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Seung-Cheol Lee

Publications and source records attributed to Seung-Cheol Lee.

At least 19 recordsLinked to original sources

Testing the spin-bath view of self-attention: A Hamiltonian analysis of GPT-2 Transformer

The recently proposed physics-based framework by Huo and Johnson~\cite{huo2024capturing} models the attention mechanism of Large Language Models (LLMs) as an interacting two-body spin system, offering a first-principles explanation for phenomena like repetition and bias. Building on this hypothesis, we extract the complete Query-Key weight matrices from a production-grade GPT-2 model and derive the corresponding effective Hamiltonian for every attention head. From these Hamiltonians, we obtain analytic phase boundaries and logit gap criteria that predict which token should dominate the next-token distribution for a given context. A systematic evaluation on 144 heads across 20 factual-recall prompts reveals a strong negative correlation between the theoretical logit gaps and the model's empirical token rankings ($r\approx-0.70$, $p<10^{-3}$).Targeted ablations further show that suppressing the heads most aligned with the spin-bath predictions induces the anticipated shifts in output probabilities, confirming a causal link rather than a coincidental association. Taken together, our findings provide the first strong empirical evidence for the spin-bath analogy in a production-grade model. In this work, we utilize the context-field lens, which provides physics-grounded interpretability and motivates the development of novel generative models bridging theoretical condensed matter physics and artificial intelligence.

cond-mat.mtrl-sci

Local Symmetry Breaking in Skyrmion-Hosting Centrosymmetric Hexagonal Compounds

Dzyaloshinskii-Moriya interaction (DMI) plays a crucial role in stabilizing the exotic topologically stable skyrmion spin textures in the noncentrosymmetric crystals. The recent discovery of biskyrmions and skyrmions in the globally centrosymmetric crystals has raised debate about the role of the DMI in causing the spin textures, since DMI vanishes in such crystal structures. Theoretical studies, on the other hand, suggest non-vanishing DMI even if there is local inversion symmetry breaking in an otherwise globally centrosymmetric crystal structure. Motivated by such theoretical predictions, we present here the results of a systematic crystal structure study of two skyrmion-hosting Ni2In-type centrosymmetric hexagonal compounds, MnNiGa and MnPtGa, using the atomic pair distribution function (PDF) technique. Our result provides information about structural correlations in the short-range (SR), medium-range (MR) and long-range (LR) regimes simultaneously. The analysis of the experimental PDFs, obtained from high flux, high energy, and high Q synchrotron x-ray powder diffraction patterns, reveals that the local SR structure of both MnNiGa and MnPtGa compounds corresponds to the noncentrosymmetric trigonal space group P3m1, while the structure in the MR+LR regimes remains hexagonal in the centrosymmetric P63/mmc space group. These findings are also supported by theoretical DFT calculations. Our results, in conjunction with the previous theoretical predictions, provide a rationale for the genesis of skyrmions in centrosymmetric materials in terms of non-vanishing DMI due to local inversion symmetry breaking. We believe that our findings would encourage a systematic search of skyrmionic textures and other topological phenomena in a vast family of centrosymmetric materials.

cond-mat.mtrl-sci

Enhancement of spin Hall angle by an order of magnitude via Cu intercalation in MoS$_2$/CoFeB heterostructures

Transition metal dichalcogenides (TMDs) are a novel class of quantum materials with significant potential in spintronics, optoelectronics, valleytronics, and opto-valleytronics. TMDs exhibit strong spin-orbit coupling, enabling efficient spin-charge interconversion, which makes them ideal candidates for spin-orbit torque-driven spintronic devices. In this study, we investigated the spin-to-charge conversion through ferromagnetic resonance in MoS$_2$/Cu/CoFeB heterostructures with varying Cu spacer thicknesses. The conversion efficiency, quantified by the spin Hall angle, was enhanced by an order of magnitude due to Cu intercalation. Magneto-optic Kerr effect microscopy confirmed that Cu did not significantly modify the magnetic domains, indicating its effectiveness in decoupling MoS$_2$ from CoFeB. This decoupling preserves the spin-orbit coupling (SOC) of MoS$_2$ by mitigating the exchange interaction with CoFeB, as proximity to localized magnetization can alter the electronic structure and SOC. First-principles calculations revealed that Cu intercalation notably enhances the spin Berry curvature and spin Hall conductivity, contributing to the increased spin Hall angle. This study demonstrates that interface engineering of ferromagnet/TMD-based heterostructures can achieve higher spin-to-charge conversion efficiencies, paving the way for advancements in spintronic applications.

cond-mat.mtrl-sci

LLM Meets Diffusion: A Hybrid Framework for Crystal Material Generation

Recent advances in generative modeling have shown significant promise in designing novel periodic crystal structures. Existing approaches typically rely on either large language models (LLMs) or equivariant denoising models, each with complementary strengths: LLMs excel at handling discrete atomic types but often struggle with continuous features such as atomic positions and lattice parameters, while denoising models are effective at modeling continuous variables but encounter difficulties in generating accurate atomic compositions. To bridge this gap, we propose CrysLLMGen, a hybrid framework that integrates an LLM with a diffusion model to leverage their complementary strengths for crystal material generation. During sampling, CrysLLMGen first employs a fine-tuned LLM to produce an intermediate representation of atom types, atomic coordinates, and lattice structure. While retaining the predicted atom types, it passes the atomic coordinates and lattice structure to a pre-trained equivariant diffusion model for refinement. Our framework outperforms state-of-the-art generative models across several benchmark tasks and datasets. Specifically, CrysLLMGen not only achieves a balanced performance in terms of structural and compositional validity but also generates more stable and novel materials compared to LLM-based and denoisingbased models Furthermore, CrysLLMGen exhibits strong conditional generation capabilities, effectively producing materials that satisfy user-defined constraints. Code is available at https://github.com/kdmsit/crysllmgen

cs.LG

Role of Oxygen during Methane Oxidation on Pd$_1$/PdO$_1$@CeO$_2$ Surface: A Combined Density Functional Theory, Microkinetic, and Machine Learning Approach

This work explores the role of oxygen in industrial methane oxidation. Oxygen, a well-known oxidizing agent, drives CH$_4$ conversion to CO$_2$ and H$_2$O. We report how oxygen influences oxidation on single Pd and PdO clusters supported on CeO$_2$(111). Oxygen is introduced by (1) lattice O in PdO and (2) O$_2$ adsorption on an isolated Pd atom, forming PdO$_x$ clusters. Density-functional theory (DFT) mapped multiple reaction pathways on the Pd$_1$/PdO$_1$@CeO$_2$(111) surface; both Pd and PdO clusters were found to thermodynamically favour methane activation. The computed barrier for CH$_4$ activation is 0.63 eV on PdO$_1$@CeO$_2$(111). A single Pd atom markedly accelerates O$_2$ dissociation to PdO$_2$, and the presence of lattice oxygen lowers this barrier by 0.36 eV relative to an oxygen-deficient surface, enhancing catalytic efficiency. Reaction selectivity, coverage-dependent production rates, degree of rate control (DRC), and intrinsic turnover frequency (TOF) were quantified through steady-state microkinetic modelling. The simulations predict full conversion of CH$_4$ to CO$_2$ and H$_2$O above 600 K, whereas partial-oxidation intermediates dominate at lower temperature and high O coverage. Rate constants for all elementary steps were derived via the Sure Independence Screening and Sparsifying Operator (SISSO) symbolic-regression method, yielding a concise predictive expression based on charge, coordination number, and key Pd-O/C-H distances. These combined DFT-microkinetic-SISSO results clarify oxygen's mechanistic participation and provide practical guidelines for designing Pd/CeO$_2$ catalysts with improved activity toward methane oxidation, a reaction of pressing environmental and industrial importance.

cond-mat.mtrl-sci

Mechanistic Insights into Complete Methane Oxidation on Single-Atom Pd Supported by SSZ-13 Zeolite: A First-Principles Study

Complete catalytic oxidation of methane is an effective strategy for greenhouse gas mitigation and clean energy conversion; yet, ensuring both high catalytic activity and stability with palladium-based catalysts remains a challenge. In the present work, we employed a theoretical investigation of methane oxidation over single-atom Pd supported on SSZ-13 zeolite using density functional theory calculations, combined with climbing-image nudged elastic band calculations to determine activation barriers. A systematic assessment of various Al distributions and Pd placements was carried out to identify the most stable configurations for Pd incorporation within the zeolite framework.Further, two mechanistic routes for methane activation were evaluated: (i) direct dehydrogenation under dry conditions, and (ii) O$_2$-assisted oxidative dehydrogenation. Our results demonstrate that the direct (dry) pathway is energetically demanding and overall endothermic, whereas the O$_2$ assisted route facilitates the exothermic energy profile, particularly in the C-H bond cleavage. The formation of stable hydroxyl and CO/CO$_2$ intermediates were also studied. The results emphasize the role of oxygen-rich environments in enabling the complete methane oxidation with improved thermodynamic feasibility. Moreover, we propose an alternate low-energy pathway based on O-assisted and multi-site mechanisms that reduce the overall reaction enthalpy. These insights provide the design principles for highly active and moisture-resistant Pd-zeolite catalysts for sustainable methane utilization.

cond-mat.mtrl-sci

Quantum Simulations of Battery Electrolytes with VQE-qEOM and SQD: Active-Space Design, Dissociation, and Excited States of LiPF$_6$, NaPF$_6$, and FSI Salts

Accurate prediction of excited states in battery electrolytes is central to understanding photostability, oxidative stability, and degradation. We employ hybrid quantum-classical algorithms -- the Variational Quantum Eigensolver (VQE) for ground states combined with the quantum equation of motion (qEOM) for vertical singlet excitations -- to study LiPF$_6$, NaPF$_6$, LiFSI, and NaFSI. Compact active spaces were constructed from frontier orbitals, mapped to qubits, and reduced via symmetry tapering and commuting-group measurements to lower sampling cost. Within $\sim$10-qubit models, VQE-qEOM agrees closely with exact diagonalization of the same Hamiltonians, while sample-based quantum diagonalization (SQD) in larger active spaces recovers near-exact (subspace-FCI) energies. The spectra display clear anion and cation trends: PF$_6$ salts exhibit higher first-excitation energies (e.g., LiPF$_6$ $\approx$13.2 eV) and a compact three-state cluster at 12-13 eV, whereas FSI salts show substantially lower onsets ($\approx$8-9 eV) with a near-degenerate (S$_1$,S$_2$) followed by S$_3$ $\sim$1.3 eV higher. Substituting Li$^+$ with Na$^+$ narrows the gap by $\sim$0.4-0.8 eV within each anion family. Converting S$_1$ to wavelengths places the onsets in the deep-UV (LiPF$_6$ $\sim$94 nm; NaPF$_6$ $\sim$100 nm; LiFSI $\sim$141 nm; NaFSI $\sim$148 nm). All results pertain to isolated species or embedded clusters appropriate to the NISQ regime; solvent shifts can be incorporated a posteriori via classical $Δ$-solvation or static embedding. These results demonstrate that current quantum algorithms can deliver chemically meaningful excitation and binding trends for realistic electrolyte motifs and provide quantitative baselines to guide electrolyte screening and design.

cond-mat.mtrl-sci

Integrating Density Functional Theory with Deep Neural Networks for Accurate Voltage Prediction in Alkali-Metal-Ion Battery Materials

Accurate prediction of the voltage of battery materials plays a pivotal role in the advancement of energy storage technologies and the rational design of high-performance cathode materials. In this work, we present a deep neural network (DNN) model, built using PyTorch, to estimate the average voltage of cathode materials across Li-ion, Na-ion, and other alkali-metal-ion batteries. The model is trained on an extensive dataset from the Materials Project, incorporating a wide range of specific structural, physical, chemical, electronic, thermodynamic, and battery descriptors, ensuring a comprehensive representation of material properties. Our model exhibits strong predictive performance, as corroborated by first-principles density functional theory (DFT) calculations. The close alignment between the DNN predictions and the DFT outcomes highlights the robustness and accuracy of our machine learning framework to effectively select and identify viable battery materials. Using this validated model, we successfully proposed novel Na-ion battery compositions, with their predicted behavior confirmed by rigorous computational assessment. By seamlessly integrating data-driven prediction with first-principles validation, this study presents an effective framework that significantly accelerates the discovery and optimization of advanced battery materials, contributing to the development of more reliable and efficient energy storage technologies.

cond-mat.mtrl-sci

Origin of unexpected weak Gilbert damping in the LSMO/Pt bilayer system

This study presents a first-principles and semiclassical analysis of the puzzling observation that a La$_{0.7}$Sr$_{0.3}$MnO$_3$ (LSMO) thin film exhibits larger Gilbert damping than an LSMO/Pt bilayer, contrary to conventional spin-pumping expectations. Density functional theory with Wannier interpolation yields an intrinsic damping of $α_{\mathrm{int}}^{\mathrm{LSMO}}\!\approx\!1.4\times10^{-3}$, supporting an extrinsic origin of the high experimental value. Guided by the self-induced inverse spin Hall effect (ISHE) demonstrated in LSMO [Gupta et al., Phys.Rev. B 109, 014437 (2024)], we argue that the large spin Hall angle $|θ_{\mathrm{SH}}|\simeq 0.093$ and low longitudinal conductivity of LSMO enable an efficient conversion of spin current to charge current boosting the effective damping. In the LSMO/Pt heterostructure the Pt cap shunts the charge current, raising $σ_{xx}$ and reducing the interfacial $|θ_{\mathrm{SH}}|$ to~0.007. A Valet-Fert analysis for layer-resolved ab-initio spin accumulation gives the Pt spin-diffusion length and a non-negligible antidamping SOT coefficient, qualitatively accounting for the observed damping reduction under current bias. The seemingly anomalous damping hierarchy is thus reconciled without invoking additional interfacial mechanisms. The distinct length scales governing spin-pumping normalization, namely, the short absorption depth relevant to self-pumping in a single LSMO film versus the full magnetic thickness applicable to an LSMO/Pt bilayer, are crucial in this context. This observation suggests a practical design strategy: by simultaneously tuning the spin Hall-to-longitudinal conductivity ratio and the spin-diffusion length, one can engineer heterostructures with minimized magnetic losses for spin-orbitronics applications.

cond-mat.mtrl-sci

Tunable Thermal Expansion in Functionalized 2D Boron Nitride: A First-Principles Investigation

This study investigates the thermal expansion coefficient of two-dimensional (2D) functionalized boron nitride (f-BN) materials using first-principles density functional theory (DFT). Two-dimensional materials, particularly hexagonal boron nitride (h-BN), have attracted significant attention due to their exceptional mechanical, thermal, and electronic properties. However, the influence of functionalization on the thermal expansion behavior remains largely unexplored. In this work, DFT calculations are employed to analyze how different functionalized forms of h-BN impact the thermal expansion of BN sheets. Density functional perturbation theory (DFPT) and the quasiharmonic approximation (QAH) are utilized to determine the thermal expansion coefficient over a range of temperatures. The results reveal that functionalization induces notable modifications in the in-plane thermal expansion of BN, affecting material stability and suggesting potential applications in nanoelectronics and thermal management. This investigation provides critical insights into the tunability of the thermal properties of 2D BN, underscoring its suitability for next-generation flexible and high-performance devices.

cond-mat.mtrl-sci

Multi-site mixing and entropy stabilization of CsPbI$_{3}$ with potential application in photovoltaics

Metal halide perovskite solar cells have achieved dramatic improvements in their power conversion efficiency in the recent past. Since compositional engineering plays an important role in optimizing material properties, we investigate the effect of alloying at Cs and Pb sites on the energetics and electronic structure of CsPbI$_{3}$ using cluster expansion method in combination with first-principles calculations. For Ge-mixing at Pb-site, the $α$ and $β$-phases are considered with emphasis on the electronic structure, transition probability, absorption coefficient, efficiency, and carrier mobility of higher-symmetry configurations. CsPb$_{0.50}$Ge$_{0.50}$I$_{3}$ (Cs$_{2}$PbGeI$_{6}$) which takes up a double perovskite (elpasolite) structure has a direct band gap with no parity-forbidden transitions. Further, we utilize the alloy entropic effect to improve the material stability and optoelectronic properties of CsPbI$_{3}$ by multi-element mixing. For the proposed mixed compositions, the Fr{ö}hlich electron-phonon coupling constant is determined. Scattering rates and electron mobility are obtained from first-principles inputs. These lower Pb-content inorganic perovskites offer great promise as efficient solar cell materials for photovoltaic applications.

cond-mat.mtrl-sci

Periodic Materials Generation using Text-Guided Joint Diffusion Model

Equivariant diffusion models have emerged as the prevailing approach for generating novel crystal materials due to their ability to leverage the physical symmetries of periodic material structures. However, current models do not effectively learn the joint distribution of atom types, fractional coordinates, and lattice structure of the crystal material in a cohesive end-to-end diffusion framework. Also, none of these models work under realistic setups, where users specify the desired characteristics that the generated structures must match. In this work, we introduce TGDMat, a novel text-guided diffusion model designed for 3D periodic material generation. Our approach integrates global structural knowledge through textual descriptions at each denoising step while jointly generating atom coordinates, types, and lattice structure using a periodic-E(3)-equivariant graph neural network (GNN). Extensive experiments using popular datasets on benchmark tasks reveal that TGDMat outperforms existing baseline methods by a good margin. Notably, for the structure prediction task, with just one generated sample, TGDMat outperforms all baseline models, highlighting the importance of text-guided diffusion. Further, in the generation task, TGDMat surpasses all baselines and their text-fusion variants, showcasing the effectiveness of the joint diffusion paradigm. Additionally, incorporating textual knowledge reduces overall training and sampling computational overhead while enhancing generative performance when utilizing real-world textual prompts from experts.

cs.LG

A Hybrid Machine Learning Framework for Predicting Hydrogen Storage Capacities in Metal Hydrides: Unsupervised Feature Learning with Deep Neural Networks

In this study, we present a sophisticated hybrid machine-learning framework that significantly improves the accuracy of predicting hydrogen storage capacities in metal hydrides. This is a critical challenge due to the scarcity of experimental data and the complexity of high-dimensional feature spaces. Our approach employs the power of unsupervised learning through the use of a state-of-the-art autoencoder. This autoencoder is trained on elemental descriptors obtained from Mendeleev software, enabling the extraction of a meaningful and lower dimensional latent space from the input data. This latent representation serves as the basis for our deep multi-layer perceptron (MLP) model, which consists of five layers and shows good precision in predicting hydrogen storage capacities. Furthermore, our results show very good agreement with the results of density functional theory (DFT). In addition to addressing the limitations caused by limited and unevenly distributed data in the field of hydrogen storage materials, we also focus on discovering new materials that show promising opportunities for hydrogen storage. These materials were identified using both feature-based approaches and predictions generated by a large language model. Finally, our investigation into the effectiveness of transferring weights from the autoencoder to the MLP, in addition to the latent features, suggests that while this strategy slightly improves model performance indicated by a slightly higher R$^2$ value and lower RMSE, it emphasizes the intricate challenge of adapting pre-trained weights for specific supervised tasks.

cond-mat.mtrl-sci

Magnetization dynamics in skyrmions due to high-speed carrier injections from Dirac half-metals

Recent developments in the magnetization dynamics in spin textures, particularly skyrmions, offer promising new directions for magnetic storage technologies and spintronics. Skyrmions, characterized by their topological protection and efficient mobility at low current density, are increasingly recognized for their potential applications in next-generation logic and memory devices. This study investigates the dynamics of skyrmion magnetization, focusing on the manipulation of their topological states as a basis for bitwise data storage through a modified Landau-Lifshitz-Gilbert equation (LLG). We introduce spin-polarized electrons from a topological ferromagnet that induce an electric dipole moment that interacts with the electric gauge field within the skyrmion domain. This interaction creates an effective magnetic field that results in a torque that can dynamically change the topological state of the skyrmion. In particular, we show that these torques can selectively destroy and create skyrmions, effectively writing and erasing bits, highlighting the potential of using controlled electron injection for robust and scalable skyrmion-based data storage solutions.

cond-mat.mtrl-sci

Customizing PBE Exchange-Correlation functionals: A comprehensive approach for band gap prediction in diverse semiconductors

Accurate band gap prediction in semiconductors is crucial for materials science and semiconductor technology advancements. This paper extends the Perdew-Burke-Ernzerhof (PBE) functional for a wide range of semiconductors, tackling the exchange and correlation enhancement factor complexities within Density Functional Theory (DFT). Our customized functionals offer a clearer and more realistic alternative to DFT+U methods, which demand large negative U values for elements like Sulfur (S), Selenium (Se), and Phosphorus (P). Moreover, these functionals are more cost-effective than GW or Heyd-Scuseria-Ernzerhof (HSE) hybrid functional methods, therefore, significantly facilitating the way for unified workflows in analyzing electronic structure, dielectric constants, effective masses, and further transport and elastic properties, allowing for seamless calculations across various properties. We point out that such development could be helpful in the creation of comprehensive databases of band gap and dielectric properties of the materials without expensive calculations. Furthermore, for the semiconductors studied, we show that these customized functionals and the Strongly Constrained and Appropriately Normed semilocal density functional (SCAN) perform similarly in terms of the band gap.

cond-mat.mtrl-sci

Controlling Moisture for Enhanced Ozone Decomposition: A Study of Water Effects on CeO$_2$ Surfaces and Catalytic Activity

This study investigates the catalytic degradation of ground-level ozone on low-index stoichiometric and reduced CeO$_2$ surfaces using first-principles calculations. The presence of oxygen vacancies on the surface enhances the interaction between ozone and catalyst by serving as active sites for adsorption and decomposition. Our results suggest that the {111} surface has superior ozone decomposition performance due to unstable oxygen species resulting from reaction with catalysts. However, when water is present, it competes with ozone molecules for these active sites, resulting in reduced catalytic activity or water poisoning. A possible solution could be heat treatment that reduces the vacancy concentration, thereby increasing the available adsorption sites for ozone molecules while minimizing competitive adsorption by water molecules. These results suggest that controlling moisture content during operation is crucial for the efficient use of CeO$_2$-based catalysts in industrial applications to reduce ground-level ozone pollution.

cond-mat.mtrl-sci

MatSciRE: Leveraging Pointer Networks to Automate Entity and Relation Extraction for Material Science Knowledge-base Construction

Material science literature is a rich source of factual information about various categories of entities (like materials and compositions) and various relations between these entities, such as conductivity, voltage, etc. Automatically extracting this information to generate a material science knowledge base is a challenging task. In this paper, we propose MatSciRE (Material Science Relation Extractor), a Pointer Network-based encoder-decoder framework, to jointly extract entities and relations from material science articles as a triplet ($entity1, relation, entity2$). Specifically, we target the battery materials and identify five relations to work on - conductivity, coulombic efficiency, capacity, voltage, and energy. Our proposed approach achieved a much better F1-score (0.771) than a previous attempt using ChemDataExtractor (0.716). The overall graphical framework of MatSciRE is shown in Fig 1. The material information is extracted from material science literature in the form of entity-relation triplets using MatSciRE.

cs.CL

Tuning the Electronic and Magnetic Properties of Double Transition Metal MCrCT$_2$ (M = Ti, Mo) Janus MXenes for Enhanced Spintronics and Nanoelectronics

Janus MXenes, a new category of two-dimensional (2D) materials, shows promising potential for advances in optoelectronics, spintronics and nanoelectronics. Our theoretical investigations not only provide interesting insights but also highlight the promise of Janus MCrCT$_2$ (M = Ti, Mo; T = O, F, OH) MXenes for future spintronic applications and highlight the need for their synthesis. Electronic structure analysis shows different metallic and semi-metallic properties: MoCrCF$_2$ exhibits metallic properties, TiCrC(OH)$_2$ and MoCrCO$_2$ exhibit near semi-metallicity with spin polarization values of 61\% and 86\%, respectively, while TiCrCO$_2$ and TiCrCF$_2$ are completely half-metallic with 100\% spin polarization at the Fermi level. All studied Janus MXenes exhibit intrinsic ferromagnetism, which is mainly attributed to the chromium (Cr) atoms, as shown by the spin density difference plots. Among them, the TiCrCO$_2$ monolayer stands out with the highest exchange constant and ferromagnetic transition temperature (T$_c$). Notably, the O-terminated Janus MXenes exhibit weak perpendicular magnetic anisotropy, in contrast to the in-plane anisotropy observed for F and OH-terminated MXenes, making them particularly interesting for future spintronic applications which we further demonstrate with micromagnetic simulation which reveal distinct current-induced switching behaviors in these Janus MXenes with different surface terminations.

cond-mat.mtrl-sci