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Physics Condensed Matter Materials Science

cond-mat.mtrl-sci Watch Materials Science

Sunday 13 September

Materials Science

Time- and Frequency-Resolved Observation of Inverse Orbital Hall Effect in Gallium Nitride via Terahertz Polarimetry

Kota Aikyo, Tomohiro Fujimoto, Ami Mi Shirai et al. (+6 more)

Orbitronics has attracted significant attention as a platform for information storage and processing that exploits the orbital angular momentum (OAM) of electrons without the need for spin-orbit coupling. However, experimental evaluation of OAM-charge interconversion remains a challenge and the results are often controversial due to the coexistence of bulk and interfacial contributions and the complexity in sample structures. Here, using circularly polarized light pulses and terahertz (THz) polarimetry, we developed a non-contact method to observe the inverse orbital Hall effect as a bulk response within a single material without employing heterostructure samples. In a semiconductor GaN, we directly captured the OAM-to-charge current conversion of holes in the THz frequency range. By analyzing the sharp frequency dependence of the Hall conductivity, we disentangled the competing microscopic mechanisms and revealed the dominant role of extrinsic contributions to the orbital Hall effect in the dc limit. By contrast, the Hall conductivity at THz frequencies above the impurity scattering rate is attributed to the intrinsic Berry-curvature mechanism,allowing a quantitative comparison with the microscopic theory. Furthermore, the ultrafast dynamics of the inverse orbital Hall signal directly revealed sub-picosecond OAM relaxation of holes, comparable to that of phonon-mediated thermalization. The quantitative argument based on theoretical calculations suggested the existence of an even faster decay channel due to momentum redistribution by acoustic phonons, suggesting a sub-nanometer-scale OAM relaxation length. Our results provide comprehensive and crucial insights into OAM transport and establish an ultrafast, contact-free approach for investigating OAM-to-charge conversion.
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All authors Kota Aikyo, Tomohiro Fujimoto, Ami Mi Shirai, Yuta Murotani, Mitsuru Funato, Shinji Miwa, Jun Yoshinobu, Yoichi Kawakami, Ryusuke Matsunaga

Materials Science

Cryothermal Measurements of Variable-Emittance Coatings with Lower Phase Transition Temperatures for Space Thermal Control

Chloe Stoops, Vishwa Krishna Rajan and Liping Wang

Space thermal control is critically important to ensure proper operation of on-board equipment in a regulated temperature range. Passive thermal control with variable-emittance coatings (VECs) could help save power consumption in a dynamically changing space thermal environment. Vanadium dioxide (VO2) based VECs have been studied for space thermal control but its intrinsic phase transition around 68{\deg}C limits its wider space applications where lower temperature ranges are expected. In this work, we experimentally demonstrate enhanced radiative heat dissipation in space-like thermal environment via cryothermal measurements with VECs of undoped and tungsten doped VO2. The fabricated undoped VEC exhibits a large emittance change of 0.6 across the phase transition, while the 1 at.% tungsten doped one shows an appreciable emittance variable of 0.4 with phase transition temperature lowered by 25{\deg}C. A vacuum cryothermal setup is developed with a liquid nitrogen cooled coldfinger to mimic cold space thermal background and a custom-designed sample mount suspended by nylon wires. After careful calibration and validation, greatly enhanced radiative heat dissipation upon VO2 phase transition up to 3.5 times with transition temperature lowered by 25{\deg}C from 1 at.% tungsten doping is clearly observed from the cryothermal tests. In the actual space thermal environment, radiative heat flux could further increase across phase transition from 160 W/m2 to 650 W/m2 with undoped VO2 coating from 55{\deg}C to 80{\deg}C, and from 175 W/m2 to 493 W/m2 with 1 at.% tungsten doped VEC from 30{\deg}C to 55{\deg}C.
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Saturday 12 September

Materials Science

Ultrafast Magnetization Induced from Raman-Active Axial Chiral Phonons

Chuankun Huang, Alexander Milner, Jiaming Luo et al. (+8 more)

Axial chiral phonons, which carry angular momentum and exhibit unusually large magnetic moments, provide a new degree of freedom for controlling the time-reversal symmetry and magnetic properties of quantum materials. While infrared-active axial phonons are efficiently excited to large amplitudes by circularly polarized terahertz pulses, their application may be constrained by short lifetimes, small penetration depths, low spatial resolution, and limited availability of optical sources. Here, we report that an axial Raman-active phonon mode in CeF3 exhibits a significant magnetic moment and an exceedingly long lifetime that more closely matches the paramagnetic spin dynamics. The axial phonon population is resonantly driven by a near-infrared laser pulse with rotating linear polarization, known as an optical centrifuge, a coherent control scheme never applied to solids before. The phonon-driven magnetization observed by time-resolved Faraday rotation scales quadratically with incident power and rapidly decreases at high temperatures, consistent with phonon inverse Faraday effect from many-body spin-phonon coupling. Our findings open a new avenue for using shaped laser pulses from widely accessible light sources to manipulate coherent axial chiral phonons and ultrafast spintronics.
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All authors Chuankun Huang, Alexander Milner, Jiaming Luo, Jianbo Ye, Gaihua Ye, Junjie Zhang, Cynthia Nnokwe, Boris I. Yakobson, Rui He, Valery Milner, Hanyu Zhu

Materials Science

Spinodals and Domain Instabilities in Ionically-compensated Ferroelectric Films

Sergei V. Kalinin

A ferroelectric surface in contact with an ionic or molecular reservoir is intrinsically a ferroionic state in which polarization and compensating surface charge are thermodynamically coupled. Surface chemical compensation is known to control the magnitude and sign of ferroelectric polarization, yet the competing instability toward domain formation has usually been treated separately. Here we develop a static theory in which polarization, electrochemical surface charge, and finite-wave-vector domain formation are analyzed within a single thermodynamic framework for uniaxial polarization orientation. The central quantity is the differential chemical capacitance, which determines how strongly the surface charge can respond to a spatial modulation of polarization and therefore differs fundamentally from the equilibrium screening charge. We derive the homogeneous equation of state, the finite-wave-vector stability kernel, analytical domain-onset wavelengths and thickness scalings, and weakly nonlinear stripe and checkerboard solutions for both second- and first-order ferroelectrics. For a first-order transition, a finite-amplitude stripe state can become thermodynamically favorable before the homogeneous linear spinodal when the effective quartic coefficient is negative; this pre-spinodal window closes as the biased background polarization increases. Dense numerical phase maps confirm the analytical structure and show how chemical potential and film thickness reorganize weakly polar, monodomain, and polydomain states. Numerical analysis for BaTiO3 realization illustrates the corresponding temperature, oxygen-pressure, and thickness scales and identifies experimentally testable regimes in which chemical screening stabilizes the homogeneous state against the columnar 180{\deg} instability considered here or domain formation becomes the preferred route for depolarization-energy reduction.
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Materials Science

Exchange-Driven Chiral Magnons and Weyl States in Room-Temperature Metallic XCoB$_2$ (X= Ta, Zr and Hf) Altermagnets

Arafat Rahman, Tareq Mahmud and Alamgir Kabir

Metallic altermagnets remain rare, particularly in low-symmetry three-dimensional crystals where spin-split electronic bands and chiral magnon excitations can coexist. We report a family of metallic $d_{yz}$-wave altermagnets in the orthorhombic ternary borides XCoB$_2$ (X = Ta, Zr, Hf), which crystallize in the centrosymmetric $Pnma$ structure with G-type collinear magnetic order. Symmetry analysis within the magnetic space group $Pnm'a'$ (BNS No.~62.447) predicts a nonrelativistic spin splitting proportional to $k_yk_z$, with symmetry-enforced degeneracy on the $k_y$ and $k_z$ nodal planes, consistent with first-principles calculations. On the $k_x=0$ plane, the momentum-averaged spin splitting reaches 88.4, 52.3, and 70.6~meV at the Fermi level in TaCoB$_2$, ZrCoB$_2$, and HfCoB$_2$, respectively, with maxima exceeding 200~meV in all three compounds. Exchange analysis shows that the altermagnetic magnon splitting originates from symmetry-inequivalent sixth-neighbour inter-sublattice interactions. The chirality splitting reaches 1.51, 2.03, and 3.10 meV below 50 meV in TaCoB$_2$, ZrCoB$_2$, and HfCoB$_2$, respectively, making it accessible to inelastic neutron scattering. Monte Carlo simulations yield N'eel temperatures of $67\pm1.1$, $330\pm5.7$, and $307\pm5.0$~K, placing ZrCoB$_2$ and HfCoB$*2$ above room temperature. With spin-orbit coupling included, all three compounds host symmetry-protected Weyl points near the Fermi level, Fermi-arc surface states and sizable intrinsic anomalous Hall conductivities $\sigma*{zx}$ of $+342$, $-392$, and $-221$~S/cm at the Fermi level, reaching maximum magnitudes of $763$, $942$, and $924$~S/cm for TaCoB$_2$, ZrCoB$_2$, and HfCoB$_2$, respectively. $X$CoB$_2$ therefore provides a single compensated platform carrying both magnonic and electronic chirality, one in the spin waves and the other in the Berry curvature, without any stray field.
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Materials Science

Large spin splitting metallic altermagnets from machine-learned design rules

Ali Sufyan, Brahim Marfoua, J. Andreas Larsson et al. (+2 more)

Altermagnets combine compensated magnetic order with momentum-dependent spin splitting, providing spin-polarized electronic states without a net magnetization. Metallic $d$-wave altermagnets are particularly promising because they can support time-reversal-odd spin currents in linear response, yet experimentally validated bulk realizations remain scarce. Here, we use high-throughput density-functional-theory data to relate the magnitude of altermagnetic band splitting to compositional, structural, and DFT-derived magnetic descriptors. An interpretable gradient-boosted model identifies two candidate-prioritization criteria: compact unit cells and magnetic sublattices that sustain sizable local moments. Guided by these trends, we screen tetragonal $A_2XY$ Heusler compounds in space group $P4/mmm$. Among 307 structures, symmetry identifies 169 altermagnetic arrangements, of which 157 remain metallic altermagnets in DFT. Sixteen realize an altermagnetic collinear ground state, of which 15 are dynamically and mechanically stable and 10 also lie on or below the calculated thermodynamic hull. Six candidates exceed the CrSb splitting obtained under the same computational protocol, led by Co$_2$AlSc ($\Delta_\mathrm{max}=2.24$~eV) and Fe$_2$AlGe ($2.07$~eV). A Julliere-model estimate gives a tunneling magnetoresistance of up to $203\%$ at the Fermi level for Co$_2$AlSc. These results identify a chemically tunable family of metallic $d$-wave altermagnets and demonstrate how interpretable machine learning can guide targeted first-principles searches.
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All authors Ali Sufyan, Brahim Marfoua, J. Andreas Larsson, Rickard Armiento, Erik van Loon

Materials Science

Sodium Incorporation in CsPbBr$_{3-x}$I$_x$ Nanocrystal Electrodes: Lattice Contraction and the Suppression of Field-Driven Iodine Expulsion

Arun Kumar and Monojit Bag

Mixed-halide perovskite nanocrystal electrodes fail in supercapacitors through field-driven halide segregation. In undoped $\mathrm{CsPbBr_2I}$, this appears as a capacitance that climbs to 218% of its first-cycle value by cycle 1378 and then collapses to 39% by cycle 2500, with complete loss of the iodine signal from the cycled electrode. This work tests whether sodium incorporation suppresses that failure mode. Na-doped $\mathrm{CsPbBr_{3-x}I_x}$ ($x = 0, 1, 2$) nanocrystals were prepared by ligand-assisted reprecipitation at a Na/Pb precursor ratio of 1.25:1.00 and compared with undoped analogues in 0.1 M tetrabutylammonium tetrafluoroborate in anhydrous dichloromethane. Sodium contracts the pseudocubic lattice parameter of $\mathrm{CsPbBr_3}$ from $5.908 \pm 0.029$ to $5.851 \pm 0.019$ $\mathring{\mathrm{A}}$ after correction for specimen displacement. Specific capacitance at 0.3 A g$^{-1}$ rises for every composition, from 42 to 75, from 63 to 96, and from 56 to 84.5 F g$^{-1}$. Na-$\mathrm{CsPbBr_2I}$ gives the lowest charge-transfer resistance at 175 $\Omega$ and the highest ion diffusion coefficient at $1.6 \times 10^{-16}$ m$^2$ s$^{-1}$, and power-law exponents between 0.33 and 0.45 at all potentials examined show that charge storage is limited by ion transport through the pore network rather than by the interfacial process. In the sodium-containing (Na-$\mathrm{CsPbBr_2I}$) electrode, the capacitance rise reaches only 115% at cycle 600, no collapse follows, and 97% is retained at 2500 cycles, the excess above the first-cycle value being reduced by a factor of 7.9. Iodine is retained at unchanged binding energy, and the Br:I ratio measured by elemental mapping is 2.30 after cycling against 2.25 before.
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Materials Science

Towards a Metal-Organic Framework with Pore-Confined Electrons

Julia H. Baratta and Andrew S. Rosen

Electrides are an unconventional class of materials in which electrons are localized in crystallographic void spaces rather than solely around atomic nuclei, giving rise to appealing properties such as low work functions, strong electron-donating character, and even superconductivity. Here, we use ab initio methods to investigate metal-organic framework (MOF) electrides, a new class of materials that combines the interstitial electrons of electrides with the permanent porosity and chemical tunability of MOFs. These materials host pore-confined electrons: occupied electronic states localized in the pore space and with bands slightly below or crossing through the Fermi level. Using density functional theory calculations, we establish several design rules for stabilizing pore-confined electrons in MOFs via an anion-electron exchange process and identify candidate MOF electrides. As a proof-of-concept, we also demonstrate that the pore-confined electrons can directly facilitate chemical reactions, substantially lowering the activation barrier for H2 dissociation without requiring adsorption at a surface site. We envision that pore-confined electrons in nanoporous materials may enable a fundamentally new type of catalysis in which chemical reactions take place in the pore space, driven by electron-centered active sites.
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Materials Science

Unbiased first-principles construction of complete tensorial spin Hamiltonians

Haichang Lu, Boyang Deng, Hiroshi Katsumoto et al. (+3 more)

Magnetic ground states are commonly predicted using spin Hamiltonians whose interaction terms are selected a priori, potentially overlooking the microscopic interactions that govern complex magnetic order. Here, we introduce a general framework for the unbiased first-principles construction of symmetry-complete tensorial spin Hamiltonians and its automated implementation in AMATIS. The framework constructs the Hamiltonian directly from density-functional theory while rigorously enforcing quantum spin algebra and crystallographic symmetry. Applied to representative two-dimensional van der Waals magnets, the framework reproduces established magnetic interactions and uncovers hidden physics beyond conventional spin models, including chiral interactions that stabilize metastable skyrmions, higher-rank tensorial interactions that reconstruct the magnetic phase diagram and establish stabilizing competing multi-Q phases, and an emergent p-wave altermagnetic electronic structure. Our results demonstrate that unbiased tensorial Hamiltonian construction provides a predictive alternative to the conventional practice of manually selecting spin-model interactions, enabling first-principles discovery of unconventional magnetic phases.
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All authors Haichang Lu, Boyang Deng, Hiroshi Katsumoto, John Robertson, Weisheng Zhao, Stefan Blügel

Materials Science

Quantum interpretation of classical LiF simulations

Federico Brivio and Luca Salasnich

Recent studies have shown that classical LiF simulations can reproduce low-temperature experimental spectra when performed at a simulation temperature $T^*$ higher than the physical temperature $T$. We show that the characteristic scale of this rescaling follows naturally from quantum vibrational statistics. An effective temperature $T_{\rm eff}(T)$ is obtained by matching classical and quantum harmonic energies and is evaluated using an analytic acoustic-optical model and a first-principles LiF vibrational density of states $D(\varepsilon)$. The resulting temperature reproduces the low-temperature scale of the reported spectral temperature and approaches the physical temperature in the classical regime. Our results identify zero-point motion and Planck-Bose-Einstein statistics as the origin of the reported temperature scale.
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Materials Science

A Direct Algebraic Approach to Normal Ordering of Exponential Bosonic Operators with Applications to Two-Dimensional Excitonic Form Factors

Duy-Anh P. Nguyen, Ngoc-Tram D. Hoang, Dang-Khoa D. Le et al. (+1 more)

We develop a systematic algebraic approach, based on the Wei–Norman factorization method, to the normal ordering of exponential bosonic operators and apply it to derive analytical excitonic form factors in two-dimensional semiconducting materials. By introducing an auxiliary parameter, the normal-ordering problem is reduced to a system of ordinary differential equations determined by the commutation relations of the underlying closed Lie algebra. The approach is first illustrated for exponential operators associated with the Heisenberg–Weyl and $su(1,1)$ algebras, and is then extended to two-mode bosonic operators involving $su(2)$ and a six-generator closed algebra that contains two coupled $su(1,1)$ subalgebras. For the excitonic application, the Levi–Civita transformation maps the two-dimensional exciton problem onto an oscillator representation, providing a natural formulation in terms of bosonic creation and annihilation operators. Combined with the Laplace and Fourier representations of the Rytova–Keldysh potential, this formulation reduces the interaction matrix elements to the evaluation of exponential bosonic form factors. The isotropic problem is governed by a three-generator $su(1,1)$ algebra, whereas the anisotropic case requires the full six-generator algebra together with an additional $su(2)$ factorization. Explicit analytical expressions for both form factors, $\langle e^{-rt}\rangle$ and $\langle e^{i\mathbf q\cdot\mathbf r}\rangle$, are obtained, providing useful building blocks for matrix-element calculations in two-dimensional excitonic systems and potentially in other quantum problems involving exponential bosonic operators.
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All authors Duy-Anh P. Nguyen, Ngoc-Tram D. Hoang, Dang-Khoa D. Le, Van-Hoang Le

Materials Science

B-type Quadratic Planar Hall Effect as a Probe of Altermagnetic Order

Yiwei Zhao, Junwei Liu, Jian Zhou et al. (+1 more)

Conventional transport and optical responses, such as the Hall effect, can only distinguish material phases with substantially different symmetries. However, many quantum materials, such as candidate altermagnetic materials, host competing phases with similar structures, making it difficult to differentiate them using conventional transport or optical measurements. Here, guided by symmetry principles, we introduce a B-type quadratic planar Hall effect (B2-PHE) as a sensitive probe of magnetic structures. B2-PHE features a planar Hall current that scales quadratically with the applied magnetic field. This response originates from the interplay among external magnetic fields, intrinsic magnetic order, and quantum geometric properties of the electronic bands. We investigate B2-PHE in two altermagnetic candidates, KV2Se2O and RuO2, whose ground-state magnetic orders are under intense debate. Remarkably, B2-PHE emerges in their altermagnetic phases but is symmetry-forbidden in their antiferromagnetic (nonmagnetic) phases. We also show that B2-PHE should be detectable under a moderate magnetic field on the order of 1 Tesla. These findings establish B2-PHE as an experimentally convenient and potentially unambiguous probe of altermagnetic order, which is otherwise difficult to realize.
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All authors Yiwei Zhao, Junwei Liu, Jian Zhou, Haowei Xu

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

Heating of black-Si by microwaves at 2.45 GHz: effect of nano-needle orientation

Massimiliano Zamengo, Haoran Mu, Hsin-Hui Huang et al. (+4 more)

Silicon, which is highly reflective and has negligible absorption at the microwave 2.45 GHz range, can be heated when it is turned into black-Si with a surface texture of nano-needles made by SF6/O2 plasma etching. Microwave heating of flat Si and of black-Si with vertical and with tilted (oriented) nano-needles was compared under identical conditions in a cylindrical TM010 resonator. Samples were placed horizontally on a 150-micrometer-thick cover glass, which standardized their height and position inside the cavity and allowed a common calibration of the radiation thermometer against a K-type thermocouple. Under a stepwise protocol of only 2-3-4 W of microwave power (60 s per step), black-Si with vertical needles reached ~ 260 C, systematically exceeding flat Si (~ 190 C), while black-Si with oriented needles showed a delayed but abrupt onset of heating at 3 W. In situ monitoring of the cavity resonance revealed a 2-3 MHz downshift of the resonance frequency f for all samples, with the drift consistently appearing once the sample temperature exceeded ~ 120 - 150 C, consistent with thermally activated carrier generation in Si. At a given temperature, each sample loads the cavity at a different f and quality factor Q, indicating an orientation-dependent effective permittivity of the nano-needle array, in line with the strong form birefringence of tilted black-Si. Application potential and challenges in the quantitative temperature and permittivity determination are discussed.
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All authors Massimiliano Zamengo, Haoran Mu, Hsin-Hui Huang, Tomas Katkus, Darius Gailevičius, Saulius Juodkazis, Junko Morikawa

Materials Science

Probing (sub)nanoscale ferrons in an electron microscope

Mahir Manna, Fei Yang, Shayantan Chaudhuri et al. (+13 more)

Ferrons are collective excitations of polarization fluctuations that can enable terahertz communications and quantum transduction due to long propagation lengths. Although ferrons have been experimentally demonstrated in van der Waals ferroelectrics and relaxor ferroelectrics, there is no direct (sub)nanoscale experimental evidence of ferrons in three-dimensional ferroelectrics. Here, we detect two types of ferrons, Higgs and pseudo-Goldstone, at the (sub)nanoscale in lead titanate by measuring vibrational signals due to polarization fluctuations. By harnessing momentum transfer in electron energy loss spectroscopy (EELS), we directly distinguish between soft-phonons and ferrons. We observe that the Higgs mode originates from the soft optical phonon parallel to the polar axis, whereas the pseudo-Goldstone mode originates from the soft optical phonon perpendicular to the polarization axis. Together with Landau theory, Raman spectroscopy measurements, and EELS, we observe that Higgs group velocities, in the bulk limit, are eight times greater than those of out-of-plane soft phonons and the pseudo-Goldstone ferrons have group velocities six times greater than in-plane soft phonons due to long-range dipole interactions. We further show that the domain size confinement effects lead to doubling of the respective bulk ferron group velocities, reaching up to approximately 15 km per second (almost 15 times higher than the out-of-plane soft phonon modes). Overall, this study opens a pathway to the detection of ferrons in three-dimensional ferroelectrics with domain engineering as a promising avenue for terahertz communication and transduction.
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All authors Mahir Manna, Fei Yang, Shayantan Chaudhuri, Sourav Shenoy, Guo-Dong Zhao, Mohit Tanwani, Surya Prakash Reddy, Patrick J. Hays, Sriram Sankar, Cauê de Souza Coutinho Nogueira, Srilekshmi Muraleedharan, Xin Xu, Sujit Das, Katherine Inzani, Long-Qing Chen, Sandhya Susarla

Materials Science

Physics-aware global Rietveld refinement for high-energy X-ray diffraction microscopy with application to reconstructing intragranular orientation and strain fields

Carter K. Cocke, Eitan Camacho, Sara F. Gorske et al. (+2 more)

High-energy X-ray diffraction microscopy (HEDM) has emerged as a critical technique for studying the microstructure and, increasingly, strain fields in solids. However, current algorithmic or experimental methods to obtain intragranular fields are time-intensive, provide limited spatial resolution, or yield stress and strain fields that do not satisfy the universal laws of deformation (compatibility and equilibrium). In the context of standard HEDM, a novel physics-aware approach is presented in which the physics of deformation is included in the forward diffraction simulation to ensure that the reconstructed fields are physically meaningful. The entire simulated and experimental diffractograms are compared with a differentiable optimal transport–type objective, and a Rietveld refinement is carried out globally on the internal fields and grain topology using gradient-based optimization. The method is developed, verified with synthetic data, and demonstrated experimentally using near-field HEDM data from aluminum oxynitride (a brittle ceramic), with a reference implementation released as PARA-X. The reconstructions show remarkable improvement over existing methods (improved completeness and loss), and the high-fidelity, high-resolution recovery paves the way for using HEDM to study fine-scale deformation mechanics over large polycrystalline volumes.
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All authors Carter K. Cocke, Eitan Camacho, Sara F. Gorske, Katherine T. Faber, Kaushik Bhattacharya

Friday 11 September

Materials Science

Reducing the Gate-Induced Drain-Leakage Current of Carbon-Nanotube Transistors by Subliming Dispersants with Back-End-of-Line Compatible Temperature

Takumi Inaba, Yuichi Kato, Yoko Iizumi et al. (+4 more)

Carbon nanotube field-effect transistors (CNTFETs) are promising for monolithic 3D integration with silicon CMOS circuits in back-end-of-line (BEOL) processes. Further reduction in off-state leakage is essential for practical applications. In this study, we develop a low-temperature cleaning process for CNT-deposited wafers using a sublimable CNT dispersant. The process is carried out below 250 {\deg}C, making it BEOL-compatible, and does not deteriorate CNT morphology or lattice structure, as confirmed by atomic force microscopy and Raman spectroscopy. As a result, gate-induced drain leakage current originating from residual dispersants is reduced by approximately one order of magnitude. In addition, improvements in on-current, subthreshold slope, and threshold voltage variability are observed after the cleaning process. This study demonstrates a material-enabled approach to improve the transfer characteristics of CNTFETs and provides a practical route toward low-power CNT electronics.
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All authors Takumi Inaba, Yuichi Kato, Yoko Iizumi, Yasuhiko Fujita, Kazufumi Kobashi, Takahiro Morimoto, Toshiya Okazaki

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

Disorder-driven transport in ZrN thin films grown by ion-beam-assisted sputtering

Maximo DiPreta, Samuel Jiang, Serhii Kruhlov et al. (+3 more)

We investigate the structural and electronic transport properties of zirconium nitride (ZrN) thin films grown by dc ion-beam assisted sputtering (IBAS) as a function of nitrogen partial pressure, sputtering power and deposition temperature. Variation of growth conditions enables controlled tuning from disordered metallic and superconducting behavior to insulating transport. Increasing nitrogen flow drives an increase in sheet resistance, suppression of superconducting transition temperature, and non-metallic conduction. XRD shows no measurable change in long range crystallinity or order. In the insulating regime, low-temperature transport is well described by 3D Mott variable-range hopping (VRH), with the characteristic temperature $T_0$ increasing monotonically with sheet resistance over four orders of magnitude. Despite this strong correlation between $T_0$ and disorder, $T_c$ exhibits no systematic dependence on $T_0$, indicating a decoupling between localization physics and the superconducting energy scale. Magnetotransport measurements are not well described by the standard BCS model nor the dirty type-II Werthamer-Helfand-Hohenberg model. The phase boundary is instead captured by a free-exponent power law, $\mu_0 H_{c2}(T) = \mu_0 H_{c2}(0)[1 - (T/T_c)^{n}]$ with $n \approx 3.47$, and extrapolates to $\mu_0 H_{c2}(0) \approx 6.4$ T. The films have an extracted coherence length of 7 nm. These results establish IBAS-grown ZrN as a broadly tunable platform for investigating disorder-driven transport and the crossover between metallic conduction, electronic localization, and superconductivity.
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All authors Maximo DiPreta, Samuel Jiang, Serhii Kruhlov, Yi Li, Valentine Novosad, Tomas Polakovic

Materials Science

Local Response Theory of Electrified Interfaces from Screened Effective Charges

Nicolas G. Hörmann, Nicolas Bergmann and Karsten Reuter

First-principles, electronic-structure simulations provide direct access to ground-state, global system properties. In the context of computational electrochemistry these are, e.g., bias-dependent energies, free energies, work functions, and capacitances. However, a comparably systematic local description of how these quantities respond to biasing via interfacial charging is still missing. Here, we introduce the screened electrochemical Born effective charge (SEBEC), a mixed total-energy derivative that measures the force response of an atomic degree of freedom to interfacial charging under electrochemical boundary conditions. SEBECs play the role for electrochemistry that Born effective charges play in the modern theory of polarization: they provide an unambiguous decomposition of global response and generate the same formal structures for structural relaxation, capacitance, and electrochemical Stark tuning that are familiar from solid-state response theory. The broader implication is a local response framework that brings electrochemical interfaces closer to the conceptual rigor long established for insulating solids.
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Materials Science

Slow Thermalization and Long-Lived Coherence across Acoustic Phonon Branches in BAs

Zeyu Xiang, Ying Peng, Ange Benise Niyikiza et al. (+11 more)

The exceptionally high thermal conductivity of cubic boron arsenide (BAs) arises from suppressed three-phonon scattering associated with its large acoustic–optical gap. In this regime, four-phonon processes become non-negligible, creating an unusual scattering hierarchy with unexplored consequences for nonequilibrium phonon dynamics. Here, time-resolved x-ray diffuse scattering reveals exceptionally slow, branch-dependent acoustic phonon thermalization and long-lived coherence. Exploiting branch sensitivity in one-phonon diffuse scattering, we resolve transverse acoustic (TA) and longitudinal acoustic (LA) thermalization times of 29.2 and 13.9~ps, respectively; even the LA timescale is at least three times that in common semiconductors. Phonon dispersion calculations assign coherent oscillations at 0.19 and 0.27~THz to the TA and LA modes, respectively; both persist with little decay over 50~ps, with comparable coherence found only in diamond. These findings provide a direct dynamical manifestation of the weak phonon scattering underlying the exceptional thermal transport of BAs.
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All authors Zeyu Xiang, Ying Peng, Ange Benise Niyikiza, Fanghao Zhang, Haoyuan Li, Takahiro Sato, Thomas Linker, Yanwen Sun, Meredith Henstridge, Vincent Esposito, James F. Cotter, Diling Zhu, Zhifeng Ren, Bolin Liao

Materials Science

Non-reactive sintering enhances density and ionic conductivity of NASICON solid electrolytes

Andrea Cornelio, Björn Mieller, Johannes Baller et al. (+6 more)

NASICON materials are promising solid electrolytes for room-temperature sodium solid-state batteries and are typically synthesized via solid-state reaction. While sintering has been extensively studied, the effect of calcination on electrolyte properties remains poorly understood. In this work, the temperatures at which the NASICON phase forms in Na3Zr2Si2PO12 and Na3.4Zr2Si2.4P0.6O12 are identified. Calcination temperature is then varied between 900 {\deg}C and 1200 {\deg}C to obtain powders with different degrees of reaction prior to sintering. Under identical sintering conditions, higher NASICON phase content in the calcined powder is shown to yield denser electrolytes. Non-reactive sintering also improves grain boundary conductivity, increasing it by 130% for Na3.4Zr2Si2.4P0.6O12 and raising total conductivity from 1.60 to 2.95 mS/cm for powders calcined at 900 {\deg}C and 1200 {\deg}C, respectively. Finally, it is shown that phosphorus loss during processing compromises cycling stability against Na metal electrodes, and that adding off-stoichiometric phosphorus resolves this issue, while reaching a critical current density of 5.0 mA/cm^2 and a room-temperature conductivity of 3.82 mS/cm with over 400 hours of stable cycling. Overall, these findings directly relate synthesis and processing conditions to the final material properties and electrochemical performance of NASICON solid electrolytes.
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All authors Andrea Cornelio, Björn Mieller, Johannes Baller, Andrea Fantin, Janina Roik, Jessica Kindt, Jonas Krug von Nidda, Tim-Patrick Fellinger, Gustav Graeber

Materials Science · Cross-listed from physics.optics

Transverse-Anderson localization of light in disordered silicon pores

S. Erfanifam, C. Yanik and M. Erfanifam

Transverse light localization of Anderson type through disorders has made intriguing fundamental topics. Toward this, we found that in the disordered porous Si (PSi) a nearly "zero reflection" (from 450 to 900 nm) can be observed. The localization length versus disorder parameter is experimentally visualized and calculated based on a self consistent theory and solution of stochastic Helmholtz equation for electric fields traveling in a transverse disordered media with the results determined to be in a reasonable agreement with experiments. Based on these calculations for different pore diameters in a constant order parameter, diffusion length can vary from 260 nm to 2.4\mu m, accounting as controllability of such structure for further applications in photonic devices. Reflection from ordered PSi structure are evaluated that shows no similar responses to those seen in disordered PSi.
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Materials Science

Symmetry- and Property-Aware Crystal Generation with Reinforcement Learning for Inverse Materials Design

Ting-Wei Hsu, Arun Bansil and Qimin Yan

The inverse design of crystalline materials ultimately seeks structures with desired physical properties. However, for many functional responses, a favorable numerical value is meaningful only when supported by the symmetry of the underlying crystal. Without the appropriate crystallographic constraints, an apparent response may be ill defined, accidental, or not symmetry protected. Here we introduce SPARC, a symmetry- and property-aware reinforcement learning framework that optimizes physical objectives while preserving the structural conditions required for their realization. We demonstrate SPARC on two complementary tasks. The first targets strong uniaxial dielectric anisotropy, a tensorial response that is well defined only within appropriate crystal classes. The second maximizes the spectroscopic limited maximum efficiency, a scalar device-level objective without a prescribed symmetry class, allowing the framework to identify favorable crystallographic motifs. These results show that symmetry is not merely an additional design constraint, but a physical foundation for generating candidates with meaningful, robust, and realizable functional properties.
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Materials Science

Particle Inertia-Driven Pore Formation over Material Property Effects in Laser Powder-blown Directed Energy Deposition

Dong Hee Kang, Samantha Webster, Sampson Canacoo et al. (+3 more)

Laser Powder-blown Directed Energy Deposition (LP-DED) offers flexibility for process and materials and high productivity (~5 kg/h), but process-induced pores often compromise mechanical properties. This study utilizes in-situ X-ray synchrotron imaging to compare pore formation mechanisms in Ti-6Al-4V (Ti64) and stainless steel 316L (SS316L), focusing on the interplay between particle dynamics and thermophysical properties. Four distinct pore formation mechanisms were identified, with most large pores originating from the closure of cavities formed behind incident particles impinging on the melt pool. High Weber number (We >> 1) governs this behavior, indicating that particle inertia, rather than thermophysical property differences, is the primary driver of large pore formation. The study demonstrates that increased energy density leads to larger melt pool volumes, facilitating deeper particle penetration. This greater penetration depth directly correlates with increased pore diameters. While thermophysical properties secondarily influence pore-formation frequency and cavity symmetry, particle inertia remains the dominant factor. These findings provide a physically grounded basis for understanding and controlling porosity in powder-blown DED processes.
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All authors Dong Hee Kang, Samantha Webster, Sampson Canacoo, Samuel J. Clark, Kamel Fezzaa, Jihoon Jeong

Materials Science

Cracking the case: fluctuations enhance ductility in refractory alloys

Manura Liyanage, Julia Chmielewska, Tijmen Vermeij et al. (+4 more)

Refractory body-centered cubic (BCC) alloys are attractive candidates for structural applications at extreme temperatures, yet combining room-temperature ductility with high-temperature strength remains the unsolved challenge. Ductility in crystals requires that dislocations emit from a sharp crack tip before brittle cleavage, but continuum theories that treat disordered alloys as chemically homogeneous incorrectly predict brittleness for many experimentally ductile alloys. Here we show that atomic-scale stress fluctuations in disordered alloys create an additional local stress intensity at the crack tip, enabling dislocation loop nucleation below the cleavage threshold. Accounting for these fluctuations yields a local ductility criterion where alloys deemed brittle by conventional fracture mechanics can be intrinsically ductile. Atomistic simulations with machine-learned interatomic potentials and an analytic fracture mechanics model correctly predict composition-driven brittle-to-ductile transitions in binary and ternary Mo-Nb-Ti alloys, in Nb-Ti alloys at 4 K, and in several commercial BCC alloys at room temperature. Guided by this criterion, we predict, fabricate, and test the Hf$_{15}$Mo$_{15}$Nb$_{32}$Ti$_{38}$ alloy, confirming its room-temperature ductility. This fluctuation-driven mechanism provides a quantitative basis for designing ductile multicomponent BCC alloys.
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All authors Manura Liyanage, Julia Chmielewska, Tijmen Vermeij, Johann Michler, Christian Leinenbach, W. A. Curtin, Anirudh Raju Natarajan

Materials Science

Precessional modes of phonon angular momentum

Daniel A. Bustamante Lopez and Dominik M. Juraschek

Magnons are collective precessional excitations of electron spins and are ubiquitous in emerging information technologies. Here, we show that the crystal lattice can support an analogous precessional mode of phonon angular momentum. Superposition of a circularly polarized phonon and a linearly polarized phonon normal to the circular-motion plane generates a transverse angular-momentum component that rotates at their difference frequency and decays on a timescale set by the participating phonon linewidths, defining a mode with its own resonance and lifetime. Coupling between spin and phonon angular momentum hybridizes this precessional mode with a magnon near resonance. Our results establish phonon angular momentum precessional modes as lattice analogues of magnons and identify their spectroscopic and time-domain signatures.
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Materials Science · Cross-listed from cond-mat.supr-con

Topological superconductivity in an altermagnet-superconductor heterostructure

Michael Liudeng, Hrishikesh Patel, Marcel Franz et al. (+1 more)

Fully gapped spin-triplet superconductors offer a natural setting for topological edge transport and Majorana excitations. Here we propose a heterostructure that interfaces altermagnetic monolayer V$_2$Se$_2$O with a conventional $s$-wave superconductor. Starting from an ab-initio description of V$_2$Se$_2$O, we construct a low-energy model of its spin-split Fermi surface and study the superconducting instability of the coupled stack. We find that the momentum-dependent exchange splitting of the altermagnet strongly favors equal-spin pairing and converts the proximity-induced order into a fully gapped $p$-wave state. Over a broad range of interface parameters, the resulting Bogoliubov-de Gennes bands carry a nonzero Chern number, and slab spectra exhibit chiral Majorana edge modes traversing the bulk gap. We further quantify the inverse proximity effect and show how the induced gap evolves across a finite multilayer stack. These results establish a route to topological triplet superconductivity by interfacing a conventional superconductor with an experimentally available altermagnetic semiconductor, and provide practical guidance for interface fabrication and experimental detection.
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All authors Michael Liudeng, Hrishikesh Patel, Marcel Franz, Niclas Heinsdorf

Materials Science

Visualizing impurity-driven scattering phase textures in EuCd2As2

Raquel Sánchez-Barquilla, Rafael Pineda Medina, Pablo García Talavera et al. (+11 more)

Understanding how disorder modifies electronic states in magnetic semiconductors is important for controlling spin-dependent transport and topological responses. Here we use scanning tunneling microscopy to visualize scattering phase textures in EuCd2As2. By isolating a single surface wavevector we reconstruct spatial phase maps of the local density of states and identify phase dislocations characterized by 2pi winding around impurity sites. These phase singularities emerge systematically within charge puddles generated by Eu interstitials and their positions evolve with bias voltage. We show that their spatial structure is consistent with interference between multiple scattering channels, including contributions from spin-orbit coupling. We provide a model which reproduces phase dislocations and relates the decay of the phase gradient to the relative strength of spin-orbit and scalar scattering. Our results establish a route to access the phase of electronic scattering in real space and study the role of local disorder and spin-orbit interactions in shaping electronic states in quantum materials.
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All authors Raquel Sánchez-Barquilla, Rafael Pineda Medina, Pablo García Talavera, Adrian Valadkhani, Edwin Herrera, Brinda Kuthanazhi, Lin-Lin Wang, Sergey L. Bud'ko, Paul C. Canfield, Roser Valentí, Isabel Guillamón, William J. Herrera, Alfredo Levy Yeyati, Hermann Suderow

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

Topological classification through knotted graphs: Fermi surface dispersions and Lifshitz transitions

Hakan Akgün, Xianquan Yan and Ching Hua Lee

Knot theory has provided a rich topological taxonomy for band structures, but its reach is fundamentally limited: knot invariants classify only 1D nodal lines at gap closure, and cannot encode the full dispersion or rich Fermi surface structure of realistic materials. Here we show that knotted graphs (knots that admit graph-like intersections in 3D space) - which have so far been elusive in condensed matter literature - provide a unified topological language for classifying the entire band dispersion, and even the eigenstate topology in some contexts. We propose a new framework beyond the existing Yamada polynomials that can topologically characterize the intricacies of realistic Fermi surfaces completely, crucially including how their multiple disconnected pieces are nested. This yields the Yamada set, a boundary-resolved extension which organizes the full topological evolution across energy into a Yamada sequence: a compact dispersion-level fingerprint directly tied to experimental signatures of Lifshitz transitions. Our framework is demonstrated with DFT-based band structures of real materials. Beyond dispersion-level classifications, this framework can be extended to non-Hermitian exceptional surfaces, where Berry-curvature flux further equips the knotted-graph skeleton with a directed Abelian edge flow that also captures the eigenstate topology.
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Materials Science · Cross-listed from physics.chem-ph

Can Autonomous LLM Agents Execute Multireference Quantum Chemistry Calculations?

Victor Chang Lee and James M. Rondinelli

Multireference electronic-structure calculations remain difficult to automate because critical workflow decisions, including active-space selection, state averaging, convergence recovery, and state identification, traditionally rely on expert judgment. Here, we investigate whether an autonomous large language model (LLM) agent can perform these tasks without human intervention. The agent selects active spaces using literature-grounded analogies or explicitly documented chemical reasoning, generates and submits ORCA calculations, analyzes outputs, and records all decisions in an auditable reasoning log. Benchmarking against 558 vertical transition energies (VTEs) from QUESTDB shows that an unguided baseline agent achieves 24.9% coverage with a mean absolute error (MAE) of 0.373 eV. Introducing a structured decision ladder increases coverage to 44.1% while reducing the MAE to 0.339 eV. The largest gains are observed for double and Rydberg excitations, demonstrating that expert-informed procedural guidance substantially improves active-space construction and state identification. When provided with complete workflow information, the agent successfully reproduces published QUEST calculations with an MAE of only 23 meV, resolving 75% of target configurations within seven attempts. These results demonstrate that contemporary LLM agents can autonomously execute and reproduce complex multireference quantum-chemical workflows, while highlighting the importance of structured reasoning frameworks for achieving reliable high-throughput and high-fidelity electronic-structure calculations.
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Materials Science

RS-CIDER: A non-local machine learning model for approximating screened hybrid functionals

Zhuotao Jin, Mohamed S. Abdallah, Boris Kozinsky et al. (+1 more)

Screened hybrid functionals such as HSE06 improve the description of band gaps, charge localization, and redox energetics relative to semilocal approximations, but their explicit Hartree-Fock exchange term is computationally costly for large, periodic systems, especially in plane-wave basis set calculations. Here we present RS-CIDER, a machine-learned non-local exchange functional that approximates the short-range Hartree-Fock exchange term in HSE06 by explicitly fitting both ground-state energies and single-particle energy levels. RS-CIDER combines scale-invariant semilocal and non-local density descriptors and can be evaluated self-consistently without explicitly applying the short-range Hartree-Fock exchange operator. RS-CIDER shows close agreement with HSE06 for molecular reaction energies and solid-state band gaps. Further tests across distinct materials show agreement between RS-CIDER and HSE06 for local magnetism, Cu-O phase competition, polaron localization, and neutral-defect energetics. For an Fe olivine, chemistry-specific fine-tuning recovers the HSE06 Li intercalation voltage. A timing benchmark shows that RS-CIDER reduces the measured per-SCF-step wall time by more than an order of magnitude relative to HSE06. Together, these molecular and solid-state results establish RS-CIDER as an efficient self-consistent machine-learned surrogate for HSE06.
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All authors Zhuotao Jin, Mohamed S. Abdallah, Boris Kozinsky, Kyle Bystrom