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Physics Condensed Matter Materials Science

cond-mat.mtrl-sci Watch Materials Science

Thursday 3 September

Materials Science · Cross-listed from cond-mat.mes-hall

Generalized s-d model for Wannier-Mott excitons in layered magnetic semiconductors

Sonu Verma, Bashab Dey and Akashdeep Kamra

The recent discovery of excitons coupled to the magnetic order, and the consequent strong magneto-optic responses, in some van der Waals magnetic semiconductors has triggered intense activity at the interface of magnetism and semiconductor optics. Here, we present an analytically tractable minimal model that describes magnetic order, electrons, holes, and excitons within a unified framework, thereby capturing a wide range of phenomena. It treats the magnetic order and itinerant carriers to be comprised by distinct electronic orbitals that are mutually coupled via orbital-dependent onsite exchange, similar to the treatment of metallic magnets using an s-d model. Investigating CrSBr bilayer as a case study, we benchmark our model and its predictions against recent experimental and ab-initio results finding good agreement as well as new insights enabled by the model's simplicity. Examining the optical selection rules, we find the conservation of a quantum number formed from a combination of spin and layer pseudospin to be a useful guiding principle, even in noncollinear magnetic configurations. Our analysis finds a series of bright and dark excitonic states in such layered A-type antiferromagnets. The presented framework should be valuable in achieving intuitive understanding of recently discovered excitonic phenomena and guiding the discovery of other excitonic states in layered magnetic semiconductors.
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Materials Science

Multimodal and Multiscale Interrogation of a Mechanically Tough Glass Forming Copper-Based Metal-Organic Framework

Mounir El Skafi, Guo-Qiang Li, Sophie R. Thomas et al. (+8 more)

A copper-based metal-organic framework, Cu(Im)2, was synthesized using a sol-gel process and subsequently melt-quenched into glass upon heating above 240 {\deg}C. In this paper, we present a multimodal, multiscale interrogation of the MOF nanocrystals and the resulting glasses. Structural characterization using X-ray diffraction, atomic force microscopy, and electron microscopy was performed to understand the morphology and size of the synthesized nanocrystals and glasses. Thermogravimetric analysis and differential scanning calorimetry were employed to understand the melting process of the crystals to form the glass. Synchrotron pair distribution function analysis was performed to verify that the framework structure is maintained upon melting, and nearfield infrared nanospectroscopy provided insight into the local chemical structure of the materials. The mechanical characterization via nanoindentation revealed that the resulting glasses exhibit an appreciably high elastic modulus (~10 GPa) and the highest fracture toughness (K_1c ~ 0.5 MPa m^1/2) yet reported for MOF glasses. This development is central to the emerging field of MOF-based materials processing and shaping, while upholding mechanical robustness and resistance to cracking.
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All authors Mounir El Skafi, Guo-Qiang Li, Sophie R. Thomas, James D. Taylor, Mark Frogley, Gianfelice Cinque, Marc Pignitter, Michael Reithofer, Jia-Min Chin, Sebastian Henke, Jin-Chong Tan

Materials Science

Gd-4f Exchange Splitting and Mo-4d Crystal-Field Redistribution in Gd/W Co-doped La2Mo2O9: A DFT+U Study

Amogh U. Lanjewar, Saurabh Shiwankar and Smita Acharya

La2Mo2O9 (LAMOX) is a promising oxide-ion conductor for intermediate-temperature solid oxide fuel cells, but its practical application is limited by a first-order monoclinic-to-cubic (alpha to beta) phase transition. Here, we investigate the electronic structure of pristine La2Mo2O9 and the Gd/W co-doped composition La1.6Gd0.4Mo1.7W0.3O9 using spin-polarized density functional theory with an on-site Hubbard correction for the localized Gd-4f states. The projected density of states reveals that pristine La2Mo2O9 is an O-2p/Mo-4d charge-transfer oxide in which La contributes negligibly near the band edges. Gd/W co-doping introduces a strongly exchange-split Gd-4f manifold with a majority-minority separation of approximately 1011 eV, substantially redistributes the Mo-4d electronic states through a threefold increase in crystal-field splitting, and reduces the O-2p contribution near the valence-band maximum from 78% to 66%. These electronic signatures are consistent with the experimentally observed lattice contraction, MoO Raman-mode softening, and the non-monotonic evolution of oxide-ion conductivity across the co-doped series. In particular, the pronounced crystal-field splitting and localized Gd magnetism at the highest doping level provide a microscopic electronic explanation for the observed suppression of ionic conductivity. The present results establish an atomistic electronic-structure framework for understanding dopant-induced phase stabilization and oxide- ion transport in Gd/W co-doped LAMOX electrolytes, providing design principles for improved solid oxide fuel cell materials.
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Materials Science · Cross-listed from cond-mat.stat-mech

Frenkel line of Yukawa fluids within the self-consistent relaxation theory

Ilnaz I. Fairushin and Anatolii V. Mokshin

For a simple model fluid, the Yukawa fluid, the condition for dynamic crossover, known as the Frenkel line, is defined. The condition is related to the fact that the roton minimum in the dispersion relation of longitudinal acoustic-like excitations exists only when the collective vibrational dynamics of particles dominates in the liquid. Based on the self-consistent relaxation theory for the Yukawa fluid, thermodynamic states are determined in which the roton minimum disappears. The obtained values of the state parameters for the Frenkel line are consistent with the results of studies in which the position of this line on the phase diagram of the Yukawa fluid was determined using molecular dynamics simulations. It is shown that the Frenkel line in this system can be determined directly from the structural characteristic – the static structure factor. A physical interpretation of the roton minimum frequency for the simple liquids near the Frenkel line is proposed.
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Materials Science

High-Throughput Computational Discovery of Inverted Resistive Switching in Two-Dimensional Materials

Sanchali Mitra, Arnab Kabiraj, Benjamin W. J. Chen et al. (+8 more)

Atomristors, non-volatile resistive switching devices based on two-dimensional (2D) monolayers, are promising building blocks for energy-efficient memory and neuromorphic computing. However, their design remains restricted to a few materials such as MoS2 and h-BN, limiting functional diversity and design flexibility. Here, a high-throughput computational framework combining density functional theory, machine-learning molecular dynamics, and quantum transport simulations screens about 2,900 exfoliable monolayers for vacancy-mediated resistive switching, identifying 17 thermally stable candidates in two mechanistically distinct classes. In Class 1 monolayers, such as GaS, Au adsorption at the native vacancy introduces conducting states, switching the insulating monolayer from a high- to a low-resistance state (HRS-to-LRS). Class 2 monolayers, comprising ionically bonded metal oxyhalides and nitrohalides such as BiOCl, exhibit previously unreported inverted switching. Vacancy-released electrons delocalize and push the Fermi level into the conduction band, placing the device natively in the LRS; Au adsorption re-localizes these carriers and returns the Fermi level to the gap, driving LRS-to-HRS switching. Quantum transport simulations confirm both mechanisms, while migration-barrier calculations identify the electrode-2D separation as a key parameter governing Au migration and the resistance window. These findings expand the atomristor landscape and establish complementary switching as a design paradigm for multifunctional memory and neuromorphic hardware.
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All authors Sanchali Mitra, Arnab Kabiraj, Benjamin W. J. Chen, Han Zhang, Haiyu Meng, Shi-Jun Liang, C. S. Lau, Lei Shen, Lain-Jong Li, Kah-Wee Ang, Yee Sin Ang

Materials Science

SALTED: a symmetry-adapted machine-learning program for predicting electron-densities in molecules and materials

Zekun Lou, Alan M. Lewis, Théophane Bernhard et al. (+5 more)

SALTED provides an open-source Python package for machine learning the quantum-mechanical electron density, $n(\mathbf{r})$, in molecular and condensed-phase systems based on input atomic coordinates and species. The program adopts a linear atom-centered decomposition of the electron density, which makes it highly transferable across diverse atomistic configurations sharing similar chemical environments. Because of this representation choice, SALTED is naturally interfaced with state-of-the-art electronic-structure programs based on atomic orbitals, namely CP2K, FHI-aims, and PySCF, from which reference electron-density data can be generated and used to train a model. The learning algorithm is based on a symmetry-adapted extension of Gaussian process regression, making SALTED especially efficient in small-data regimes. Thanks to the implementation of vector-field kernel functions, SALTED can also learn the first-order response of the electron density to applied electric fields, $\partial n(\mathbf{r})/\partial \mathbf{E}$. The application of SALTED within computational workflows has already shown its utility in a wide variety of contexts, including the calculation of polarization vectors and polarizability tensors, the accurate evaluation of Coulomb forces in QM/MM molecular-dynamics simulations, and electronic-structure studies of large-scale 2D materials.
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All authors Zekun Lou, Alan M. Lewis, Théophane Bernhard, Lukas Seifert, Agustin Salcedo, Florian Kleemiss, Mariana Rossi, Andrea Grisafi

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

Non-Resonant Impulsively Stimulated Raman Scattering by a Terahertz Field: a Case Study of 1T-TaS2

Haotian Zhang, Yuheng Guo, Zidu Yu et al. (+7 more)

Time-domain ultrafast and nonlinear terahertz spectroscopy techniques are recently applied to many condensed matter systems for investigating their collective excitations. In centrosymmetric systems, these collective modes are typically Raman-active and therefore do not couple directly to the terahertz electric field. The mechanism by which light-matter interaction realizes in these studies has not been explicitly discussed in detail. In this work, we perform terahertz pump - optical probe and terahertz third harmonic generation investigations on 1T-TaS2, a material exhibiting a rich charge-density-wave (CDW) phase diagram including the commensurate, nearly-commensurate and incommensurate CDW phases. The transition between these distinct states leaves a clear signature on the dynamical Raman response. We investigate how the Raman-active phonons couple to a broadband monocycle terahertz field as well as a narrowband multicycle terahertz field. Our results indicate that a modified impulsively stimulated Raman scattering mechanism involving two-photon absorption, also known as non-resonant Raman scattering, underlies the coherent excitation and observation of the lattice modes. These results are relevant for future spectroscopy investigation and coherent control of collective modes using low-energy terahertz field as well as cavity electrodynamical dressing of solids.
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All authors Haotian Zhang, Yuheng Guo, Zidu Yu, Yongbo Lv, Yiting Wang, Liwen Feng, Jiaying Xu, Tianlong Xia, Xinbo Wang, Hao Chu

Materials Science

Orbital-Free DFT-Assisted Machine-Learned Molecular Dynamics for Electric-Field-Driven Ionic Transport

Yusuke Nishiya, Hiroya Nakata, Yosuke Harada et al. (+1 more)

We propose an orbital-free density functional theory (OFDFT)-assisted machine-learned molecular dynamics method in which field-independent interatomic forces are evaluated using a machine-learned potential and atomic charges that depend on the local environment are obtained from OFDFT calculations. The atomic charges obtained by Bader partitioning of the OFDFT electron density are multiplied by the electric-field vector and added to the forces from the machine-learned potential. This approach enables molecular dynamics simulations under an electric field at a lower computational cost than Kohn-Sham DFT (KSDFT)-based molecular dynamics. As a proof of concept, the method was applied to beta-Li3PS4 bulk and an S8/Li3PS4 heterostructure under periodic boundary conditions. For Li3PS4 bulk, OFDFT yielded Li charges and a total charge of the PS4 unit consistent with those obtained using KSDFT. In the heterostructure, Li ions migrated from the Li3PS4 region into the S-rich region within a simulation time of approximately 170 ps. Accompanying this migration, the mean Bader charge of the S atoms that initially formed S8 rings changed from nearly neutral to negative. A comparison with KSDFT for a representative interfacial structure also confirmed that the negative charging of the S atoms upon the arrival of Li and the magnitude of the Li charges were qualitatively reproduced. These results demonstrate the possibility of treating field-driven ionic transport and changes in interfacial charge states using a universal machine-learned potential without training an additional material-specific charge-prediction model.
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All authors Yusuke Nishiya, Hiroya Nakata, Yosuke Harada, Yu-ichiro Matsushita

Materials Science

Electron-phonon coupled hydrodynamics in semimetal TaAs_2

Shan Jiang, Wei Xie, Xiaokang Li et al. (+2 more)

Hydrodynamic corrections to diffusive transport can arise when momentum-conserving collisions between quasiparticles become prominent, and they have been documented for both electrons and phonons. An emerging frontier topic is coupled electron-phonon (e-ph) hydrodynamics. Here, through electrical and thermal transport measurements on TaAs2 crystals with different impurity levels, we document the emergence of an e-ph bifluid in the temperature window of 5 to 15 K. Within this range, the lattice thermal conductivity exhibits a faster-than-T^3 temperature dependence, as a consequence of non-monotonic and purity-dependent phonon mean free paths, a signature of phonon Poiseuille flow. However, strong e-ph coupling impedes the emergence of a ballistic regime. This is corroborated by the observation of quantum oscillations in the lattice thermal conductivity. Prominent phonon-mediated momentum exchange between electrons amplifies the violation of the Wiedemann-Franz law and yields a two-order-of-magnitude discrepancy between quantum and transport lifetimes, a signature of electron hydrodynamics in semimetals. Our results imply that in semimetals with optimized e-ph coupling, thanks to matching between the cryogenic phonon wave?length and the Fermi wavelength, momentum and energy flow between the electron and phonon reservoirs as frequently as within each reservoir.
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All authors Shan Jiang, Wei Xie, Xiaokang Li, Kamran Behnia, Zengwei Zhu

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

Competing lattice structures induced by Sn substitution in CsV$_3$Sb$_5$

Anshu Kataria, Ilija K. Nikolov, Armando Consiglio et al. (+8 more)

Understanding the effect of chemical substitution on competing phases of kagome metals is crucial for disentangling the interplay between local structural distortions and electronic instabilities. In \cvs, Sn substitution strongly modifies the electronic phase diagram, yet the microscopic mechanism driving this remains unclear. Here, we combine $^{121}$Sb nuclear quadrupole resonance (NQR) measurements and density functional theory calculations to investigate the atomic-scale effects of Sn substitution in CsV$_3$Sb$_{5-x}$Sn$_x$. At low Sn concentrations, the observed satellite NQR peaks exhibit signatures of local structural distortion induced by Sn substitution, qualitatively consistent with our computational analysis. These impurity-induced features persist across the entire experimentally investigated doping range, up to $x$ = 0.65, and remain observable up to room temperature. For $x=1$, the fully doped idealized case, the estimated dynamical instabilities of the kagome lattice suggest the stabilization of two nearly energy-degenerate equilibrium structures characterized by V-trimers, distinguished by a zero- or $\pi$-phase shift between adjacent layers along the $c$-axis. Together, these results show that Sn substitution drives a complex interplay between local impurity-induced distortions and competing structural instabilities in vanadium-based kagome compounds.
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All authors Anshu Kataria, Ilija K. Nikolov, Armando Consiglio, Giuseppe Allodi, Ginevra Corsale, Andrea Capa Salinas, Stephen D. Wilson, Domenico Di Sante, Vesna F. Mitrović, Samuele Sanna, Pietro Bonfà

Materials Science

Interplay of B-Site Off-Centering and Molecular Orientations in the Mixed Hybrid Perovskite MAGe1xSnxI3

Erik Fransson, Apinya Ngoipala, Oskar Öjstedt et al. (+3 more)

B-site mixing is a common strategy for tuning properties of halide perovskites. In the lead-free system MAGe1-xSn_xI3, it brings tilting and off-centering into competition. Using large-scale molecular dynamics driven by a machine-learned interatomic potential, we map the structural behavior across the full composition range. MAGeI3 exhibits strong polar B-site off-centering that remains nearly constant up to the cubic transition, together with methylammonium (MA) orientational order that weakens progressively on heating. By contrast, MASnI3 combines octahedral tilting with weaker, predominantly antipolar off-centering. Ge-like behavior persists upon alloying and gives way to Sn-like behavior only beyond roughly 65 % Sn. In the high-temperature phases, the B-site cations remain locally off-centered but directionally disordered. On the Ge-rich side, the distorted inorganic framework biases the soft MA orientational landscape toward a restricted set of preferred directions. This coupling shows how the composition of the inorganic sublattice can tune molecular ordering in lead-free hybrid perovskites.
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All authors Erik Fransson, Apinya Ngoipala, Oskar Öjstedt, Maths Karlsson, Paul Erhart, Julia Wiktor

Materials Science

Polaron Self-Trapping Rates from First Principles

Mark E. Turiansky, Joel B. Varley, Audrius Alkauskas et al. (+1 more)

Polaron formation, also known as self-trapping, is a process akin to nonradiative carrier capture at point defects or impurities. In this work, we develop the formalism to determine how long it takes to form a small hole or electron polaron from first principles. We employ an accurate, fully first-principles approach based on a Koopmans compliant hybrid functional. The self-trapping rate is the product of two components: the nonradiative capture coefficient, which we evaluate using a one-dimensional approximation, and the maximum density of polaron sites, whose physics we elucidate based on finite-size interactions present in supercells. We apply our methodology to several technologically relevant materials known to host hole polarons, Ga$_2$O$_3$, Al$_2$O$_3$, BeO, KBr, MgO, NaCl, SiO$_2$, SnO$_2$, TiO$_2$, and ZnO, and to an electron polaron in rutile TiO$_2$. We also study an emerging semiconductor, rutile GeO$_2$, where we find that polaron formation could hamper $p$-type conductivity. The calculated self-trapping lifetimes span 7 orders of magnitude, from $10^{-1}$ to $10^6$~ps, in agreement with experiments where available, and providing detailed insight into the dynamics of carrier localization and relaxation in solids.
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All authors Mark E. Turiansky, Joel B. Varley, Audrius Alkauskas, Chris G. Van de Walle

Materials Science

Grain boundary evolution in nanoparticles

Manoj Settem, Pranav Kumar and Ajeet K. Srivastav

Grain boundary evolution is a key dynamical process that enables structural rearrangements in nanoparticles and drives them towards low energy configurations. Grain boundaries can also enhance catalytic properties, making it important to understand the elementary processes underlying their evolution for grain boundary engineering in nanoparticles. Compared with bulk materials, nanoparticles have additional rotational and translational degrees of freedom, can accommodate structural changes through shape relaxation, and grain boundaries terminate at free surfaces. However, the atomic-scale mechanisms of GB evolution under these less constrained conditions remain comparatively less understood than in bulk materials. Here, using atomistic simulations, we focus on low energy $\Sigma3$ (coherent twin boundary) and $\Sigma11$ grain boundaries, which are among the persistent compact GB structures that emerge during nanoparticle structural evolution. We identify two fundamental atomic displacements, column shift (C) and screw shift (S), that recur during the evolution of these grain boundaries and their junctions. These displacements occur through different atomic pathways and combine in different ways to generate grain boundary migration, structural transformations, and junction evolution. In particular, the same initial and final grain boundary configurations can be connected through different atomic pathways, and a column shift can occur either as a full shift or through disconnection kinks. C and S remain identifiable even when the grain boundary character changes, for example during a $\Sigma11$ to $\Sigma3$ transformation. An understanding of these elementary GB processes can help identify strategies to control grain boundary evolution and thereby engineer GB structures in nanoparticles.
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Wednesday 2 September

Materials Science · Cross-listed from quant-ph

Quantization and Mirror Reduction Do Not Commute in Hamiltonian Embeddings of Nonreciprocal Dynamics

Gaurav Sarmah and Ramakrishna Podila

Hamiltonian embeddings can represent dissipative nonreciprocal classical dynamics exactly on invariant manifolds of enlarged reciprocal systems. We show that canonical quantization of such an embedding need not commute with reduction to the target dynamics. For the mirror construction recently introduced for pairwise nonreciprocal interactions, the invariant manifold is Lagrangian. Exact quantum enforcement of the mirror condition therefore removes the dynamical sector rather than producing a quantum analogue of the reduced flow. If the constraint is imposed only semiclassically, contraction of the target dynamics generates inverse-transpose expansion in the conjugate mirror directions. Quantum uncertainty then gives $\ln D\ge\Xi(t)+n\ln[\pi/(\sigma\epsilon)]$, where $\Xi=-\ln|\det M|$ is the accumulated contraction and $D$ the torus Hilbert-space dimension. Exact finite-dimensional Weyl evolution of one- and two-degree-of-freedom nonreciprocal models confirms the resulting logarithmic correspondence time, including its predicted change when the initial localization scales with $\hbar$. Thus the classical embedding is exact, but its direct canonical quantization is a singular semiclassical construction.
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Materials Science

A Strategy Toward Room Temperature Topological Hall Effect via Local Moment Magnetism

Karthik Rao, Kevin Allen, Yuxiang Gao et al. (+10 more)

Topological spin textures in local moment systems hold great promise for technological applications due to their large magnetic moments, strong spin-orbit coupling (SOC), and high tunability. Finding new spin textures that are stable near room temperature is paramount to maximizing their potential for applications. Here, we provide a strategy for realizing topological spin textures at high temperatures by identifying rare earth ($R$) magnets ordering at or near room temperature. We demonstrate the feasibility of this strategy in one of these magnets, hexagonal Gd$_5$Pb$_3$, which orders at $T_C$ = 285 K. The indication for topological spin textures comes from topological Hall effect (THE), which, in Gd$_5$Pb$_3$, occurs between $T$ = 100 - 200 K, an order of magnitude higher temperature than in other reported $R$-based systems. Our results present an opportunity to explore the role of SOC, anisotropic exchange, geometric frustration, and magnetic interactions in stabilizing topological spin textures, and provide a pathway toward realizing them near room temperature in $R$-based magnets.
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All authors Karthik Rao, Kevin Allen, Yuxiang Gao, Arushi, Sanu Mishra, Birender Singh, Kenneth S. Burch, Liangzi Deng, Shanta R. Saha, Johnpierre Paglione, Minseong Lee, Vivien Zapf, Emilia Morosan

Materials Science

Thermal history controls the optoelectronic response of lead halide perovskites through structure and dynamics

Milos Dubajic, Xia Liang, Johan Klarbring et al. (+26 more)

Lead halide perovskites are promising optoelectronic materials for photovoltaics, light emission and detection. Their efficiencies in PV now approach the detailed-balance limit, leaving stability as the principal barrier. The intrinsic instabilities studied to date centre on ionic motion within a fixed, homogeneous lattice. Here we identify a further source of intrinsic structural instability, hidden in the lattice dynamics. Mapping caesium, methylammonium and formamidinium-based compositions with Cl, Br, I and mixed X-sites through all accessible phases, using single crystal X-ray and neutron diffuse scattering, machine-learning-assisted molecular dynamics, a phenomenological octahedral tilt model and hyperspectral photoluminescence, we find that nearly every composition hosts equilibrium local structural fluctuations: dynamic nanodomains of correlated octahedral tilts, a few nanometres in size, that locally break the crystallographic symmetry. Three complementary levers control them. The A-site cation sets their symmetry, shape and anisotropy, from sparse, isotropic and tetragonal in formamidinium-based compositions to dense, anisotropic and orthorhombic in nominally cubic caesium-based ones, the most locally disordered we studied. The halide controls the dynamic disorder and the phase-transition sequence. Thermal history is the third: different ramp rates drive nominally identical compositions into distinct crystallographic phases, each with its own hidden local order. In MAPbI3, the heating rate alone changes the photoluminescence quantum efficiency across the phase transition. Because these transitions lie within device operating ranges, from terrestrial thermal cycling to the extremes of space, thermal history may shape the local structure, and hence the optoelectronic response, throughout fabrication and operation, establishing it as a design variable alongside composition.
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All authors Milos Dubajic, Xia Liang, Johan Klarbring, Yang Lu, Thomas A. Selby, Erik Fransson, Philippe Holzhey, Benjamin M Gallant, Qichun Gu, Ganbaatar Tumen-Ulzii, Khasim Saheb Bayikadi, Isaiah Gilley, Martin v. Zimmermann, Christian Orr, Chwenhaw Liao, Josh S. Moon, Jacek Jasieniak, Makhsud Saidaminov, Michael P. Nielsen, Tom Wu, Stephen P. Bremner, Anita Ho-Baillie, Julia Wiktor, Paul Erhart, Steve Albrecht, Mercouri Kanatzidis, Henry J Snaith, Aron Walsh, Samuel D. Stranks

Materials Science

An Ultrathin Laterally Conductive Mesh Interphase Enables Spatially Extended Zinc Deposition for Aqueous Zinc Batteries

Yirong Zhao, Xingyuan Chu, Bing Wu et al. (+15 more)

Zn metal anodes often suffer from nonuniform interfacial reactions during cycling, resulting in uneven deposition and dendrite growth. Existing artificial interphases can mitigate side reactions or regulate nucleation, but rarely achieve regulation of the interfacial electron/field distribution to sustain uniform deposition at the evolving Zn/electrolyte interface. Here, we develop an Au mesh interphase (AuMI), an ultrathin two-dimensional Au aerogel network that couples lateral electron redistribution with open pathways for ions. During Zn plating/stripping, the conductive AuMI distributes electron transport across the Zn surface, while its porous mesh preserves Zn$^{2+}$ access, enabling more uniform interfacial reactions. Experiments and simulations show that AuMI homogenizes the interfacial electric field and current distribution, promotes more uniform Zn plating/stripping, and limits dendrite growth. As a result, this regulated interfacial reaction mode enables AuMI Zn symmetric cells to operate stably for 3000 h at 1 mA cm$^{-2}$/1 mAh cm$^{-2}$ and for 1100 h at 10 mA cm$^{-2}$/10 mAh cm$^{-2}$, while AuMI Zn||NVO (NaV$_3$O$_8$\cdot$1.5H$_2$O) full cells retain 80.8 % capacity after over 5000 cycles at 1 A g$^{-1}$. These findings highlight the importance of combining ultrathin architecture, lateral electron transport, and open Zn2+ access in artificial interphases for stable aqueous Zn metal anodes.
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All authors Yirong Zhao, Xingyuan Chu, Bing Wu, Pavel Khavlyuk, Johannes Kresse, Yue Dong, Jingwei Du, Xinmei Song, Songshan Bi, Vlastimil Mazanek, Xia Wang, Xiaodong Li, Shilei Liu, Shuangying Wei, Jan Luxa, Junming Zhang, Zdenek Sofer, Alexander Eychmuller

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

Antiferromagnetism-altered plasmon dynamics

Yifan Su, Suheng Xu, Rocco A. Vitalone et al. (+17 more)

The interaction between plasmons and magnons is a long-sought phenomenon with implications for fundamental physics and spintronics applications. In three-dimensional systems, this coupling is suppressed by the large mismatch in energy scales, but two-dimensional (2D) plasmons with gapless dispersion can overlap with magnons over a broad spectral range. Despite numerous theoretical predictions, experimental observation of magnon-plasmon interaction has remained elusive. In this work, we study a first-of-its-kind hybrid plasmon-magnon platform based on 2D materials. By deploying scattering-type scanning near-field optical microscopy (s-SNOM) with terahertz radiation, we image propagating plasmon wavepackets at a graphene/NiPS$_3$ interface and track their dynamics across the antiferromagnetic transition of NiPS$_3$. We observe a clear renormalization of the plasmon-polariton dispersion concurrent with the onset of antiferromagnetic order. With complementary Raman scattering and nano-terahertz spectroscopy, we unveil spectral weight redistribution and dielectric screening changes, potentially associated with the multi-magnon continuum, as the underlying mechanism. These results provide solid evidence of coupling between plasmon and antiferromagnetic order, marking a cornerstone for a potential platform for hybrid magnon-plasmon interactions in 2D materials, opening avenues for coherent spin-plasmon devices and tunable terahertz spintronic components.
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All authors Yifan Su, Suheng Xu, Rocco A. Vitalone, Ziyu Liu, Emil Viñas Boström, Na Wu, Chun-Ying Huang, Zhuquan Zhang, Jaehoon Jung, Daniel G. Chica, Vinícius da Silveira Lan Avelar, Yiping Wang, Takashi Taniguchi, Kenji Watanabe, James C. Hone, Xiaoyang Zhu, Cory R. Dean, Xavier Roy, Angel Rubio, D. N. Basov

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

Reactive calcium carbonate precipitation from an atomic cluster expansion potential and enhanced sampling

Eslam Ibrahim, Yury Lysogorskiy, Ralf Drautz et al. (+1 more)

Calcium carbonate formation from aqueous solution is central to biomineralization and to carbon sequestration through mineral carbonation. At near-neutral pH, the process is highly reactive, with proton transfer mediating the interconversion between carbonate species. Most atomistic simulations to date either treat carbonate speciation as fixed or consider proton transfer only in small clusters. Here, we combine an ab initio trained atomic cluster expansion (ACE) machine-learning potential for molecular dynamics with enhanced sampling to enable reactive simulations of the early stages of calcium carbonate precipitation at previously inaccessible length and time scales. We study proton transfer and carbonate speciation in ion pairs and triplets, as well as in the collective aggregation of many ions. Our simulations with few ions show that ion association provides a favorable pathway for proton transfer, facilitating interconversion between carbonate, bicarbonate, and carbonic acid. In many-ion systems, proton transfer occurs spontaneously alongside aggregation, and we observe significant changes in the coordination environments as species evolve during the simulations. These results show that ion aggregation and chemical reactivity can be strongly coupled during the early stages of nucleation from solution.
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All authors Eslam Ibrahim, Yury Lysogorskiy, Ralf Drautz, Pablo M. Piaggi

Materials Science

Interplay between Isomerization and Spin Crossover in 1D Fe-Indigo Coordination Polymers on Ag substrates

Ritam Chakraborty, Hongxiang Xu, Biao Yang et al. (+5 more)

Spin-crossover (SCO) compounds offer a route to switchable molecular functionality in reduced dimensions. However, one-dimensional (1D) SCO chains, which offer the possibility to study ligand fields other than the paradigmatic octahedral field, remain comparatively little studied. Here, we use first-principles density functional theory (DFT+$U$) to investigate Fe-indigo coordination-polymer chains synthesized experimentally on Ag(111) and Ag(100) substrates. These display a rich interplay between changes in ligand field (isomerization) and spin crossover. On-surface isomerization on Ag(111) interconverts (N,O)-chelated trans configuration and (N,N)-/(O,O)-chelated cis configurations at the Fe centers. The lowest-energy trans and cis solutions on Ag(111) have different spin configurations over the interval $0.66<U<3.00$~eV. At the reference value $U=1$~eV, the preferred trans solution is the mixed LS–LS–HS configuration, whereas the preferred cis solution is LS–LS–LS. The experimentally observed preference for cis chains on Ag(111) and trans chains on Ag(100) is reproduced for the range $0.88<U<3.75$~eV. To interpret these results, toy models and spin-resolved Fe $3d$ projected densities of states are used, while freestanding-chain calculations reveal a strain-sensitive LS–HS competition. These results provide a microscopic explanation for isomerization-controlled spin-state switching in a 1D coordination polymer.
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All authors Ritam Chakraborty, Hongxiang Xu, Biao Yang, Harshdeep Singh Chhabra, Joachim Reichert, Johannes V. Barth, Anthoula C. Papageorgiou, Shobhana Narasimhan

Materials Science

IDMate: Finite-temperature error bounds for window-resolved self-consistent-field screening

Peng Kang, Da Wan, Shulin Bai et al. (+5 more)

We formulate a finite-temperature residual test in IDMate that bounds window-resolved electronic errors without a spectral-gap assumption. For a fixed Hamiltonian and exact electron number, strong convexity of the matrix Fermi entropy bounds the density-matrix distance and free-energy error within a selected window. The bound remains finite at spectral crossings and extends to weighted k points with a shared chemical potential. We also derive a distance correction for particle-number mismatch. Across $3{,}586$ stress trials in $70$ seeded perturbation ladders, $1{,}942$ proposals satisfy the screen with no observed violation of the $0.05$ window-distance criterion plus its numerical allowance. This criterion differs from the uncorrected exact-trace bound, which six of ten historical in-loop candidates exceed at the numerical-error scale. An accept-or-recover loop replaces ten reference-map evaluations while meeting terminal comparison criteria in three configurations that include oracle-subspace controls. Additional candidates built only from preceding-iteration orbitals yield two acceptances and one abstention. The silicon candidate has a window distance of $1.891\times10^{-13}$ but a normalized real-space density error of $3.754\%$. Analytic examples separate errors from complement occupations and interblock coupling. Window-level accuracy therefore does not imply full-state accuracy; the screen tests compressed proposal quality, independently of nonlinear SCF convergence or net acceleration.
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All authors Peng Kang, Da Wan, Shulin Bai, Zhen Li, Yu Liu, Lei Zheng, Li-Dong Zhao, Huibin Xu

Materials Science

Battery open-circuit voltage is not purely chemical

Andrea Giudici, Christoph Pohl, Alberto Salvadori et al. (+3 more)

Open-circuit-voltage (OCV) curves are commonly treated as intrinsic chemical properties of electrode materials. However, this view is incomplete. In ion-insertion batteries, OCV also depends on mechanical state and microstructure. Using finite-element simulations and asymptotic analysis, we show that particle swelling and external loads promote particle–particle contact that generates compressive stresses, shifting the inserted-ion chemical potential. The OCV correction is nonlinear, follows Hertzian contact scaling, and depends on particle arrangement. Identical materials can therefore exhibit different OCV curves in different electrode microstructures. Furthermore, in full cells, electrodes are mechanically coupled through the common stack stress. Thus, cell OCV is a chemo-mechanical property of the entire battery architecture, not chemistry alone.
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All authors Andrea Giudici, Christoph Pohl, Alberto Salvadori, Colin Please, Manuel Landstorfer, Jon Chapman

Materials Science

Physics-Informed Neural Network Surrogate for Oxygen Vacancy Dynamics in epitaxial $\mathrm{SrTiO_3}$ on Si memristors via Dynamic Spectral Optimization

Rodion Podorozhny, Nikoleta Theodoropoulou and Jelena Tešić

Physics-informed neural networks (PINNs) offer a promising framework for modeling semiconductor devices, yet standard architectures struggle with severe numerical stiffness and multiscale spatial discrepancies inherent to oxide heterostructures. Here, we demonstrate a cascaded PINN architecture coupled with a custom second-order Chebyshev second kind polynomial spectral optimizer (DSO V2 Hybrid) to model ion-electronic drift-diffusion transport in Pt/SrTiO$_3$/Si memristive heterostructures across a 20 nm STO film on a 380 $\mu$m Si substrate. By isolating potential, carrier density, and vacancy transport into four sequentially trained sub-neural-networks, our model circumvents condition numbers exceeding $10^{16}$ without operator splitting. The trained surrogate reproduces experimental conductive-AFM current-voltage hysteresis ($R^2 > 0.96$) while ensuring strict Poisson consistency across continuous space. Compared to conventional finite-element solvers (e.g., COMSOL), the PINN surrogate enables differentiable inverse parameter estimation and linear time inference.
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Materials Science · Cross-listed from math.NA

Buckling Prediction for Nonlinear Elastic Beams with Soft Inclusions

Thien Tran-Duc, J.E. Bunder and A.J. Roberts

We develop an efficient and accurate multiscale computational framework for predicting the buckling and post-buckling behaviour of elastic beams containing periodically distributed soft inclusions. The framework extends our previous multiscale, patch, computational homogenisation for linear elasticity by incorporating nonlinearity, and thus enables accurate prediction of both the buckling onset and the subsequent post-buckling response. Microscale computations are performed only within a sparse set of small subdomains (patches), while the macroscale behaviour is recovered through a proven patch-coupling algorithm. The scheme is assessed through quarter- and half-domain patch computations for beams with inclusion-to-matrix Young's modulus ratios ranging from 0.001 to 1. The results show that reducing the inclusion stiffness lowers both the critical buckling strain and the critical buckling stress, indicating an increased susceptibility to instability, while producing a milder post-buckling response with smaller transverse deflections and stress drops. Eigenvalue analysis of the Jacobian matrix accurately predicts the onset of instability and the corresponding critical strain and stress. Bifurcation diagrams of the nonlinear buckled configurations under compressive loading, and a quantitative analysis of the effect of the interpolation order on the predicted buckling and post-buckling responses, are also presented. Comparisons with full-domain simulations demonstrate that the proposed framework accurately predicts both the buckling threshold and the post-buckling behaviour while substantially reducing the computational cost. The methodology is readily extendable to heterogeneous beams, plates, shells, and other engineering structures.
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Materials Science

Repairing PBE-Spurious Metallicity for HSE06-Level Screening of 2D Photocatalysts for Green Hydrogen Production

Ritam Chakraborty and Arpan Das

Semilocal PBE calculations can remove viable photocatalysts before screening by labeling narrow-gap semiconductors as metals. We address this failure mode in the Computational 2D Materials Database (C2DB) by combining leakage-aware repair of PBE-spurious metallicity with HSE06–PBE $\Delta$-learning. Stage~I classifies HSE06-unknown PBE metals using structural, chemical, magnetic, and stability descriptors, while excluding HSE06/GW quantities and PBE electronic shortcuts. Stage~II learns $E_g^{HSE} - E_g^{PBE}$ for the corrected insulating population. The curated XGBoost regressor reconstructs HSE06 gaps with a mean absolute error of 0.108~eV ($R^2=0.989$), compared with 1.036~eV for raw PBE. The Stage~I classifier is used only for triage because the labeled true-metal class contains 29 materials; its best holdout performance gives 87.5% accuracy, 0.286 true-metal recall, and 0.643 balanced accuracy. The corrected pH~0 electronic screen yields 10 strict and 29 initial relaxed green-hydrogen photocatalyst candidates. Four strict and 18 relaxed candidates would fail the same 1.6–2.8~eV gap window at the PBE level. Targeted VASP HSE06 calculations for six ML-predicted compounds give material-level MAEs of 0.417, 0.182, and 0.110~eV for the C2DB-native, Magpie+structural, and curated models, respectively; \feat{1AgBr-1} shifts above the upper gap cutoff, leaving 28 retained relaxed candidates. The workflow shows that high-fidelity correction must be evaluated by candidate membership, not only by global regression error.
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Materials Science · Cross-listed from physics.chem-ph

Low-Temperature Transport in Li-Ion Battery EC/EMC/FEC Electrolytes: Molecular Dynamics and Machine-Learning Modeling

İpek Yenda Ç{\i}nar, Oguzhan Orhan, M. Oluş Özbek et al. (+1 more)

Low-temperature operation imposes severe limitations on lithium-ion transport in battery electrolytes, yet the coupled effects of solvent composition and fluorinated additives in the cold-temperature regime remain insufficiently resolved. Here, we combine classical molecular dynamics (MD) and machine learning (ML) to investigate 1 M LiPF$_6$ electrolytes containing ethylene carbonate (EC), ethyl methyl carbonate (EMC), and EC/EMC (3:7), with 0-10 mol% fluoroethylene carbonate (FEC), from 298 to 233 K. MD simulations quantify Li$^+$ self-diffusion, Nernst-Einstein (NE) and Green-Kubo (GK) conductivities and local coordination, while Gaussian-process surrogates model conductivity across composition and temperature. Cooling produces a pronounced transport penalty, particularly in EMC-containing electrolytes, whose GK conductivity decreases by more than 98% at 233 K, compared with approximately 90% in EC-rich systems. Li$^+$ self-diffusion activation energies are 0.49-0.54 eV for EMC-containing systems and 0.27-0.29 eV for EC-based systems. Within the EC family, 0-2 mol% FEC gives comparable cold-temperature transport, whereas 5-10 mol% FEC shows lower conductivity retention at the coldest simulated temperature. The analyzed coordination channels remain solvent dominated, while direct Li$^+$-FEC coordination is not quantified in the present RDF set.The Gaussian-process surrogates achieve composition-disjoint cross-validated RMSE values of 0.56 and 0.57 mS cm$^{-1}$ for NE and GK conductivity. Within the simulated liquid-state trajectories, temperature and host-solvent composition dominate the bulk-transport response, with FEC acting as a secondary modifier.
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All authors İpek Yenda Ç{\i}nar, Oguzhan Orhan, M. Oluş Özbek, Şener Özönder

Materials Science

First Principle Analysis of the Magnetism and Electronic Structure of Fe2XSi (X=Ti, V)

Hanieh Kachooee, Cindy Kim, Jason Carbajal et al. (+2 more)

The electronic, magnetic, and mechanical properties of Fe2XSi, where X is titanium (Ti) and vanadium (V), are investigated using computational methods. Volume optimization reveals that the ground state of Fe2TiSi is a nonmagnetic narrow-band gap semiconductor, and that of Fe2VSi is a ferrimagnetic metal. The negative formation energies of both materials confirm the stability of their crystal structures. Mechanical properties confirm the static stability of the crystal structure and suggest that the titanium compound is ductile; however, the vanadium material is brittle. Density of states and band structure studies confirm the nonmagnetic semiconducting nature with an indirect band gap at {\Gamma} and X for the titanium material and the ferrimagnetic-metallic nature of the vanadium material. Electronic and magnetic properties of the materials were investigated with applied tension (negative pressure) and compression (positive pressure) to the crystal structure. The pressure study on Fe2TiSi shows a tunable band gap and a possible semiconductor-metal transition, and Fe2VSi shows a tunable magnetic moment and a possible low-spin/high-spin magnetic transition.
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All authors Hanieh Kachooee, Cindy Kim, Jason Carbajal, K. Hettiarachchilage, N. Haldolaarachchige

Materials Science

AlterSeeK-Path: Systematic construction of generalized band-structure paths for displaying altermagnetic spin splitting

Yujia Teng, Mesfin Eshete, Andrea Urru et al. (+4 more)

Altermagnetic materials exhibit spin splitting in their electronic band structures while maintaining zero net magnetization. However, conventional high-symmetry k-paths generally hide this splitting because they follow symmetry lines that in most cases enforce spin degeneracy. We present AlterSeeK-Path, an open-source Python tool that systematically constructs generalized band-structure paths for collinear altermagnets. The method selects the centroid of the conventional irreducible wedge used in routine band-structure calculations as the representative general k-point, maps it to a spin-flip-related partner, and inserts paired segments through these points into the standard high-symmetry path; these segments systematically sample the interior of the irreducible wedge. We demonstrate the construction for all 54 three-dimensional combinations of extended Bravais lattice type and spin Laue group across the six crystal systems that support collinear altermagnetism, and for the 12 two-dimensional cases spanning the four compatible two-dimensional Bravais lattices. Representative band structures are shown for the distinct lattice/path cases. With AlterSeeK-Path, these band structures can be constructed with essentially the same effort as conventional band structures.
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All authors Yujia Teng, Mesfin Eshete, Andrea Urru, Daniel Seleznev, Se Young Park, Sebastian E. Reyes-Lillo, Karin M. Rabe

Materials Science

Systematic display of the spin splitting in band structures of representative altermagnetic crystals

Mesfin Eshete, Yujia Teng, Andrea Urru et al. (+4 more)

In this work we demonstrate a novel approach to exhibit the unique spin splitting that is typical of collinear altermagnets. This approach is to plot band structures on Brillouin zone paths that sample general k-points to show a representative picture that corresponds to Brillouin zone averages. This is in contrast to conventional band structure plotting which plots band structures on the highest-symmetry points and lines, and thus in many cases can fail to show any altermagnetic spin splitting at all. Our investigation compares the new approach with the band structures of collinear altermagnets using conventional band structure plotting. We report the band structure and symmetry analysis for MnTe, CrSb, SmFeO3, ScCrO3, LaMnO3, TlCrO3, HoFeO3, InCrO3 and DyFeO3. This result clearly demonstrates the advantage of this novel method for displaying the spin splitting of collinear altermagnets.
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All authors Mesfin Eshete, Yujia Teng, Andrea Urru, Daniel Seleznev, Se Young Park, Sebastian E. Reyes-Lillo, Karin M. Rabe

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

HiPoly: a hierarchical polymer-native AI framework for property prediction and generative design

Ge Sun, Gervasio Zaldivar, Yuan Tian et al. (+5 more)

Polymeric materials are central to modern technologies, with applications ranging from energy to health and transportation. Although AI has made significant advances in materials discovery, the hierarchical structure of polymers across multiple length scales makes them inherently difficult to represent in a unified and physically meaningful way. Here we introduce HiPoly, a polymer-native AI framework that processes complete polymer descriptions through a three-level hierarchical graph architecture built on the G2RINS representation. HiPoly encodes stochastic inter-monomer connectivity, composition, and molecular weight directly within its architecture, using physically motivated design principles that mirror the multi-scale nature of polymeric systems. The framework establishes an end-to-end AI-driven workflow from experimental formulation data to property prediction, generative molecular design, and physics-based validation through molecular simulations, all unified by a single polymer representation. We demonstrate state-of-the-art prediction accuracy for thermophysical properties of multi-component polymer systems, with ablation studies confirming that each hierarchical design choice contributes independently to model performance. As an example, the generative design pathway is applied here to the discovery of sustainable alternatives to persistent fluorinated polymers, where it is possible to identify and independently validate PFAS-free candidates with target surface-energy properties. This work demonstrates how polymer-native AI can accelerate discovery by linking representation, prediction, and design across complex polymer chemistries.
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All authors Ge Sun, Gervasio Zaldivar, Yuan Tian, Gustavo Perez Lemus, Juhae Park, Daryna Safarian, Ming Han, Juan J. de Pablo