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Physics Condensed Matter Materials Science

cond-mat.mtrl-sci Watch Materials Science

Thursday 26 March

Materials Science

Charge and spin photogalvanic effects in the p-wave magnet NiI2

Giuseppe Cuono, Srdjan Stavric, Javier Sivianes Castano et al. (+4 more)

NiI2 is an exotic van der Waals material in which a noncollinear spin spiral breaks spatial inversion symmetry without sizeable structural distortion, generating improper ferroelectric polarization, and stabilizing p-wave magnetic states with electron-volt-scale odd-parity spin splitting. Using first-principles calculations, here we establish that nonlinear optical transport can directly probe and separate these effects. Magnetically-induced inversion breaking associated with the spin spiral produces a photogalvanic shift current under linearly polarized light, with conductivities exceeding those of conventional ferroelectrics. In contrast, a large photogalvanic injection current under circularly polarized light originates from helicity-selective transitions between spin-split states at opposite crystal momenta, directly exposing the nonrelativistic p-wave spin texture. We further predict pure spin photocurrents whose flow direction exchanges with that of the charge current under linear and circular excitation. The ability to generate and control pure spin currents without accompanying charge currents makes NiI2 a promising material platform for all-optical spin injection in van der Waals heterostructures.
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All authors Giuseppe Cuono, Srdjan Stavric, Javier Sivianes Castano, Julen Ibanez-Azpiroz, Paolo Barone, Andrea Droghetti, Silvia Picozzi

Materials Science

Interfacial charge-transfer in 3d/5d complex oxide heterostructures

Arun Kumar Jaiswal, Di Wang, Ji Soo Lim et al. (+6 more)

Interfacial charge transfer (ICT) provides a powerful route to engineer electronic phases in correlated oxide heterostructures, yet predictive design principles remain elusive. Here, we systematically investigate superlattices composed of the 5d spin-orbit coupled semimetal SrIrO3 and a series of correlated 3d perovskites (LaMnO3, LaFeO3, LaCoO3, and NdNiO3), thereby establishing a quantitative framework for ICT across 3d/5d interfaces. Combining element-specific x-ray absorption spectroscopy with spatially resolved electron energy loss spectroscopy, a homogeneous electron transfer from the 5d to the 3d layers is directly quantified, reaching up to 0.35 e per unit cell in the cobaltate superlattice. We show that the magnitude of ICT scales linearly with the difference in electronegativity between the transition-metal oxide layers, identifying electronegativity-driven band alignment as the dominant mechanism for ICT. Beyond interfacial doping, we find that strong 3d-5d hybridization induces a complete low-spin to high-spin conversion in the cobaltate layers, demonstrating interface-controlled spin-state engineering without chemical substitution. These results establish electronegativity mismatch as a predictive design parameter for correlated oxide interfaces and provide a materials platform for tailoring band filling, orbital hierarchy, and spin configurations in quantum oxide heterostructures, paving the way towards advanced oxide electronics and next-generation information technologies.
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All authors Arun Kumar Jaiswal, Di Wang, Ji Soo Lim, Shruti Roy, Fabrice Wilhelm, Vanessa Wollersen, Andrei Rogalev, Matthieu Le Tacon, Dirk Fuchs

Materials Science

Berry curvature induced giant anomalous and spin texture driven Hall responses in the layered kagome antiferromagnet GdTi3Bi4

Shobha Singh, Shivam Rathod, Rong chen et al. (+5 more)

In recent years, layered kagome magnets have emerged as promising platforms for Berry-curvature engineering and unconventional transport phenomena. Here, we present the single-crystal growth, magnetization, and electrical transport characterizations of the van der Waals-like layered antiferromagnet GdTi3Bi4. The system exhibits pronounced field-induced first-order phase transitions. Comprehensive frequency, temperature, and field-dependent ac susceptibility measurements, and Hall analysis, reveals the formation of a spin-cluster-like glassy magnetic phase attributed to noncollinear spin textures. Additionally, the system demonstrates a colossal anomalous Hall conductivity {\sigma}_xy^{A}~ 8.6(7)10^{3} Ohm-1 cm-1 at 2 K). Detailed scaling analyses reveal the coexistence of skew scattering and intrinsic Berry-curvature contributions to the anomalous Hall effect. First-principles calculations highlight flat-band near the Fermi level, with f-electrons of the Gd ion contributing large intrinsic Hall response. Thus, GdTi3Bi4 emerges as a rare layered kagome magnet, exhibiting Berry curvature-induced giant anomalous and spin texture-driven Hall responses, providing a versatile platform for exploring spin-texture physics and advancing low-dimensional spintronic functionalities.
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All authors Shobha Singh, Shivam Rathod, Rong chen, Lipika, Sneh, Rie Y. Umetsu, Yan Sun, Kaustuv Manna

Materials Science

Martensitic-like transition between liquid crystalline and crystalline phases of prototypical discotic organic semiconductor

Nurjahan Khatun, Joe F. Khoury, Agnes C. Nkele et al. (+7 more)

Phase transitions between crystalline solids occur either through the nucleation and growth mechanism, a process that is slow and destructive or through the diffusion-less and order preserving Martensitic route. In both organic and inorganic materials, Martensitic transformations are known to occur only between phases with crystalline symmetry. We demonstrate here that for canonical discotic organic semiconductor HAT6, the transition between the liquid crystalline columnar hexagonal phase (ColH) and the crystalline solid can occur through a mechanism that exhibits the hallmarks of Martensitic transformations: orientational correlations between parent and daughter phases, structural reversibility, and ultrafast kinetics. To access Martensitic-like solidification, the ColH phase of HAT6 is biaxially aligned in lithographically defined microchannels and crystallization is induced on deep supercooling. The transition mechanism is studied using a combination of polarized optical microscopy and X-ray scattering. At the largest accessible supercooling, the ColH - Crystal phase transition occurs at speeds of ~100 micrometer/s, a value that is seven orders of magnitude greater than the theoretical prediction for growth from isotropic melts. Our work suggests that Martensitic-like transformations can occur even between liquid crystals and crystals and are therefore more general than previously believed. Further, our work demonstrates that Martensitic-like transformations of anchored liquid crystals can be used to grow biaxially aligned crystals of organic molecules over arbitrarily long distances. As lattice alignment over large areas is desirable for devices like field-effect transistors and as several high-performance molecular semiconductors exhibit a ColH phase, our results hold general significance for organic electronics.
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All authors Nurjahan Khatun, Joe F. Khoury, Agnes C. Nkele, Lingyu Wang, Tieqiong Zhang, Partha P. Paul, Paul Chibuike Okoli, Nabila Shamim, Matteo Pasquali, Kushal Bagchi

Materials Science

Self-thermometry measurements of the adiabatic temperature change in first-order phase transition magnetocaloric materials

Daniela O. Bastos, André M. R. Soares, Leonor Andrade et al. (+8 more)

Accurately measuring the magnetocaloric effect is necessary to foster the development of magnetic refrigeration devices. However, current methods are inconvenient, requiring different instruments to measure each individual property or a custom-made setup. By measuring the time-varying magnetization in a commercially available VersaLab\textsuperscript{\textregistered} PPMS\textsuperscript{\textregistered} from Quantum Design, we have determined the adiabatic temperature change ($\Delta$T$_{\textrm{ad}}$) of the first-order phase transition material Gd$_5$Si$_2$Ge$_2$, for a magnetic field change of 0 to 1 T, under high vacuum ($<$ 0.1 mTorr). For each temperature and magnetic field, the equilibrium magnetization is used as the magnetization-to-temperature conversion curve, allowing us to extend the validity of a previously proposed technique to the first-order phase transition material Gd$_5$Si$_2$Ge$_2$, which exhibits significant hysteresis. Our method thus enables full characterization (magnetic entropy change, adiabatic temperature change, and heat capacity) of any magnetocaloric material, whether it has a first-order or a second-order phase transition, using a single instrument. Comparing to a directly measured $\Delta$T$_{\textrm{ad}}$, our method resulted in a peak $\Delta$T$_{\textrm{ad}}$ value of 4.47 K, within 1% of the directly measured value for a sample of the same composition.
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All authors Daniela O. Bastos, André M. R. Soares, Leonor Andrade, Randy K. Dumas, João S. Amaral, Kyle Dixon-Anderson, Yaroslav Mudryk, Victorino Franco, João P. Araújo, Rafael Almeida, João H. Belo

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

Correlation-Driven Orbital Order Realizes 2D Metallic Altermagnetism

Nirmalya Jana, Atasi Chakraborty, Anamitra Mukherjee et al. (+1 more)

Two-dimensional metallic altermagnets are rare, and no correlated 2D material has been established to host large nonrelativistic spin splitting. Here we show that spontaneous orbital order, driven by electronic correlations and Fermi surface nesting, provides a general microscopic route to two-dimensional metallic altermagnetism. Antiferro-orbital ordering between the d$_{xz}$ and d$_{yz}$ orbitals breaks the equivalence of magnetic sublattices with opposite spins and generates a symmetry-enforced altermagnetic spin texture. As a concrete realization, we identify monolayer YbMn$_2$Ge$_2$ as a stable correlated metallic altermagnet exhibiting giant nonrelativistic spin splitting of order 1 eV. The resulting phase supports an exceptionally large and gate-tunable transverse spin conductivity. These results establish correlation-driven orbital order as a robust and general mechanism for designing correlated altermagnets with large spin splitting.
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All authors Nirmalya Jana, Atasi Chakraborty, Anamitra Mukherjee, Amit Agarwal

Materials Science

Machine-Learned Interatomic Potentials for Predicting Physicochemical Properties of Molten Metal-Salt Systems for Calcium Electrolysis

M. Polovinkin, N. Rybin, D. Maksimov et al. (+5 more)

The design of efficient electrolysis devices for pure metal production requires accurate data on the properties of the melts used in the process. This work focuses on two key systems for calcium production: the molten Ca-Cu alloy and the CaCl$_2$-KCl electrolyte. High-temperature experiments are often expensive and time-consuming; however, we demonstrate that molecular dynamics (MD) simulations driven by machine-learned Moment Tensor Potentials (MTPs), trained on highly accurate density functional theory data, offer an effective and accurate alternative. Our MTP-driven MD simulations accurately reproduce the structural, thermodynamic, and transport properties across a range of temperatures and compositions relevant to electrolysis systems. We report calculated densities, radial distribution functions, heat capacities, thermal conductivities, ionic conductivities (for the electrolyte), viscosities, and diffusion coefficients, with deviations from experimental data within 20%. The strong agreement between calculations and experiments validates the proposed approach, establishing a robust framework for the computational exploration and optimization of liquid systems in metallurgical applications.
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All authors M. Polovinkin, N. Rybin, D. Maksimov, F. Valiev, A. Khudorozhkova, M. Laptev, A. Rudenko, A. Shapeev

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

Flat band driven competing charge and spin instabilities in the altermagnet CrSb

A. Korshunov, M. Alkorta, C.-Y. Lim et al. (+8 more)

The confinement of electronic wavefunctions in momentum space can give rise to flat electronic bands, where the quenching of kinetic energy enhances the density of states and amplifies interaction effects. Such conditions are fertile ground for emergent quantum phases, as spin, charge and lattice degrees of freedom become strongly entangled. In these regimes, subtle competitions between intertwined order parameters often dictate the macroscopic ground state, producing complex and sometimes unexpected collective behavior. Here we show that the altermagnet CrSb provides a realization of this scenario, and uncover short-range charge-order fluctuations at the M point of the Brillouin zone, q*=(1/2 0), persisting above the Neel temperature (TN). Remarkably, these fluctuations collapse upon entering the magnetically ordered phase, revealing a direct and robust competition between charge and spin order. At TN, the phonon dispersion at q* develops a pronounced Kohn-like anomaly, signaling strong electron-phonon coupling in the vicinity of the magnetic transition. Below TN, exchange striction dramatically renormalizes the associated soft phonon mode by approximately ~6 meV, the largest spin-phonon coupling ever reported. First-principles calculations attribute this behavior to a strong coupling between nearly dispersionless electronic states and a phonon branch that appears unstable at the harmonic level only when no magnetic order is considered, revealing the large sensitivity of the lattice to magnetic symmetry breaking. The competition between charge and spin order parameters, amplified by flat-band physics, drives the observed phonon anomaly and its abrupt reconstruction at TN. With its chemically simple structure and symmetry-protected altermagnetic state, CrSb emerges as a model platform to explore how flat electronic bands mediate giant spin-phonon coupling and competing broken symmetries.
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All authors A. Korshunov, M. Alkorta, C.-Y. Lim, F. Ballester, Cong Li, Zhilin Li, D. Chernyshov, A. Bosak, M. G. Vergniory, Ion Errea, S. Blanco-Canosa

Materials Science

Upcycling solar glass into Ce-doped oxyfluorides: spectroscopic and crystallization properties

Marcos Paulo Belançon, Rafaela Valcarenghi, Marcelo Sandrini et al. (+9 more)

Oxyfluorides containing up to 80 wt% recycled glass from end-of-life solar panels have been investigated. Reduced processing temperature and high transparency have shown that the material has potential for optical applications. In this work, cerium-doped samples were investigated. Spectroscopic study reveals the presence of Ce$^{3+}$, and luminescence from these ions and oxygen-deficient centers was detected. Raman demonstrated that cerium affects the glass network by promoting polymerization. In turn, thermal analysis indicated some changes in the crystallization events between 500-800 $^o$ C, which were confirmed by in situ X-ray powder diffraction measurements. Crystallization of fluorite, xonotlite, and combeite was confirmed, while other phases give minor contributions to the XRD patterns. Cerium addition reduced the formation of xonotlite, mainly above 700 $^o$ C. The potential applications of the material and the further studies required are discussed.
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All authors Marcos Paulo Belançon, Rafaela Valcarenghi, Marcelo Sandrini, Brenno Greatti, Robson Ferrari Muniz, Vitor Santaella Zanuto, Sandra Ory, Aurélien Canizares, Maxence Vigier, Emmanuel Veron, Mathieu Allix, Michael Pitcher

Materials Science · Cross-listed from quant-ph

Epitaxial CeO2 Films as a Host for Quantum Applications

Pralay Paul, Kusal M. Abeywickrama, Nisha Geng et al. (+18 more)

In highly purified host, the coherence of quantum emitters is ultimately limited by hyperfine interactions between the emitter and lattice nuclei possessing non-zero nuclear magnetic moments. This limitation can only be mitigated through isotopic purification. In this work, we investigate CeO2 as a host composed entirely of nuclei with zero nuclear moment. High-quality CeO2 thin films were grown by PLD and doped with Tm and Er ions. Structural characterization using X-ray diffraction, atomic force microscopy, and ion channeling confirms single-crystalline, atomically smooth films with dopants substitutionally incorporated at Ce lattice sites. Photoluminescence lifetime measurements show significantly longer lifetimes for Er-doped CeO2 (2.9 - 5.3 ms) compared with Tm-doped films (14 - 68 {\mu}s). Moreover, the Er-doped PLD films exhibit longer lifetimes at ~1% dopant concentration than previously reported for MBE-grown films. Density functional theory calculations reveal a substantial overlap between unoccupied O 2p and Tm 4f states near the valence band maximum, whereas Er 4f states remain well isolated. This electronic interaction likely introduces non-radiative recombination pathways in Tm-doped CeO2, explaining the reduced lifetimes. These findings highlight the importance of selecting appropriate dopant-host combinations and optimized growth conditions to minimize non-radiative channels for quantum applications.
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All authors Pralay Paul, Kusal M. Abeywickrama, Nisha Geng, Mritunjaya Parashar, Levi Brown, Mohin Sharma, Darshpreet Kaur Saini, Melissa Ayala Artola, Todd A. Byers, Bibhudutta Rout, Yiwei Ju, Xiaoqing Pan, Sumit Goswami, Sreehari Puthan Purayil, Casey Kerr, Dhiman Biswas, Ben Summers, Bin Wang, Horst Hahn, Alisa Javadi, T. Venkatesan

Materials Science

Pulsed Laser Template Engineering- PLATEN

Dhiman Biswas, Junyeob Song, Francisco Guzman et al. (+16 more)

Thin films of functional inorganic materials, particularly oxides, play a vital role in optoelectronics, enabling applications that range from active optical components to MEMS-based architectures. Achieving high aspect ratio patterning of these functional materials remains a significant challenge, as many of their constituent elements do not readily form volatile compounds required for conventional reactive ion etch processes. We introduce a novel approach, Pulsed Laser Template ENgineering (PLATEN), which offers a more accessible route for patterning materials that are typically difficult to etch. This technique involves depositing functional films using the Pulsed Laser Deposition (PLD) process onto silicon substrates that have been pre-patterned using reactive ion etching to create high aspect ratio features. Due to the highly forward-directed nature of the PLD process, the deposited films replicate closely the topography of the patterned silicon, without coatings the sidewalls. This process remains effective even at feature sizes down to approximately 50 nm. The oxide films replicate the underlying silicon pattern to a thickness of 80 nm. For thickness beyond 80 nm the patterns develop a waist at the midpoint which scales with film thickness and is not dependent on the feature size. In this paper, we present a detailed analysis of the PLATEN process, including deviations from ideal pattern replication in sub-micron features as a function of film thickness, and demonstrate near single crystalline growth of oxides on the patterned silicon substrate, demonstrating the potential of PLATEN technique for active opto-electronic materials.
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All authors Dhiman Biswas, Junyeob Song, Francisco Guzman, Levi Brown, Yiwei Ju, Nisha Geng, Pralay Paul, Sumit Goswami, Casey Kerr, Sreehari Puthan Purayil, Ben Summers, Preston Larson, Binbin Weng, Bin Wang, Horst Hahn, Xiaoxing Pan, Alisa Javadi, Henri Lezec, Thirumalai Venkatesan

Materials Science

Decoding the Electronic and Structural Fingerprints of Single-Atom Catalysts via DFT-Assisted XANES Analysis

Petr Lazar and Michal Otyepka

Single-atom catalysts (SACs), composed of isolated metal atoms dispersed on solid supports, represent the ultimate expression of atomic efficiency in catalysis. Their remarkable activity and selectivity arise from local coordination environments and adjustable oxidation states, yet precise determination of these features remains an enduring challenge. Among modern characterization techniques, X-ray absorption near-edge structure (XANES) spectroscopy stands out for its sensitivity to both electronic and geometric structure, though its interpretation is often constrained by empirical comparison with bulk references. Here we introduce a density functional theory (DFT) based computational spectroscopy framework for the quantitative interpretation of Cu K-edge XANES spectra. We then employ this framework to reveal the oxidation state, coordination geometry, and hydration environment of Cu single atoms supported on cyanographene, demonstrating direct correspondence between spectral signatures and atomic-scale structure. This methodology establishes a robust and transferable route for connecting XANES features with the underlying electronic and structural characteristics of SACs, thereby advancing the rational design of atomically precise catalysts.
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Materials Science

Distinguishing apparent and hidden altermagnetism via uniaxial strain in $\mathrm{CsV_2Te_2O}$-family

San-Dong Guo and Yang Liu

The hidden altermagnetism has been theoretically proposed and then experimentally confirmed in metal $\mathrm{Cs_{1-\delta}V_2Te_2O}$, which exhibits two nearly degenerate ground-state magnetic configurations (C-type and G-type) corresponding respectively to apparent and hidden altermagnetism. Here, we propose that in-plane uniaxial strain can be utilized to distinguish apparent and hidden altermagnetism. Under uniaxial strain, apparent altermagnetism exhibits an obvious net magnetic moment, whereas hidden altermagnetism maintains zero net magnetic moment. The magnetic moment induced by uniaxial strain here, namely the piezomagnetic effect, differs from that in semiconductors, where strain must be applied first followed by carrier doping to generate net magnetism. First-principles calculations verify our proposal, revealing that the magnetic moment induced by uniaxial strain in C-type antiferromagnetic $\mathrm{CsV_2Te_2O}$ is much larger than that in the previously studied altermagnetic semiconductors. Furthermore, we also investigate the electronic state transitions of semiconductors featuring a crystal structure analogous to $\mathrm{CsV_2Te_2O}$ under uniaxial strain, and verify our proposal in specific material via first-principles calculations. Our work provides an experimentally feasible strategy to distinguish apparent and hidden altermagnetism in material $\mathrm{Cs_{1-\delta}V_2Te_2O}$, and extends the physical implication of the piezomagnetic effect, which can be directly verified in experimentally synthesizable $\mathrm{KV_2Se_2O}$ and $\mathrm{Rb_{1-\delta}V_2Te_2O}$.
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Materials Science

Effect of Pb doping on the crystallization process and thermoelectric properties of Ge2Sb2Te5 phase change material

M. Zhezhu, A. Vasil'ev, M. Yaprintsev et al. (+3 more)

Phase change materials based on Ge-Sb-Te alloys are widely explored for their potential in both memory devices and thermoelectric applications. In this study, films of Ge2Sb2Te5 (GST) doped with varying concentrations of Pb were prepared and systematically investigated to trace the effect of Pb doping on crystallization-induced phase transformations and thermoelectric properties. Via X-ray diffraction and Raman spectroscopy, the impact of Pb doping on the crystallization behavior was revealed and examined. According to the specific electrical resistivity measurements, the Pb doping resulted in decreasing both the amorphous-to-cubic and cubic-to-hexagonal transition temperatures, thereby facilitating the formation of the hexagonal phase at a lower thermal regime. Furthermore, Seebeck coefficient and electrical resistivity data of hexagonal Pb-doped GST were used to calculate the power factor, PF. A PF maximum equal to 1.3 was found for 2.5 at. Pb-GST at 633 K, with the highest carrier mobility also observed for this composition. Controlled Pb doping effectively modulates both structural transitions and thermoelectric performance, highlighting the potential of Pb-GST for applications that combine phase-change memory and thermoelectric functionality, such as opto-thermoelectric devices and non-volatile thermoelectric sensors.
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All authors M. Zhezhu, A. Vasil'ev, M. Yaprintsev, A. Musayelyan, E. Pilyuk, O. Ivanov

Materials Science

Dual migration modes of unfaulted disconnections on curved twin boundaries

Hongrui He, Hao Lyu and Xueting Si

Grain boundary migration governs microstructural evolution in crystalline materials, directly influencing mechanical properties such as strength and thermal stability. Disconnections, which are line defects formed at grain boundaries in response to local curvature, have been identified as critical carriers of boundary migration. Here, we investigate the glide of unfaulted disconnections (UFDs) on a coherent twin boundary in aluminum at elevated temperatures using molecular dynamics simulations combined with the Nudged Elastic Band (NEB) method. Our results reveal a striking bifurcation in migration behavior depending on the disconnection core structure. UFDs with a pure edge Burgers vector migrate via a thermally activated double-kink mechanism, exhibiting a migration velocity that increases monotonically with temperature. In contrast, UFDs containing a screw dipole component possess an energy barrier approximately eight times lower, and their core structure undergoes a continuous transformation during glide, giving rise to stochastic, bidirectional motion with no systematic temperature dependence. These findings demonstrate that the disconnection core structure fundamentally dictates the migration mode and kinetics of twin boundaries, offering new mechanistic insights into disconnection-mediated grain boundary migration.
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Materials Science

Forster energy transfer boosts indirect anisotropic interlayer excitons in 2L-MoSe2/perovskite heterostructures

Yingying Chen, Zihao Jiao, Haizhen Wang et al. (+1 more)

Interlayer excitons (IXs) in two-dimensional (2D) van der Waals heterostructures have attracted considerable attention due to their unique optical and electronic properties. Owing to the spatially indirect nature, the radiative emission efficiency highly sensitive to interlayer twist angles. Further considering that their uniformly oriented out-of-plane dipole moments limit directional emission, strategies to simultaneously improve emission efficiency and induce optical anisotropy warrant in-depth investigation. In this work, we report significant photoluminescence (PL) enhancement and optical anisotropy of IXs in 2L-MoSe2/perovskite heterostructures mediated by energy transfer from ReS2. We attribute this enhancement to Forster resonance energy transfer (FRET), which increases the 2L-MoSe2 emission by approximately eight-fold at room temperature, and nearly doubles the emission intensity of momentum-indirect IXs in 2L-MoSe2/perovskite heterostructures at 78 K. Importantly, the optical anisotropy of ReS2 can be effectively imprinted onto 2L-MoSe2 and associated indirect IXs during the energy transfer process, yielding a linear dichroism of approximately 1.1 for both intralayer excitons and IXs with identical polarization directions. These findings expand the scope of IX study beyond direct bandgap materials with strong intrinsic emission to include systems with indirect bandgaps, offering new avenues for realizing high-performance polarization-sensitive optoelectronic devices.
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All authors Yingying Chen, Zihao Jiao, Haizhen Wang, Dehui Li

Materials Science

The ground state of CuInP$_2$S$_6$ thin films: A study of the deep potential method

Shengxian Li, Jiaren Yuan, Tao Ouyang et al. (+2 more)

The two-dimensional ferroelectric (FE) material CuInP$_2$S$_6$ (CIPS) has garnered considerable interest due to its out-of-plane ferroelectricity at room temperature. However, a notable discrepancy exists between experiments and density functional theory (DFT) calculations regarding the ground state of CIPS thin films: experiments suggest a state with net polarization, while DFT predicts an antiferroelectric (AFE) state as the lowest-energy state. Here, we investigate the stability of polarization states in CIPS thin films by combining first-principles calculations with the deep potential (DP) method. Our results reveal that for films thicker than the bilayer, an AFE state that has intralayer AFE ordering in the inner layers and intralayer FE ordering in the two surface layers has the lowest electronic energy. This state is significantly lower than the uniform FE state. In addition, we find that a ferrielectric (FiE) state with pure intralayer FE ordering is very close to the AFE state in energy. By using the DP model, we calculated the phonon free energy of CIPS thin films. For the monolayer, the intralayer FE ordering possesses a lower phonon free energy than the intralayer AFE ordering. This energetic preference for the intralayer FE ordering maintains as the thickness grows. Consequently, when the phonon-free energy is incorporated, the FiE state becomes energetically favorable over the AFE state for multilayers CIPS. Our findings demonstrate that the inclusion of vibrational entropy stabilizes the FiE state as the ground state in multilayers CIPS at finite temperatures, reconciling the previous discrepancy between experimental observations and DFT predictions. This insight is vital for understanding the FE properties of CIPS and its potential applications in devices.
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All authors Shengxian Li, Jiaren Yuan, Tao Ouyang, Anlian Pan, Mingxing Chen

Wednesday 25 March

Materials Science · Cross-listed from cs.AI

Toward Full Autonomous Laboratory Instrumentation Control with Large Language Models

Yong Xie, Kexin He and Andres Castellanos-Gomez

The control of complex laboratory instrumentation often requires significant programming expertise, creating a barrier for researchers lacking computational skills. This work explores the potential of large language models (LLMs), such as ChatGPT, and LLM-based artificial intelligence (AI) agents to enable efficient programming and automation of scientific equipment. Through a case study involving the implementation of a setup that can be used as a single-pixel camera or a scanning photocurrent microscope, we demonstrate how ChatGPT can facilitate the creation of custom scripts for instrumentation control, significantly reducing the technical barrier for experimental customization. Building on this capability, we further illustrate how LLM-assisted tools can be extended into autonomous AI agents capable of independently operating laboratory instruments and iteratively refining control strategies. This approach underscores the transformative role of LLM-based tools and AI agents in democratizing laboratory automation and accelerating scientific progress.
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Materials Science · Cross-listed from physics.chem-ph

Implementation of the multigrid Gaussian-Plane-Wave algorithm with GPU acceleration in PySCF

Rui Li, Xing Zhang, Qiming Sun et al. (+3 more)

We introduce a GPU-accelerated multigrid Gaussian-Plane-Wave density fitting (FFTDF) approach for efficient Fock builds and nuclear gradient evaluations within Kohn-Sham density functional theory, as implemented in the GPU4PySCF module of PySCF. Our CUDA kernels employ a grid-based parallelization strategy for contracting Gaussian basis function pairs and achieve up to 80% of the FP64 peak performance on NVIDIA GPUs, with no loss of efficiency for high angular momentum (up to f-shell) functions. Benchmark calculations on molecules and solids with up to 1536 atoms and 20480 basis functions show up to 25x speedup on an H100 GPU relative to the CPU implementation on a 28-core shared memory node. For a 256-water cluster, the ground-state energy and nuclear gradients can be computed in ~30 seconds on a single H100 GPU. This implementation serves as an open-source foundation for many applications, such as ab initio molecular dynamics and high-throughput calculations.
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All authors Rui Li, Xing Zhang, Qiming Sun, Yuanheng Wang, Junjie Yang, Garnet Kin-Lic Chan

Materials Science

Suppression of Metallic Transport in Nitrogen-rich Two-Dimensional Transition Metal Nitrides

Hongze Gao, Da Zhou, Nguyen Tuan Hung et al. (+12 more)

The recent experimental realization of two-dimensional (2D) transition metal nitrides (TMNs, e.g., Mo5N6, {\delta}-MoN, and W5N6) opens new opportunities for exploring their fundamental physical properties at the two-dimensional limit. In this work, we propose a unified picture of transport phenomena in the nitrogen-rich 2D W5N6 and Mo5N6, and the stoichiometric 2D {\delta}-MoN based on several observations and first-principles calculations. Temperature coefficient of resistance (TCR) and magnetoresistance (MR) from Hall measurements consistently suggest disorder-induced transport mechanism at low temperatures (10-30 K). Notably, we observe a transition from metal to semimetal driven by the variation of nitrogen content in TMNs, supported by the suppressed density of states at the Fermi energy in nitrogen-rich TMNs (e.g. Mo5N6) from first-principle calculations. Carrier density calculations of bulk TMNs and 2D TMNs with -NH termination groups further reveal the switching of majority carrier type of Mo5N6 at reduced thickness, which is in great agreement with Hall measurement results. Our findings demonstrate that high nitrogen content in metallic molybdenum nitrides can induce the transition to a semimetallic phase at the 2D limit, shedding light on both the fundamental aspects of these materials and directions in future material design.
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All authors Hongze Gao, Da Zhou, Nguyen Tuan Hung, Chengdong Wang, Zifan Wang, Ruiqi Lu, Yuxuan Cosmi Lin, Jun Cao, Michael Geiwitz, Gabriel Natale, Kenneth S. Burch, Xiaofeng Qian, Riichiro Saito, Mauricio Terrone, Xi Ling

Materials Science

Efficient all-electron Bethe-Salpeter implementation using crystal symmetries

Jörn Stöhler, Stefan Blügel and Christoph Friedrich

We describe an all-electron implementation of the Bethe-Salpeter equation (BSE) for the calculation of optical absorption spectra in the full-potential linearized augmented-plane-wave (FLAPW) method. So far, FLAPW implementations have resorted to a simple plane-wave basis for the bare and screened Coulomb potentials, thereby forgoing the all-electron description to some extent. In contrast, we expand the interaction potentials in the all-electron mixed basis. As in most implementations, the BSE is solved by the diagonalization of a two-particle Hamiltonian matrix, whose dimension is proportional to the number of $\mathbf{k}$ points. Due to the large number of $\mathbf{k}$ points required to converge the BSE, the resulting matrix becomes large even for small unit cells. We describe a method that exploits the crystal symmetries to accelerate the construction and diagonalization of the two-particle Hamiltonian. In particular, we employ group theoretical tools to bring the Hamiltonian into block-diagonal form. Furthermore, it is shown that often only one of the blocks needs to be taken into account for the optical absorption spectrum leading to a considerable speedup of the diagonalization step. The code allows for the inclusion of spin-orbit coupling and is parallelized with the possibility of storing the Hamiltonian in distributed memory over many nodes, keeping the memory demands low. To validate our implementation, we show optical absorption spectra and report exciton binding energies for bulk Si, LiF, and MoS$_2$. By exploiting the crystal symmetries, we can reduce the dimension of the Hamiltonian matrix of Si by a factor of five, resulting in a 125-fold speedup in its diagonalization. The calculated exciton binding energies of 22~meV and 76~meV for Si and MoS$_2$ are closer to experimental values than in previous BSE studies.
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Materials Science

Engineering Nonlinear Optical Responses via Inversion Symmetry Breaking in Bilayer Bi2Se3

Vineet Kumar Sharma, Alana Okullo, Barun Ghosh et al. (+2 more)

Paucity of naturally occurring noncentrosymmetric materials is stimulating growing interest in engineered two-dimensional systems for nonlinear optical applications. Here, we show that breaking inversion symmetry in centrosymmetric bilayer Bi$_2$Se$_3$ through twisting, point-defect insertion, or the application of an external electric field unlocks rich nonlinear optical responses. In twisted bilayer Bi$_2$Se$_3$ at the first commensurate angle of 21.78$^\circ$, we find peak shift and injection current conductivities of -14 $ nm.\mu AV^{-2}$ and 104 $\times 10^8$ $nm.A V^{-2}s^{-1}$, respectively, which lie in the visible spectrum and enable efficient THz applications. The external electric field and point-defect insertion both transform the bilayer into C$_ {3v}$ symmetry, with the selenium vacancy (V$_{Se}$) achieving peak shift and injection current conductivities of -190 nm.$\mu AV^{-2}$ and -170 $\times 10^8$ $nm.A V^{-2}s^{-1}$. In all three cases, the peak nonlinear optical responses are found to be comparable to those of benchmark 2D materials such as GeS, and the broadband responses, including helicity-dependent current generation, make these engineered bilayers viable candidates for next-generation 2D photovoltaics.
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All authors Vineet Kumar Sharma, Alana Okullo, Barun Ghosh, Arun Bansil, Sugata Chowdhury

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

Permeation of hydrogen across graphdiyne: molecular dynamics vs. quantum simulations and role of membrane motion

Mateo Rodríguez, José Campos-Martínez and Marta I. Hernández

Previous research based on electronic structure calculations and molecular dynamics (MD) simulations have demonstrated that graphdiyne (GDY) is a very suitable two-dimensional membrane for the separation of small molecules in a gas mixture of different species. However, quantum effects may play a role in the dynamics of these permeation processes when light molecules are the ones involved in the crossing of the GDY subnanometric pores. In this work we report rigorous quantum-mechanical calculations together with equivalent MD simulations of the transport of H2 molecules through a static GDY membrane, as a case study for the validity of the application to these problems of classical dynamics. The force fields employed are based on an improved Lennard-Jones formulation, with parameters optimized by means of accurate ab initio calculations. It is found that, although quantum effects are still significant at the temperatures of interest (between 250 and 350 K), MD simulations are able to reasonably reproduce the dependence of the quantum permeances with the temperature. Moreover, MD permeances computed with quantum corrections through Feynman-Hibbs effective potentials provide a lower bound to quantum permeances, while the pure classical counterpart gives an upper bound, thus leading to a well delimited range of confidence of the permeation results. Furthermore, within MD simulations it is possible to incorporate the thermal motion of the GDY layer and in this situation it is observed an enhancement of the permeances with respect to the fixed membrane case, due to a significant reduction of the permeation barriers when the GDY atoms are allowed to vibrate. It seems apparent therefore, that modeling the membrane motion is crucial to provide reliable simulations of the gas transport features.
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Materials Science

Concerted Electron-Ion Transport by Polyacrylonitrile Elucidated with Reactive Deep Learning Potentials

Rajni Chahal-Crockett, Michael D. Toomey, Logan T. Kearney et al. (+4 more)

Charge transport in polymers, such as polyacrylonitrile (PAN), is crucial for electronics and energy storage. For instance, PAN can transport cations e.g., Li+, by facilitating dynamic cation-nitrile coordination in batteries. However, little is known regarding the underlying role of complex reactive polymer configurations. Herein, we develop a deep-learning potential, trained on ab initio energies and forces of nonequilibrium reactive PAN configurations, to unravel the kinetics of PAN cyclization initiated by a nucleophile (OH- dissociated from LiOH) attacking the terminal nitrile carbon. We find, based on the reaction free-energetics, rates, and charge analysis, that the nucleophile attack producing the first ring is the rate-limiting step, which subsequently triggers Li+-coupled electron transfer along the PAN backbone, causing ~10,000 times faster sequential ring-formation of the remaining nitriles. PAN's extended configurations, where dipolar and H-bonding interactions are minimal, enable such rapid kinetics. By validating our computational findings with IR and NMR experiments, we establish a pathway for designing reactive polymers with enhanced charge transport for energy applications.
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All authors Rajni Chahal-Crockett, Michael D. Toomey, Logan T. Kearney, Yawei Gao, Joshua T. Damron, Amit K. Naskar, Santanu Roy

Materials Science

Visualizing Millisecond Atomic Dynamics of Nanocrystals in Liquid

Sungsu Kang, Jinho Rhee, Joodeok Kim et al. (+11 more)

Atomic structures of nanomaterials are inherently dynamic, continuously reshaped through interactions with chemical species and external stimuli. Such dynamics are further amplified as the size and dimensionality of nanomaterials are reduced. Despite advances in analytical methods, it remains challenging to capture structural dynamics of nanomaterials in reactive environments with both atomic spatial resolution and commensurate temporal resolution. Here, we directly visualize atomic-scale dynamics of gold (Au) nanocrystals in reactive liquid environments with millisecond-speed liquid cell electron microscopy (EM) and deep-learning denoising. We uncover reversible fluctuations in local crystallinity of Au nanocrystals dependent on the surrounding chemical environment. These transient fluctuations, driven by interactions at nanocrystal-liquid interfaces, critically influence dissolution kinetics and grain boundary relaxation. By overcoming the spatiotemporal limitations in conventional liquid cell EM, our findings provide insights into how transient nanoscale structures dictate the stability and reactivity of nanomaterials.
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All authors Sungsu Kang, Jinho Rhee, Joodeok Kim, Sam Oaks-Leaf, Minwoo Kim, Shengsong Yang, Chang Liu, Dongsu Kim, Sungin Kim, Binyu Wu, Won Bo Lee, David T. Limmer, A. Paul Alivisatos, Peter Ercius Jungwon Park

Materials Science · Cross-listed from cond-mat.supr-con

Electrodynamic Signatures of Bogoliubov Fermi Surfaces in Moiré Graphene

Ke Wang, Qijin Chen, Rufus Boyack et al. (+1 more)

Understanding the superfluid stiffness \(D_s\) is a central problem in flat-band superconductivity. It is often interpreted together with spectroscopic probes such as tunneling, since both ultimately reflect the same superconducting quasiparticles. Their relationship is nevertheless complicated in flat bands, where quantum-geometric contributions to \(D_s\) must be included. The situation in moiré graphene is particularly complex: tunneling experiments in some cases reveal an evolution between V- and U-shaped spectra together with a quite universal finite zero-bias conductance (ZBC). These two phenomena along with others have been argued to suggest the presence of a Bogoliubov Fermi surface (BFS), often generated by finite-momentum pair-density-wave (PDW) superconductivity. In this paper we calculate the superfluid stiffness in the presence of such a PDW. Virtual interband processes provide the familiar positive geometric contribution that gives phase rigidity to the flat-band condensate, allowing superconductivity to survive even in the presence of a BFS. At the same time, the multiband PDW pair structure enables the gapless BFS quasiparticles to respond to a phase gradient despite the negligible ordinary flat-band velocity. Their resulting counterflow reduces the stiffness even at zero temperature. As an experimentally accessible consequence, we predict a correlated evolution of the residual ZBC and the low-temperature stiffness: enhanced zero-bias spectral weight should accompany reduced phase rigidity. Observation of this correlation would support the presence of a BFS and indicate that the residual zero-energy states are intrinsic.
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All authors Ke Wang, Qijin Chen, Rufus Boyack, K. Levin

Materials Science

Chalcogen Doping Effect on the Insulator-to-Metal Transition in GdPS

Gokul Acharya, Rabindra Basnet, Santosh Karki Chhetri et al. (+5 more)

Topological semimetals offer a rich platform for exploring massless fermion physics and realizing exotic properties with potential technological applications. GdPS, a magnetic semiconductor derived from the nodal-line semimetal ZrSiS family, exhibits a field-induced insulator-to-metal transition driven by exchange splitting. This transition is accompanied by an unusual, isotropic, and gigantic negative magnetoresistance, attributed to negligible magnetic anisotropy resulting from the weak spin-orbit coupling of half-filled Gd3+ 4f orbitals and light S atoms. In this work, we investigate Se substitution, which is expected to enhance spin-orbit coupling. Indeed, we observe slightly increased magnetic anisotropy in magnetotransport. Moreover, Se substitution suppresses the field-induced insulator-to-metal transition, likely due to an enlarged band gap that demands a higher exchange splitting to close. These findings provide deeper insights into the interplay between spin-orbit coupling, magnetic anisotropy, and transport behavior in GdPS, offering guidance for future materials design for desired functionalities.
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All authors Gokul Acharya, Rabindra Basnet, Santosh Karki Chhetri, Dinesh Upreti, M. M. Sharma, Jian Wang, David Graf, Jin Hu

Materials Science · Cross-listed from cond-mat.supr-con

Probing picosecond depairing currents in type-II superconductors

E. Wang, M. Chavez-Cervantes, J. Satapathy et al. (+8 more)

Accessing the intrinsic critical current density (Jc*) in type II superconductors has significant fundamental and technological potential, both as a probe of the microscopic superconducting properties and as a means to increase current limits in high magnetic field devices and in electrical power systems. Yet, the experimental critical current density in type II superconductors (Jc), when measured with DC currents, is generally lower than the intrinsic limit, mostly due to vortex motion and self-heating. Here, we show that ultrafast picosecond electrical pulses, which interact with the material on timescales over which vortices are inertially immobile, carry supercurrents up to the intrinsic depairing limit Jc* >> Jc. We probe picosecond critical currents in NbN and YBa2Cu3O7 (YBCO), as representative s-wave and d-wave superconductors, respectively. In NbN, we find a sharp onset of the picosecond depairing at a current density as large as Jc*=2.2 Jc, a limit that is well described by microscopic dynamics based on BCS theory. In contrast, YBCO exhibits a gradual suppression of superconductivity as a function of the picosecond current, reflecting its d-wave symmetry. These results offer a powerful new probe of superconductors beyond the reach of conventional transport measurements. The ability to reach the depairing current may also lead to robust new platforms for superconducting electronics.
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All authors E. Wang, M. Chavez-Cervantes, J. Satapathy, T. Matsuyama, G. Meier, X. Zhang, L. You, F. Marijanovic, J.B. Curtis, E. Demler, A. Cavalleri

Materials Science · Cross-listed from cs.LG

How unconstrained machine-learning models learn physical symmetries

Michelangelo Domina, Joseph William Abbott, Paolo Pegolo et al. (+2 more)

The requirement of generating predictions that exactly fulfill the fundamental symmetry of the corresponding physical quantities has profoundly shaped the development of machine-learning models for physical simulations. In many cases, models are built using constrained mathematical forms that ensure that symmetries are enforced exactly. However, unconstrained models that do not obey rotational symmetries are often found to have competitive performance, and to be able to learn to a high level of accuracy an approximate equivariant behavior with a simple data augmentation strategy. In this paper, we introduce rigorous metrics to measure the symmetry content of the learned representations in such models, and assess the accuracy by which the outputs fulfill the equivariant condition. We apply these metrics to two unconstrained, transformer-based models operating on decorated point clouds (a graph neural network for atomistic simulations and a PointNet-style architecture for particle physics) to investigate how symmetry information is processed across architectural layers and is learned during training. Based on these insights, we establish a rigorous framework for diagnosing spectral failure modes in ML models. Enabled by this analysis, we demonstrate that one can achieve superior stability and accuracy by strategically injecting the minimum required inductive biases, preserving the high expressivity and scalability of unconstrained architectures while guaranteeing physical fidelity.
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All authors Michelangelo Domina, Joseph William Abbott, Paolo Pegolo, Filippo Bigi, Michele Ceriotti

Materials Science

Chiral Epitaxy: Enantioselective Growth of Chiral Nanowires on Low-Symmetry Two-Dimensional Materials

Noya Ruth Itzhak, Kate Reidy, Maya Levy-Greenberg et al. (+20 more)

Chiral crystals exhibit useful handedness-dependent properties, including spin selectivity and circularly polarized light sensitivity, yet controlling which enantiomer forms during synthesis remains a central challenge. Existing approaches utilize molecules in solution to template crystal growth, which restricts processing conditions and introduces organic contaminants incompatible with device fabrication. Enantioselective growth of a chiral crystal on a chiral surface via vapor-phase synthesis (chiral epitaxy) has not yet been demonstrated. Here, we show chiral epitaxy of aligned tellurium nanowires on a low-symmetry two-dimensional material, ReSe2. In situ electron microscopies suggest a mechanism where handedness is determined at nucleation by the interface energy difference between Te enantiomers and the chiral substrate surface. Chiral epitaxy provides a solvent-free, vapor-solid route to homochiral crystals compatible with semiconductor and quantum manufacturing processes.
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All authors Noya Ruth Itzhak, Kate Reidy, Maya Levy-Greenberg, Paul Anthony Miller, Chen Wei, Juan Gomez Quispe, Raphael Tromer, Olle Hellman, Shahar Joselevich, Aliza Ashman, Lothar Houben, Ifat Kaplan-Ashiri, Xiao-Meng Sui, Olga Brontvein, Katya Rechav, Laurent Travers, Pedro A. S. Autreto, Douglas S. Galvão, Federico Panciera, Oded Hod, Leeor Kronik, Frances M. Ross, Ernesto Joselevich