Computational Materials Science最新文献

{"title":"Cluster transport induced by a thermal gradient on a crystalline surface","authors":"A. Roux,&nbsp;N. Combe","doi":"10.1016/j.commatsci.2024.113620","DOIUrl":"10.1016/j.commatsci.2024.113620","url":null,"abstract":"<div><div>Using molecular dynamic (MD) simulations, we study the thermomigration of small clusters consisting of 2, 3 or 4 atoms on a crystalline surface. After evidencing the thermomigration by analyzing the cluster trajectories, we generalize the thermodynamic integration method to compute a thermodynamic potential driving the probability of presence of the clusters on a substrate submitted to a thermal gradient. The study of this thermodynamic potential allows to disentangle the thermomigration effective force from the stochastic diffusion. We show that the heat of transport characterizing the effective force responsible for thermomigration is the sum of the free energy of the cluster–substrate and cluster internal energies. Finally, an unidimensional kinetic model for the thermomigration is proposed and its results compared to the MD trajectories.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113620"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhancing MXene-Based anodes with two-dimensional VO2/V2CO2 heterostructures: A first-principles calculations study","authors":"Wenjing Ji,&nbsp;Yuntong Peng,&nbsp;Yazhou Wang,&nbsp;Shangquan Zhao,&nbsp;Naigen Zhou","doi":"10.1016/j.commatsci.2024.113615","DOIUrl":"10.1016/j.commatsci.2024.113615","url":null,"abstract":"<div><div>The integration of MXene with complementary two-dimensional materials to form heterostructures has the potential to improve the electrochemical performance of MXene. In our study, we constructed a van der Waals heterostructure composed of VO₂/V₂CO₂, and evaluated its effectiveness as an anode material for Li, Na, and Mg ion batteries through first-principles density functional theory simulations. Our findings reveal that the VO₂/V₂CO₂ heterostructure demonstrates exceptional stability and inherent metallic characteristics. We identified diffusion barriers for Li, Na, and Mg ions within the interlayer to be relatively low—at 0.38 eV, 0.22 eV, and 0.51 eV, respectively—suggesting efficient ion transport. Furthermore, the average open-circuit voltages (OCVs) for Li-ion, Na-ion, and Mg-ion batteries were found to be between 0 and 1.5 V, which is advantageous for inhibiting lithium dendrite growth. Remarkably, the heterostructure showcases a theoretical storage capacity reaching up to 585mA h/g for Li, 351 mA h/g for Na, and an impressive 936 mA h/g for Mg adsorption—outstripping the capabilities of graphite and surpassing several other two-dimensional materials. These compelling results underscore the VO₂/V₂CO₂ heterostructure as a highly promising anode material, particularly for Li-ion and Mg-ion battery applications.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113615"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mechanical behavior of planar β-borophene under different loadings: Insights from molecular dynamics simulations","authors":"Yantao Yang ,&nbsp;Tongwei Han ,&nbsp;Yunyi Sun ,&nbsp;Xuanzheng Li ,&nbsp;Xiaoyan Zhang","doi":"10.1016/j.commatsci.2025.113687","DOIUrl":"10.1016/j.commatsci.2025.113687","url":null,"abstract":"<div><div>Borophene, a two-dimensional (2D) nanomaterial composed of boron, exhibits remarkable mechanical properties and anisotropic structural characteristics, making it a promising candidate for advanced applications in flexible electronics, energy storage, and nanoscale mechanical systems. This study employs molecular dynamics simulations to systematically investigate the mechanical responses of planar β-borophene under tensile, shear, and nanoindentation loading. Key mechanical parameters, including Young’s modulus, tensile strength, and shear modulus, are evaluated along the zigzag and armchair directions, revealing weak anisotropy and brittle fracture behavior. Nanoindentation simulations using spherical and cylindrical indenters highlight distinct deformation mechanisms, with stress distributions and bond elongation dynamics dictating failure modes. The findings elucidate the influence of atomic bonding configurations on β-borophene’s load-bearing capacity and deformation characteristics, offering critical theoretical insights and design guidelines for its integration into next-generation electromechanical devices.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113687"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"First-principles design of high speed nanoscale interconnects based on GaN nanoribbons","authors":"Ankita Nemu ,&nbsp;Sangeeta Singh ,&nbsp;Kamal K. Jha ,&nbsp;Neha Tyagi ,&nbsp;Neeraj K. Jaiswal","doi":"10.1016/j.commatsci.2024.113625","DOIUrl":"10.1016/j.commatsci.2024.113625","url":null,"abstract":"<div><div>Investigation of efficient interconnects for upcoming nano-electronic devices is an active area of research. In the present work, we gauged the effect of O-passivation on zigzag GaN nanoribbons (ZGaNNR) as well as armchair GaN nanoribbons (AGaNNR) for interconnect applications. Various possible configurations of O-passivation were considered and the findings thus obtained were compared. It is reported that O-passivated ZGaNNR nanoribbons exhibit metallic character unlike H-passivated counterparts. On the other hand, the magnitude of band gap for AGaNNR is drastically reduced upon O-passivation. It is also noticed that replacing H with O for passivation purpose also enhances the structural stability of the ribbons making them preferable. The non equilibrium Green’s formalism coupled with density functional theory was employed to study the transport properties. The obtained current–voltage (I-V) characteristics confirm maximum current for O@both-edges while minimum current has been obtained for O@Ga-edge. The small-signal dynamic performance parameters such as <span><math><msub><mrow><mi>R</mi></mrow><mrow><mi>Q</mi></mrow></msub></math></span>, <span><math><msub><mrow><mi>C</mi></mrow><mrow><mi>Q</mi></mrow></msub></math></span>, and <span><math><msub><mrow><mi>L</mi></mrow><mrow><mi>K</mi></mrow></msub></math></span> are derived using the two-probe model for the interconnect modeling. The O@N-edge functionalized ZGaNNR has the lowest values of <span><math><msub><mrow><mi>R</mi></mrow><mrow><mi>Q</mi></mrow></msub></math></span> (12.9 K<span><math><mi>Ω</mi></math></span>), <span><math><msub><mrow><mi>C</mi></mrow><mrow><mi>Q</mi></mrow></msub></math></span> (8.60 pF/<span><math><mi>μ</mi></math></span>m), <span><math><msub><mrow><mi>L</mi></mrow><mrow><mi>K</mi></mrow></msub></math></span> (358.511 nH/<span><math><mi>μ</mi></math></span>m), and quantum latency <span><math><msub><mrow><mi>τ</mi></mrow><mrow><mi>p</mi></mrow></msub></math></span> (0.111 ms) and higher Fermi velocity. Our work paves the way for the realization of low-power nanoscale high-speed interconnect applications.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113625"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151101","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"On the numerical sensitivity of cellular automata grain structure predictions to large thermal gradients and cooling rates","authors":"Matt Rolchigo,&nbsp;Benjamin Stump,&nbsp;John Coleman,&nbsp;Samuel Temple Reeve,&nbsp;Gerry L. Knapp,&nbsp;Alex Plotkowski","doi":"10.1016/j.commatsci.2024.113648","DOIUrl":"10.1016/j.commatsci.2024.113648","url":null,"abstract":"&lt;div&gt;&lt;div&gt;Cellular automata (CA) models of as-solidified grain structure, originally developed and applied to casting, have become a common means of predicting grain structure resulting from Additive Manufacturing (AM) processes. The majority of these models are based on the decentered octahedron approach, which attempts to correct for the effect of grid anisotropy on the prediction of competitive solidification of dendritic grains. However, AM solidification occurs under cooling rates (&lt;span&gt;&lt;math&gt;&lt;mover&gt;&lt;mrow&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;̇&lt;/mo&gt;&lt;/mrow&gt;&lt;/mover&gt;&lt;/math&gt;&lt;/span&gt;) and thermal gradients (&lt;span&gt;&lt;math&gt;&lt;mi&gt;G&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;) that are orders of magnitude larger than those encountered in casting, and no systematic investigation on the effect of the CA model cell size (&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;x&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;) and time step (&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;t&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;) on AM microstructure predictions has been performed. In this study, such an investigation is first performed via simulation of individual grains of various crystallographic orientations with a fixed, unidirectional &lt;span&gt;&lt;math&gt;&lt;mi&gt;G&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;, showing that CA prediction of the steady-state undercooling matched the expected values based on the interfacial response function at small &lt;span&gt;&lt;math&gt;&lt;mi&gt;G&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt; and deviated from the expected values at large &lt;span&gt;&lt;math&gt;&lt;mi&gt;G&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;. Simulation of competitive growth of multiple grains showed a weakening of the predicted texture as &lt;span&gt;&lt;math&gt;&lt;mi&gt;G&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt; and &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;x&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; became large. Simulation of solidification under AM conditions, where &lt;span&gt;&lt;math&gt;&lt;mi&gt;G&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt; and &lt;span&gt;&lt;math&gt;&lt;mover&gt;&lt;mrow&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;̇&lt;/mo&gt;&lt;/mrow&gt;&lt;/mover&gt;&lt;/math&gt;&lt;/span&gt; vary spatially across the melt pools, showed that not only does grain selection weaken and deviate from expectations at large &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;x&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;, but grains with crystallographic &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mo&gt;〈&lt;/mo&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;mspace&gt;&lt;/mspace&gt;&lt;mn&gt;0&lt;/mn&gt;&lt;mspace&gt;&lt;/mspace&gt;&lt;mn&gt;0&lt;/mn&gt;&lt;mo&gt;〉&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; aligned with the grid directions are more adversely affected by the temperature field discontinuities than grains with other crystallographic orientations. Despite the fact that the exact grain competition results depended on &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;t&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;, the overall texture development was notably less sensitive to &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;t&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; than &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;x&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;, provided that a reasonable value of &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;t&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; is selected based on the ratio of &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;mi&gt;x&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; to the maximum local solidification velocity in the simulation domain. Finally, from the directional solidification and AM simulation results, an analysis","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113648"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unraveling the role of temperature on the onset of ejecta formation at atomic scales","authors":"Marco J. Echeverria ,&nbsp;Alison M. Saunders ,&nbsp;Robert E. Rudd ,&nbsp;Tomorr Haxhimali ,&nbsp;Saryu J. Fensin ,&nbsp;Avinash M. Dongare","doi":"10.1016/j.commatsci.2025.113659","DOIUrl":"10.1016/j.commatsci.2025.113659","url":null,"abstract":"<div><div>Shock wave interactions with perturbations on a free surface can lead to the inversion and growth of the perturbation and eventual ejection of a jet of material, referred to as an ejecta microjet, from shocked surfaces. This study carries out large-scale molecular dynamics (MD) simulations using single-crystal Cu and Sn systems with a pre-existing groove to characterize the localized gradients in temperatures and pressures generated that render the microjet formation. MD simulations are carried out for three loading orientations (along the [001], [011], and [111] directions) and shock pressures ranging from 16 GPa to 100 GPa to understand the role of temperatures generated at the groove vertex on the formation of ejecta. The simulations suggest that the interaction of the shock wave with the groove results in a localized increase in temperatures, leading to localized softening at the groove vertex and the generation of an ejecta microjet. For Cu systems, the simulations suggest that the orientation effects on shock wave structures, velocities, and localized softening affect the ejecta formation at low pressures. Jetting is only observed when temperatures at the groove vertex are high enough to induce localized softening (close to melting temperature), and the jet velocity increases with shock pressure. In contrast, the loading orientation is rendered inconsequential for Sn systems due to the melting of the material during shock compression at the pressures chosen. The jet velocities are similar, regardless of crystal orientation in Sn systems.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113659"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151133","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ab initio investigation on intrinsic Ga vacancies in β-Ga2O3 utilizing hybrid functional combined with the shell DFT-1/2 approach","authors":"L.Y. Hao ,&nbsp;X.P. Zhang ,&nbsp;M.Y. Niu ,&nbsp;S.K. Shen ,&nbsp;X. Liu ,&nbsp;S.L. Zhang ,&nbsp;J.L. Du ,&nbsp;P.P. Wang ,&nbsp;P. Liu ,&nbsp;E.G. Fu","doi":"10.1016/j.commatsci.2024.113607","DOIUrl":"10.1016/j.commatsci.2024.113607","url":null,"abstract":"<div><div>The monoclinic crystal system β-gallium oxide (β-Ga₂O₃) is an advantageous semiconductor, characterized by a substantial bandgap of approximately 4.8 eV, exceptional stability under ambient conditions, and transparency to ultraviolet (UV) light. In practical applications, it is critical to effectively manage defects within β-Ga₂O₃. Failure to rigorously control defect types and concentrations can significantly compromise device stability and reliability. Among the prevalent and impactful defects, Ga intrinsic vacancies notably affect the optoelectronic performance of β-Ga₂O₃, yet they have not been comprehensively studied using suitable generalized approximations. This paper systematically examines the electronic and optical properties of β-Ga₂O₃ with intrinsic Ga vacancies using hybrid functional methods combined with the shell DFT-1/2 approach. Key properties analyzed include electronic bandgap and density of states, structural properties like elastic constants and phonon dispersion, and optoelectronic properties such as permittivity, absorption spectra, and electronic energy-loss spectra. Detailed discussion is provided on the formation energy curves of these Ga intrinsic defects.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113607"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Accurate prediction of structural and mechanical properties on amorphous materials enabled through machine-learning potentials: A case study of silicon nitride","authors":"Ganesh Kumar Nayak ,&nbsp;Prashanth Srinivasan ,&nbsp;Juraj Todt ,&nbsp;Rostislav Daniel ,&nbsp;Paolo Nicolini ,&nbsp;David Holec","doi":"10.1016/j.commatsci.2024.113629","DOIUrl":"10.1016/j.commatsci.2024.113629","url":null,"abstract":"<div><div>Ab initio calculations represent the technique of election to study material system, however, they present severe limitations in terms of the size of the system that can be simulated. Often, the results in the simulation of amorphous materials depend dramatically on the size of the system. Here, we overcome this limitation for the specific case of mechanical properties of amorphous silicon nitride (a-Si<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>N<span><math><msub><mrow></mrow><mrow><mn>4</mn></mrow></msub></math></span>) by training a machine learning (ML) interatomic model. Our strategy is based on the generation of targeted training sets, which also include deliberately stressed structures. Using this dataset, we trained a moment tensor potential (MTP) for a-Si<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>N<span><math><msub><mrow></mrow><mrow><mn>4</mn></mrow></msub></math></span>. We show that molecular dynamics simulations using the ML model on much larger systems yield elastically isotropic response and can reproduce experimental measurement. To do so, models containing at least <span><math><mrow><mo>≈</mo><mn>3</mn><mo>,</mo><mn>500</mn></mrow></math></span> atoms are necessary. The Young’s modulus calculated from the MTP at room temperature is 220<span><math><mrow><mspace></mspace><mi>GPa</mi></mrow></math></span>, which is very well in agreement with the nanoindentation measurement. Our study demonstrates the broader impact of machine learning potentials for predicting structural and mechanical properties, even for complex amorphous structures.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113629"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unveiling electronic constraints on basal planes of 2D transition metal chalcogenides for optimizing hydrogen evolution catalysis: A theoretical analysis","authors":"Faling Ling ,&nbsp;Shuijie Zhang ,&nbsp;Zheng Dai ,&nbsp;Shaobo Wang ,&nbsp;Yuting Zhao ,&nbsp;Li Li ,&nbsp;Xianju Zhou ,&nbsp;Xiao Tang ,&nbsp;Dengfeng Li ,&nbsp;Xiaoqing Liu","doi":"10.1016/j.commatsci.2025.113658","DOIUrl":"10.1016/j.commatsci.2025.113658","url":null,"abstract":"<div><div>Two-dimensional transition metal dichalcogenides (2D-TMDs) have emerged as promising alternatives to noble metal platinum for hydrogen evolution reaction (HER) electrocatalysts. However, their inert basal planes present a significant challenge, and effective activation strategies have not been fully explored. In this study, we address this gap by performing density functional theory (DFT)-based first-principles calculations to develop a comprehensive theoretical framework for activating the basal planes of 2D-TMDs. We reveal two key electronic descriptors—(1) the energy of the lowest unoccupied state (<em>E</em>_lu) and (2) the degree of valence electron localization—that govern hydrogen adsorption on the basal planes. These insights form the foundation of a novel strategy: precision doping of metal atoms onto the basal planes of Mo- and W-based 2D-TMDs. This strategy provides unprecedented control over the electronic structures at the active sites, significantly enhancing valence electron localization and improving HER activity. Additionally, we determine the optimal doping concentration, offering crucial guidance for experimental studies. Our work presents a pioneering, descriptor-driven methodology for activating 2D-TMD basal planes, providing transformative insights for HER electrocatalyst design. This research sets a new direction for developing highly efficient water-splitting technologies, accelerating progress toward sustainable hydrogen production.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113658"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151130","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-throughput screening of ternary and quaternary chalcogenide semiconductors for photovoltaics","authors":"Md Habibur Rahman,&nbsp;Arun Mannodi-Kanakkithodi","doi":"10.1016/j.commatsci.2024.113654","DOIUrl":"10.1016/j.commatsci.2024.113654","url":null,"abstract":"<div><div>Composition engineering offers a promising approach to discover new semiconductors with attractive optoelectronic properties. Screening based on high-throughput atomistic simulations provides a way to perform multi-objective optimization across a combinatorial compositional space. In this study, we used density functional theory (DFT) to explore the chemical space of ternary ABX₂ and quaternary A₂BCX₄ chalcogenide semiconductors with X <span><math><mo>⊂</mo></math></span> {S, Se, Te}, focusing on their thermodynamic stability, optoelectronic properties, and defect behavior. The A₂BCX₄ chemical space was defined as A <span><math><mo>⊂</mo></math></span>{Na, K, Rb, Cs, Cu, Ag}, B <span><math><mo>⊂</mo></math></span>{Mg, Ca, Sr, Ba, Zn, Cd}, and C <span><math><mo>⊂</mo></math></span> {Sn, Ge}, while the ABX₂ chemical space was defined as A <span><math><mo>⊂</mo></math></span> {Na, K, Rb, Cs, Cu, Ag} and B <span><math><mo>⊂</mo></math></span> {Al, Ga, In}. Each composition in either space was simulated using the Kesterite-type ordering as well as the Stannite-type ordering. For a total of 540 compounds, we performed geometry optimization, electronic structure, and optical absorption calculations using the GGA-PBEsol functional followed by the hybrid HSE06 functional with spin–orbit coupling (SOC), to determine formation and decomposition energies, bandgap, and spectroscopic limited maximum efficiency (SLME). Based on the HSE06+SOC computations, 45 compounds were found to be stable against decomposition and showed SLME <span><math><mo>&gt;</mo></math></span> 30%, suggesting high potential as single-junction solar cell absorbers. Although the Kesterite ordering is generally more stable than Stannite, the latter shows narrower bandgaps which are more suitable for solar absorption. We performed detailed point defect calculations on two selected candidates and found that they may be prone to harmful anti-site substitutional defects, which is a common issue in ternary and quaternary chalcogenides. We believe that further composition optimization via alloying at the cation or anion sites, and doping with suitable species, will help make the compounds more defect-tolerant, and our dataset provides the impetus for future studies.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"249 ","pages":"Article 113654"},"PeriodicalIF":3.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}