but learns the tetrahedral Zn-connectivity from many body correlations within an atomistic benchmark. nb-CG-ZIF-FF quantitatively reproduces the features of bulk, crystalline ZIF-8 as well as the structural evolution of pre-nucleation species in terms of Zn n-fold coordination populations from the atomistic benchmark. While the range of rings that are formed along the synthesis process are well captured by nb-CG-ZIF-FF, the model cannot exactly reproduce ring populations. Our reactive CG force field fitting approach can be applied to any MOF, opening new research avenues in modeling MOF formation, decomposition, defect dynamics and phase transition processes.
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Materials Science · Cross-listed from cond-mat.str-el

Electric-field-tuned consecutive topological phase transitions between distinct correlated insulators in moire MoTe2/WSe2 heterobilayer

Xumin Chang, Zui Tao, Bowen Shen et al. (+10 more)

Consecutive topological phase transitions (TPTs) between strongly correlated electronic phases that differ simultaneously in symmetry breaking and topological order are of fundamental interest in condensed matter physics, yet are rarely realized experimentally. We report two consecutive electric-field-driven TPTs at half filling (nu = 1) in angle-aligned MoTe2/WSe2 moire heterobilayers. With increasing out-of-plane displacement field, a geometrically frustrated Mott insulator evolves into a ferromagnetic quantum anomalous Hall (QAH) Mott insulator, i.e., a spin-polarized topological Mott insulator without an observable charge-gap closure, and subsequently into an antiferromagnetic, valley-coherent Mott insulator (VC-AFM) accompanied by a continuous charge-gap collapse and the emergence of a critical metallic state. Layer-resolved magnetic circular dichroism (MCD), magneto-transport, and compressibility measurements jointly determine the phase diagram. The high-field evolution of the antiferromagnetic state reveals a metamagnetic-like transition at a critical field B*, above which a Chern insulating transport response reappears. Our results establish the MoTe2/WSe2 moire platform as a tunable realization of an extended Kane-Mele-Hubbard model hosting sequential correlation-topology-intertwined transitions.
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All authors Xumin Chang, Zui Tao, Bowen Shen, Wanghao Tian, Jenny Hu, Kateryna Pistunova, Kenji Watanabe, Takashi Taniguchi, Tony F. Heinz, Tingxin Li, Kin Fai Mak, Jie Shan, Shengwei Jiang

Materials Science

Hydrostatic Pressure-enhanced correlated magnetism and Chern insulator in moir'e WSe2

Pengfei Jiao, Chenghao Qian, Ning Mao et al. (+24 more)

Moiré semiconductors offer flat bands where Coulomb interactions and band topology intertwine, while interlayer coupling plays a central role in forming the moiré potential. However, limited interlayer coupling strength and the lack of efficient tuning methods hinder further exploration of correlated phenomena in moiré semiconductors. Here we introduce a cryogenic dual-gated diamond-anvil platform using helium as a pressure medium, enabling reversible hydrostatic tuning together with magneto-optical spectroscopy in twisted bilayer WSe2. Pressure enhances the moiré potential, redshifts excitons, and stabilizes Stoner ferromagnetism otherwise absent at a 3.1-degree twist. Simultaneously, the half-filled C = 1 Chern insulating state strengthens, exhibiting a reduced saturation field. Moreover, we observe a topological phase transition from a Chern insulator to a Mott insulator at around 2 GPa. First-principles calculations reveal that a Gamma-to-K valence-band-maximum switching drives this transition by converting an Ising-like topological K-valley miniband into a spin-degenerate trivial Gamma miniband. Our findings demonstrate hydrostatic pressure as a powerful, continuous control axis for correlated magnetism and topological band engineering in moiré materials.
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All authors Pengfei Jiao, Chenghao Qian, Ning Mao, Xumin Chang, Jiayong Xiao, Feng Liu, Shaozheng Wang, Xiaokai Wu, Di Peng, Cheng Xu, Hongliang Dong, Yuchen Zheng, Juncai Wu, Tong Zheng, Kenji Watanabe, Takashi Taniguchi, Jinfeng Jia, Xiaoxue Liu, Zhiwen Shi, Shiyong Wang, Guorui Chen, Tingxin Li, Ruidan Zhong, Yang Zhang, Dong Qian, Zhiqiang Chen, Shengwei Jiang

Materials Science

On the origin of in-gap states in amorphous Ge$_2$Sb$_2$Te$_5$

Omar Abou El Kheir and Marco Bernasconi

The localized states in the band gap of amorphous phase change alloys like Ge$_2$Sb$_2$Te$_5$ control the electrical conduction via the Poole-Frenkel mechanism. Understanding the origin of in-gap states and their evolution in time during aging of the glass is therefore important for the control of the resistance drift in phase change memory devices. Here, we use a machine learning interatomic potential to generate several models of Ge$_2$Sb$_2$Te$_5$ whose electronic structure is then analyzed within density functional theory with a hybrid functional. A detailed statistical analysis of the structural motifs on which the in-gap states are localized, reveals that the vast majority of in-gap states involve wrong bonds (homopolar or Ge-Sb bonds) often accompanied by Ge in tetrahedral configurations or overcoordinated Ge and Sb atoms. Metadynamics simulations mimicking glass aging support the picture that structural relaxations lead to the depletion of in-gap states and then to an increase of resistance. The simulations thus provide important insights for the mitigation of the resistance drift in phase change memory devices.
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Materials Science · Cross-listed from cond-mat.mes-hall

Isotope effect in the work function of lithium

Atef A. Sheekhoon, Abdelrahman O. Haridy and Vitaly V. Kresin

The work functions of 7Li and 6Li metals have been measured as a function of temperature, by using photoionization of pure isolated metal nanoparticles in a beam. These data reveal a marked isotope effect in the temperature variation of these work functions. Furthermore, for both isotopes the curvature of this temperature variation is found to be significantly larger than may be ascribed purely to a change in the electron gas density. These findings enhance the characterization of lithium as a quantum material in which the interplay between electronic and ionic degrees of freedom is nontrivial, and call for a microscopic understanding beyond simple models. Additionally, the slope of the work function curves was observed to vanish in the low temperature limit, as had been predicted on the basis of the Third Law of thermodynamics.
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Materials Science · Cross-listed from cond-mat.mes-hall

Temperature-dependent photoionization thresholds of alkali-metal nanoparticles reveal thermal expansion and the melting transition

Abdelrahman O. Haridy, Atef A. Sheekhoon and Vitaly V. Kresin

A precision measurement of the photoionization of pure sodium and potassium nanoparticles isolated in a beam enabled an accurate determination of their work functions as a function of temperature. In addition to resolving and quantifying the initial gradual decrease of the work function with temperature, which is associated with thermal expansion, the experiment revealed that the work function then undergoes a distinct drop both in magnitude and in slope that signifies the onset of nanoparticle melting. This establishes that a structural phase transition can be detected via a high-resolution measurement of the photoemission threshold. The melting temperature of nanoparticles with diameters of 7-9 nm is reduced by nearly 100 K relative to the bulk value. This suppression aligns with predictions from the Gibbs-Thomson equation which describes finite-size phase transitions.
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Materials Science · Cross-listed from cond-mat.mes-hall

Photoionization of temperature-controlled nanoparticles in a beam: Accurate and efficient determination of ionization energies and work functions

Atef A. Sheekhoon, Abdelrahman O. Haridy, Sebastian Pedalino et al. (+1 more)

A beam of free alkali metal nanoparticles is produced by a condensation source, passed through a thermalizing tube adjustable over a broad temperature range, and ionized by tunable light. High stability of the particle flux and an automated data acquisition routine allow efficient collection of photoionization yield curves. A careful fit of the data to the universal Fowler function makes it possible to obtain nanoparticle ionization energies, and from those, the metal work functions, with $\sim$0.2% precision. The experimental arrangement, nanoparticle thermalization rates, and ionization threshold analysis are described in detail. The use of ultrapure and temperature-controlled gas-phase nanoparticles facilitates the analysis of electronic properties, such as work functions, and of their interplay with thermal lattice dynamics.
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All authors Atef A. Sheekhoon, Abdelrahman O. Haridy, Sebastian Pedalino, Vitaly V. Kresin

Materials Science

Intrinsic low-spin state and strain-tunable anomalous Hall scaling in high-quality SrRuO3 (111) films

Harunori Shiratani, Yuki K. Wakabayashi, Yoshiharu Krockenberger et al. (+6 more)

The (111)-oriented 4d ferromagnetic perovskite SrRuO3 (SRO) offers a unique triangular-lattice geometry, making it a promising platform for exploring Berry-curvature-driven and spin-orbit-coupled transport. Here, we present a systematic study of the structure, magnetism, and magnetotransport of high-quality SRO (111) thin films with thicknesses t = 1.2-60 nm grown on SrTiO3 (111) substrates by machine-learning-assisted molecular beam epitaxy. We achieved a residual resistivity ratio of 45.5 in a 60 nm-thick film, the highest reported for this orientation, enabling access to intrinsic electronic and magnetic behavior. Temperature-dependent resistivity confirms Fermi-liquid transport below 15 K in both coherently strained (t = 10, 20 nm) and strain-relaxed (t = 60 nm) films, thereby enabling detailed magnetotransport and magnetic measurements. The linear, non-saturating positive magnetoresistance persists up to 14 T, while Hall-effect measurements and temperature scaling separate intrinsic (Karplus-Luttinger) and extrinsic (side-jump) contributions to the anomalous Hall effect, with the relative weight tuned by (111) epitaxial strain. X-ray magnetic circular dichroism at the Ru M2,3 and O K edges, together with SQUID magnetometry, demonstrates an intrinsically low-spin Ru ground state for both coherently strained and relaxed films, resolving ambiguities among prior reports. These detailed crystalline, electrical, and magnetic characterizations provide a rigorous foundation for understanding and engineering quantum transport in SRO (111).
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All authors Harunori Shiratani, Yuki K. Wakabayashi, Yoshiharu Krockenberger, Masaki Kobayashi, Kohei Yamagami, Takahito Takeda, Shinobu Ohya, Masaaki Tanaka, Yoshitaka Taniyasu

Materials Science

A brief review of high-entropy oxides in solid oxide fuel cell applications

Yueyuan Gu, Juan Shi, Dilshod Nematov et al. (+4 more)

Solid oxide fuel cells are efficient energy conversion devices essential to clean energy development, yet their broad application is limited by material challenges, including sluggish oxygen reduction kinetics at intermediate temperatures, electrode instability and vulnerability to contaminants. High-entropy oxides, a novel class of materials characterized by multiple principal elements and high configurational entropy, present a promising approach to overcome these issues via their distinctive "four core effects". This review begins with the fundamentals of high-entropy materials, covering their definition, phase stabilization mechanisms, and relevant descriptors, then systematically reviews their progress as SOFC cathodes, electrolytes, and anodes. Key advances are summarized, and current challenges are analyzed, offering guidance for the design of high-performance and stable high-entropy oxides for solid oxide fuel cells.
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All authors Yueyuan Gu, Juan Shi, Dilshod Nematov, Aoqi Liu, Yanru Yin, Hailu Dai, Lei Bi

Monday 16 February

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

Cross-disciplinary integration towards sustainable construction

Dorian Hanaor

The built environment is the basis for human experience in the world, yet its current practices contribute significantly to global greenhouse gas emissions, resource depletion, and environmental degradation. This chapter explores the critical role of cross-disciplinary integration in achieving sustainable construction, emphasising the need to bridge the gaps between material science, architecture, engineering, environmental studies, and social sciences. By examining past and present examples and trends we explore how holistic, systems-oriented approaches can drive innovation and sustainability. We examine how the siloed nature of modern disciplines has hindered progress, leading to fragmented outcomes and missed opportunities for circularity and resource efficiency. We present the case for a paradigm shift towards cross-disciplinarity, where stakeholders across sectors and disciplines collaborate to create cohesive solutions that balance technical and economic performance, environmental stewardship, and social equity. This chapter addresses the economic and regulatory barriers that impede the adoption of sustainable materials and practices, advocating for structural changes in education, industry, and policy and highlighting the tools that are now enhancing this integration of knowledge. Ultimately, this work underscores the transformative potential of cross-disciplinary integration in redefining the built environment, offering a roadmap for achieving sustainability through collaboration, innovation, and a shared commitment to planetary well-being.
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Materials Science · Cross-listed from physics.chem-ph

High-throughput screening and mechanistic insights into solid acid proton conductors

Jonas Hänseroth, Max Großmann, Malte Grunert et al. (+2 more)

Proton-conducting solid acids could enable water-free operation of high-temperature fuel cells. However, systematic materials screening has, hitherto, been computationally prohibitive. Here, we introduce a two-stage high-throughput screening strategy that directly computes proton diffusion coefficients, enabled by machine-learned interatomic potentials fine-tuned to ab initio data. Starting from more than six million materials, our screening – based on structural motifs rather than empirical descriptors – identifies $27$ high-performing proton conductors, including over ten previously unexplored compounds. These include sustainable and commercially available materials, candidates that have not yet been synthesized, organic systems that fall outside conventional design rules, and known proton conductors that validate our approach. Importantly, our findings reveal a universal oxygen–oxygen distance of approximately $2.5$~Å at the moment of proton transfer across diverse chemistries, providing mechanistic insight and showing that macroscopic proton conductivity emerges from the interplay between anion rotational dynamics, hydrogen-bond network connectivity, and proton-transfer probability.
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All authors Jonas Hänseroth, Max Großmann, Malte Grunert, Erich Runge, Christian Dreßler

Materials Science

Eutectic and peritectic equilibria in coherent binary alloys

Samiah Hassan, Jiayang Wang, Teddy Meissner et al. (+2 more)

This work extends the Cahn–Larché thermodynamic framework to binary alloys in which two coherent solid phases coexist with an incoherent liquid and investigates how coherency strain energy modifies classical eutectic and peritectic equilibria. We derive equilibrium conditions for three-phase coexistence that include an elastic energy term dependent on the molar fractions of the solid phases and apply them to model binary eutectic and peritectic systems. We find that coherency stress transforms the eutectic point into a finite three-phase equilibrium field spanning a continuous range of compositions and temperatures. In systems whose equilibrium compositions are peritectically ordered, coherency stress progressively destabilizes the two-solid equilibrium without generating a stable three-phase field and can suppress the peritectic reaction entirely. This asymmetry is governed by the geometric relationship between the compositions of the phases: when the liquid composition lies between those of the two solids (eutectic configuration), the liquid serves as a thermodynamic buffer against the coherency penalty on the solid–solid pair; when it lies outside (peritectic configuration), no such mechanism is available. These results demonstrate that coherency stress can fundamentally alter three-phase equilibria involving a liquid and suggest that such effects may be significant in systems with large coherent misfits.
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All authors Samiah Hassan, Jiayang Wang, Teddy Meissner, Pierre A. Deymier, Marat I. Latypov

Materials Science

Complex Magnetic Behavior in RuO$_2$ Thin Films Driven by Strain and Substrate Effects

Mojtaba Alaei, Nafise Rezaei, Ilia Mikhailov et al. (+2 more)

Ruthenium dioxide (RuO$_2$) has been proposed as a prototypical metallic $d$-wave altermagnet, a Néel-ordered compensated antiferromagnetic state exhibiting nonrelativistic momentum-dependent spin splitting; yet, its magnetic ground state remains controversial both theoretically and experimentally. Using comprehensive first-principles calculations, we investigate RuO$_2$ thin films with (110), (100), and (001) orientations, both (un)strained freestanding and supported on a TiO$_2$ substrate. We show that emergent magnetic moments in RuO$_2$ thin films are highly fragile, strongly influenced by strain, surface orientation, and atomic relaxation, while also being highly sensitive to the choice of the Brillouin-zone integration scheme. We find that none of the thin film structures considered can stabilize a compensated antiferromagnetic order; therefore, an altermagnetic ground state cannot be realized. Instead, substrate-supported RuO$_2$ films on TiO$_2$ exhibit pronounced layer- and site-dependent magnetic moment variations and incomplete compensation between the two antiferromagnetically coupled Ru moments, yielding a ferrimagnetic-like behavior. On the other hand, freestanding RuO$_2$ films display complex magnetic structures depending on their orientation and applied strain, with distinct behavior at the surfaces and in the inner layers. Our results reconcile conflicting theoretical and experimental reports and underscore the sensitivity of RuO$_2$ magnetism to structural and methodological details.
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All authors Mojtaba Alaei, Nafise Rezaei, Ilia Mikhailov, Artem R. Oganov, Alireza Qaiumzadeh

Materials Science

Stacking-Engineered Thermal Transport and Phonon Filtering in Rhenium Disulfide

Yongjian Zhou, Haoran Cui, Zefang Ye et al. (+3 more)

Cross-plane heat transport is a critical bottleneck for van der Waals (vdW) electronics, yet its microscopic governing principles remain elusive. We demonstrate that stacking order is an effective control knob for cross-plane phonon transport in multilayer Rhenium Disulfide (ReS2). Thickness-dependent thermal conductivity measurements reveal remarkably long cross-plane phonon mean free paths (MFPs) (>= 200-300 nm) and provide a direct experimental observation of the transition from quasi-ballistic transport to a thickness-independent ballistic limit. AA stacking exhibits nearly double the cross-plane thermal conductivity of AB stacking, driven by longer acoustic phonon lifetimes from a more "coherent" interlayer registry. Integrated deep neural-network molecular dynamics reveals that phonon filtering in ReS2 is fundamentally frequency-selective: weak vdW coupling acts as a low-pass filter, whereas stronger coupling broadens the transmission passband. These results establish ReS2 as a model system where stacking order and interlayer coupling can be engineered to tune heat conduction across diffusive, quasi-ballistic, and ballistic regimes, offering a new framework for thermal management in 2D electronics.
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All authors Yongjian Zhou, Haoran Cui, Zefang Ye, Jung-Fu Lin, Yan Wang, Yaguo Wang

Materials Science

Practical and accurate density functionals for transition-metal heterogeneous catalysis

Benjamin X. Shi and Timothy C. Berkelbach

Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in rational catalyst design. These applications require reliable density functionals, however achieving transition-metal chemical accuracy (13 kJ/mol) on these properties remains challenging. We introduce a framework for designing new functionals tailored to catalytic processes on transition-metal surfaces, building on recent non-self-consistent approaches. Within this framework, we develop a hybrid and a double-hybrid functional that achieve unprecedented accuracy, with the latter reaching transition-metal chemical accuracy on average across 39 experimental adsorption reactions. In addition, both functionals demonstrate balanced performance for 17 barrier heights and correct qualitative failures of standard functionals, including CO adsorption on Pt(111) and graphene on Ni(111). They are computationally efficient, readily integrated into existing DFT codes, and supported by open-source workflows to facilitate adoption. More broadly, this framework provides a systematic route towards improved functionals for heterogeneous catalysis and complex materials.
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Materials Science

Large Transverse Thermoelectric Effect in Weyl Semimetal TaIrTe$_4$ Engineered for Photodetection

Morgan G. Blevins, Xianglin Ji, Vivian J. Santamaria-Garcia et al. (+4 more)

Anomalous local photocurrent generation via second-order nonlinear and thermoelectric responses is a signature of many topological semimetals. The emergence of these photocurrents is inherently linked to symmetry breaking and anisotropy of their crystal lattices. Studies of type-II Weyl semimetals of group C$_{2v}$ (WTe$_2$, MoTe$_2$, TaIrTe$_4$) have reported anomalous, nonlocal photocurrents localized to crystals edges or far from electrodes, which are highly dependent on the geometry of the material sample. While originally attributed to a nonlinear charge current response, it was recently shown that these currents could instead be attributed to the anisotropic Seebeck coefficients of the materials. Here, we confirm that anomalous photocurrents observed in TaIrTe$_4$ under either visible or far-infrared far-field illumination originate from the large transverse thermoelectric effect. We engineer the mutual orientation of crystal edges and electrodes as well as the thermal environment of TaIrTe$_4$ to control and amplify its spatial photocurrent response. We show that substrate engineering can locally enhance photocurrent. This framework of thermal device engineering can enable broadband photo detection schemes by leveraging spectral and spatial dependence of photocurrents for applications like wavefront sensing, beam positioning, and edge detection.
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All authors Morgan G. Blevins, Xianglin Ji, Vivian J. Santamaria-Garcia, Abhishek Mukherjee, Thanh Nguyen, Mingda Li, Svetlana V. Boriskina

Materials Science

Anisotropy-driven interfacial magnetism in Ru-deficient SrRuO$_3$ thin films

Vítor A. de Oliveira Lima, Michael I. Faley, Asmaa Qdemat et al. (+9 more)

While stoichiometric SrRuO$_3$ (SRO) is a metallic itinerant ferromagnet with relatively homogeneous magnetization, Ru deficiency provides a powerful route to alter its electronic transport and depth-dependent magnetic properties. Ru-deficient SRO thin films grown by radio-frequency high oxygen pressure sputtering were investigated using a combination of X-ray reflectivity, polarized neutron reflectometry, off-specular neutron scattering, scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy, electrical transport, and magnetometry. Structural and compositional analyses reveal that Ru deficiency is intrinsic to the films, with an enhanced deficiency at the interfaces. As a result, coherent electronic transport is suppressed and the saturation magnetization is reduced, while the Curie temperature remains largely unaffected, placing Ru-deficient SRO in a regime consistent with ferromagnetic insulator-like behavior. Depth- and lateral-resolved magnetic measurements further show that the interfacial regions remain ferromagnetic but exhibit enhanced perpendicular magnetic anisotropy, which constrains the local magnetization to remain predominantly out-of-plane and strongly reduces its in-plane projection. Our results establish Ru deficiency as a key control parameter governing transport, magnetization, and anisotropy in SRO thin films and highlight defect and interface engineering as powerful routes to tailor interfacial magnetism in correlated oxide heterostructures.
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All authors Vítor A. de Oliveira Lima, Michael I. Faley, Asmaa Qdemat, Valeria Lauter, Haile Ambaye, Omar Concepción, Ankita Singh, Emmanuel Kentzinger, Milan Radovic, Shibrabata Nandi, Thomas Brückel, Connie Bednarski-Meinke

Materials Science

Ferrocene-functionalized covalent organic framework exceeding the ultimate hydrogen storage targets: a first-principles multiscale computational study

Marcus Djokic and Jose L. Mendoza-Cortes

The development of efficient hydrogen storage materials is crucial for advancing the hydrogen economy and meeting the U.S. Department of Energy's targets of 6.5 wt% and 50 g H<sub>2</sub>/L for automotive applications. We present a computational study of ferrocene-functionalized covalent organic frameworks (COFs) for hydrogen storage. Following the <b>M</b>ulti-binding <b>S</b>ites <b>U</b>nited in <b>C</b>ovalent-<b>O</b>rganic <b>F</b>ramework (MSUCOF) approach, we introduce MSUCOF-4-FeCp, designed by incorporating ferrocene (FeCp<sub>2</sub>) moieties into IRCOF-102. Notably, it achieves exceptional performance with gravimetric and volumetric uptakes of 18.0 wt% and 72.6 g H<sub>2</sub>/L at 298 K and 700 bar. The material exhibits optimal binding energies (15-20 kJ/mol) ensuring both high storage capacity and deliverable hydrogen under practical conditions. This work establishes ferrocene functionalization as a cost-effective alternative to precious metal incorporation in COFs.
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Materials Science

Sub-1-Angstrom-Resolution Imaging Reveals Phase Contrast Transition in Ice Ih Caused by Basal Stacking Faults

Jingshan S. Du, Suvo Banik, Lehan Yao et al. (+3 more)

Phase-contrast transmission electron microscopy (TEM) of hexagonal ice (Ih) along [0001] sometimes shows a honeycomb-like pattern, often interpreted as individual oxygen columns in single crystals. Here, we show that this pattern commonly arises from intrinsic basal stacking faults instead. A translational boundary separating domains of comparable thickness, with an in-plane offset of $(\frac{2}{3} a_{1} + \frac{1}{3} a_{2})$, produces this honeycomb-like contrast. Stacking domains translated in nonequivalent directions yields patterns resembling cubic ice (Ic) along [111] but with a 3-fold symmetry. We imaged this structure at a record-breaking line resolution of 89 picometers, finer than the O-H covalent bond length. These findings highlight the defect tolerance of ice's molecular packing and clarify the structural relationships among hexagonal, stacking-disordered, and cubic ice phases. This resolution milestone opens new avenues for characterizing subtle structural perturbations of water in the solid state.
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All authors Jingshan S. Du, Suvo Banik, Lehan Yao, Shuai Zhang, Subramanian K. R. S. Sankaranarayanan, James J. De Yoreo