Computational Materials Science最新文献

{"title":"Low lattice thermal conductance of buckled GeTe/antimonene vdW interface device: A DFT + NEGF study","authors":"A. Sakthi Balaji,&nbsp;Akash Ramasamy,&nbsp;K. Janani Sivasankar,&nbsp;Hariharan Rajalakshmi Mohanraj,&nbsp;D. John Thiruvadigal","doi":"10.1016/j.commatsci.2025.113784","DOIUrl":"10.1016/j.commatsci.2025.113784","url":null,"abstract":"<div><div>Motivated by the exceptional thermoelectric performance of 2D buckled GeTe and Sb monolayers, thermoelectric transport characteristics of the stable GeTe/Antimonene (Sb) van der Waals heterostructure (vdWH) are examined by first-principles calculations supplemented by the non-equilibrium Green’s function approach (NEGF). The electronic aspects of these thermoelectric devices are assessed by reviewing the Seebeck coefficient (S) and electrical conductance (G_e) derived from transmission spectra. Simultaneously, the thermal conductance (κ_ph) of the system was computed by analysing the lattice/phonon transmission spectrum. The thermoelectric figure of merit (ZT) for the system is calculated by integrating the electron and phonon transmission spectra across various chemical potentials (μ) and temperatures (T). In this context, the heterostructure featuring a smaller interlayer vdw gap and reduced phonon thermal conductance ultimately exhibits superior thermoelectric performance. The effective phonon scattering at the interface establishes reduced phonon thermal conductance at the heterostructure. At 300 K, low phonon thermal conductance attains 43.23 pW/K and the highest ZT attains 6.97 for heterostructure. Our theoretical research provides an innovative technique and offers valuable theoretical insights into the thermoelectric transport properties of vdW heterostructures device.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113784"},"PeriodicalIF":3.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471483","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":"Investigating the temperature and Al doping effect on the O2 adsorption Process on ZnO nanowire surface: A ReaxFF-MD approach","authors":"Waleed Ftahi ,&nbsp;Nusaibah AL-Shaeri ,&nbsp;Yuanwei Yang ,&nbsp;Sara Ahmed A. ,&nbsp;Yongliang Tang ,&nbsp;Qingxiang Liu ,&nbsp;Yuxiang Ni","doi":"10.1016/j.commatsci.2025.113774","DOIUrl":"10.1016/j.commatsci.2025.113774","url":null,"abstract":"<div><div>ZnO nanostructures have garnered significant attention from researchers and industries due to their outstanding properties as gas-sensing materials. Aluminium (Al) doping, in particular, can further fine-tune or optimize these gas-sensing properties. In this research, we investigate the adsorption of O₂ molecules on undoped and Al-doped ZnO nanowires at <span><math><mrow><mn>5</mn><mtext>%</mtext></mrow></math></span> and <span><math><mrow><mn>10</mn><mtext>%</mtext></mrow></math></span> doping concentrations using advanced reactive force field (ReaxFF)-based molecular dynamics (MD) simulations. The adsorption process is studied at temperatures of 100 K, 300 K, and 500 K, with 300 O₂ molecules in each case, and the influences of these factors on the adsorption type are analyzed through radial distribution function (RDF) analysis. The adsorption behavior of O₂ molecules on both undoped and Al-doped ZnO nanowires is compared by calculating system energy, adsorption energy, and the number of adsorbed molecules. The results show that the binding distances between O₂ molecules and Zn and Al atoms on the nanowire surfaces are 2.18 Å and 1.78 Å, respectively, as determined from RDF analysis. The O₂ adsorption process on undoped and Al-doped ZnO nanowire surfaces occurs in two distinct stages, with higher temperatures leading to an increased number of adsorbed molecules. As Al doping increases, it significantly accelerates O₂ adsorption in the initial stage, while pure ZnO shows greater adsorption number in the second stage. Chemisorption dominates the interaction in both undoped and Al-doped ZnO.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113774"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463868","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":"Investigating vacancy-defect effects on the vibration characteristics of graphene resonators with molecular dynamics simulation","authors":"Kuanshu Jiang ,&nbsp;Jiangtao Wang ,&nbsp;Jiangkai Yuan ,&nbsp;Quan Wang","doi":"10.1016/j.commatsci.2025.113794","DOIUrl":"10.1016/j.commatsci.2025.113794","url":null,"abstract":"<div><div>Due to the limitations of graphene processing technology, the as-prepared graphene will inevitably have various defects, which will have remarkable effects on the macroscopic properties of graphene. In this work, graphene resonators based on vacancy defects are investigated. The resonance properties of graphene are demonstrated by molecular dynamics simulations, in which the effects of single and double vacancy defects at different positions and numbers on the resonant frequencies of graphene nanoribbons are unveiled. The results show that the C atoms at the vacancy defect have a much larger movement in the normal direction than in the region of C atoms bound by a complete C–C bond. The resonant frequency is not affected by the location of vacancy defects. As the number of vacancy defects increases, the resonance amplitude value increases monotonically in the normal direction. However, there is no significant difference in the resonance amplitude value when comparing single and double vacancy defects. The resonant frequency decreases monotonically with the increase in the number of vacancy defects, while for the same number of vacancy defects, the resonant frequency is generally smaller for double vacancy defects than for single vacancy defects. The resonant frequency is not sensitive to individual single and double vacancy defects rather than is more affected by a large concentration of vacancy defects, suggesting that extra attention needs to be given to the case of large concentration defects. Our achievement will lay a strong foundation for graphene resonators’ design and performance optimization.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113794"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143464019","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":"Combined diffuse and sharp interface approach to unravel morphological dynamics in solid-state Li-ion batteries","authors":"Fiyanshu Kaka,&nbsp;Kalyan Sundar Krishna Chivukula","doi":"10.1016/j.commatsci.2025.113756","DOIUrl":"10.1016/j.commatsci.2025.113756","url":null,"abstract":"<div><div>Addressing the limitations of traditional Li-ion batteries, this study focuses on the crucial transition to All-Solid-State Batteries (ASSBs) by emphasizing the paramount importance of solid electrolyte morphology on battery performance. Utilizing a computational phase-field approach, the study simulates binary solid-electrolyte morphologies and integrates them into ASSBs through a robust process to assess their impact on electrochemical characteristics. The intricate process of transitioning from simulated morphology to Computer-Aided Design geometry is thoroughly explored in the manuscript. Furthermore, upon the successful incorporation of solid-electrolyte morphology, simulations are performed at a constant discharge current density of 5 A.m⁻², revealing a significant order of magnitude difference in the discharging times for ASSBs with varying volume fractions, underscoring the pivotal role of solid-electrolyte’s morphology. Additionally, mechanical strength is evaluated across volume fractions ranging from 0.3 to 0.7, showcasing a substantial threefold enhancement under a compressive stress of 10 MPa. Guided by mechano-electrochemical characteristics, an optimal blend ratio for the solid-electrolyte is identified. These findings underscore the crucial role of tailoring solid-electrolyte morphology for optimal ASSB performance, providing valuable guidance for advancing high-performance, safe, and sustainable battery technologies.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113756"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463869","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":"Computational insights into surface dynamics, Mg clustering, and dendrite formation in magnesium batteries","authors":"Fernando A. Soto","doi":"10.1016/j.commatsci.2025.113791","DOIUrl":"10.1016/j.commatsci.2025.113791","url":null,"abstract":"<div><div>This study sheds light on the surface dynamics of a MgTFSI-Cl/DME-based electrolyte solution and a pristine Mg(0001) surface, employing density functional theory (DFT) simulations to characterize the surface area and isosurface of magnesium under varying temperature and salt concentration conditions. A primary focus is understanding how these surface dynamics and factors help us understand the precursor mechanisms and structures leading to dendrite formation in magnesium batteries. The simulations reveal that the combination of high salt concentration and temperature leads to excessive surface areas, deviating from the ideal ‘Goldilocks morphology’, and can cause the isosurface to shift away from the anode’s surface. This displacement can create a concentration gradient conducive to Mg clustering, a precursor to dendrite formation. The simulations provide critical insights into the complex interplay between surface area, isosurface characteristics, and the operational parameters of magnesium anodes. The results underscore the importance of optimizing these factors to mitigate dendrite formation, offering valuable guidance for developing more efficient and safer magnesium-ion batteries (MiBs). This study enhances our understanding of the fundamental processes governing dendrite formation and proposes a novel approach to addressing one of the key challenges in advancing magnesium battery technology.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113791"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463871","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":"Prediction of lanthanide-containing ternary compounds","authors":"Huaijun Sun ,&nbsp;Chao Zhang ,&nbsp;Jianbo Huang ,&nbsp;Xingdu Fan ,&nbsp;Weiyi Xia ,&nbsp;Ling Tang ,&nbsp;Renhai Wang ,&nbsp;Kunpeng Cui ,&nbsp;Cai-Zhuang Wang","doi":"10.1016/j.commatsci.2025.113717","DOIUrl":"10.1016/j.commatsci.2025.113717","url":null,"abstract":"<div><div>By substitution of rare-earth (R) elements for La and other group 14 elements (X) for Si in the eight most stable La-Si-P ternary phases obtained previously, the stability of the R-X-P ternary compounds are investigated. We show that the formation energies of many such ternary phases are lowered after the substitution, and some stable ternary phases are obtained under the new convex hulls constructed including the newly predicted low-energy phases. Phonon spectra calculations demonstrate the dynamical stability for these lanthanides containing ternary compounds. The Gibbs formation energies as the function of temperature also demonstrate thermodynamic stability for most of the new phases with respect to the nearby competitive crystal phases in the convex hull. The electronic band structures of these ternary phases show metallic properties and indicate spin polarization for the R₅XP₃ phases. The discoveries of these ternary phases enrich the existing phase diagrams of lanthanide-containing ternary compounds.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"251 ","pages":"Article 113717"},"PeriodicalIF":3.1,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444356","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":"Relating the formation energies for oxygen vacancy defects to the structural properties of tungsten oxides","authors":"Ryan D. Kerr ,&nbsp;Mark R. Gilbert ,&nbsp;Samuel T. Murphy","doi":"10.1016/j.commatsci.2025.113781","DOIUrl":"10.1016/j.commatsci.2025.113781","url":null,"abstract":"<div><div>Tungsten is one of the materials of choice for several commercial fusion power plant designs, in particular, for divertor targets and the first wall. In maintenance conditions or during a loss of coolant accident, tungsten is expected to reach temperatures at which it readily volatilises as tungsten trioxide, potentially distributing radioactive material and posing a hazard to personnel. The oxidation of tungsten is reported to show an orientation dependence, however, the mechanism by which it occurs is not fully understood, providing an obstacle to the development of tungsten smart alloys that display reduced oxidation. Using DFT+<span><math><mi>U</mi></math></span> simulations, it is shown how key features of the electronic structure of the tungsten–oxygen system change as the tungsten–oxygen ratio evolves. Formation and migration barriers for oxygen in the different tungsten oxides are determined, allowing an assessment of its mobility in the phases observed during the oxidation process. Our results provide a new level of understanding of the sub-stoichiometric Magnéli phases that are observed during the oxidation of tungsten, which are perceived to be composed of WO₂- and WO₃-like regions.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113781"},"PeriodicalIF":3.1,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143464018","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":"The influence of N content on structures and mechanical properties of FCC_(AlCrMoTiV)1-XNX high-entropy nitrides: A density functional theory (DFT) study based on site preference","authors":"Cheng Qian ,&nbsp;Xingyu Chen ,&nbsp;Longju Su ,&nbsp;Xiaoqiong Zhang ,&nbsp;Rong Chen ,&nbsp;Jiansen Wen ,&nbsp;Bo Wu","doi":"10.1016/j.commatsci.2025.113787","DOIUrl":"10.1016/j.commatsci.2025.113787","url":null,"abstract":"<div><div>High-entropy nitrides (HENs) have been extensively studied for their exceptional mechanical properties, making them promising candidates for surface modification in machining tools and aerospace materials. However, the mechanisms by which nitrogen content influences the structure and mechanical properties of HENs remain unclear. This study constructed a theoretical model for ordered FCC_(AlCrMoTiV)_1-XN_X HENs based on the site occupying fractions (SOFs) of metal atoms and the preferred occupying distribution (POD) of nitrogen atoms. Using density functional theory, we investigated the microscopic structure and mechanical properties of these nitrides. The results show that the nitrogen content significantly affects the lattice distortion of HENs and the strength of chemical bonding, thereby altering their mechanical properties. At the ground state, the lattice distortion reaches a minimal value when the nitrogen content is 46.67 %, and the Youngʼs modulus <span><math><mrow><mi>E</mi></mrow></math></span>, and hardness <span><math><mrow><mi>H</mi></mrow></math></span> are 361.06, and 22.58 GPa, respectively. In addition, we further predicted the temperature-dependent lattice distortion and mechanical properties of FCC_(AlCrMoTiV)_1-XN_X HENs. When nitriding reaches saturation, lattice distortion is most strongly influenced by temperature. The HEN with 41.82 % nitrogen content exhibits the most outstanding mechanical properties. Even when the temperature rises to 1273 K, it maintains a hardness of 17.38 GPa and retains its ductility.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"251 ","pages":"Article 113787"},"PeriodicalIF":3.1,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444358","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":"Atomistic modelling of femtosecond laser melting of Pb nanoparticles embedded in Al film","authors":"Mikhail I. Arefev,&nbsp;Leonid V. Zhigilei","doi":"10.1016/j.commatsci.2025.113786","DOIUrl":"10.1016/j.commatsci.2025.113786","url":null,"abstract":"<div><div>Ultrashort pulse laser irradiation of nanoparticles embedded into a matrix with a higher melting point presents a case study for investigation of the kinetics and mechanisms of nanoscale melting occurring in the absence of surface nucleation of liquid phase. The ultrahigh heating rates induced by femtosecond laser irradiation, ∼10¹⁵ K/s, create conditions of substantial superheating prior to the onset of rapid homogeneous melting. The suppression of surface nucleation of liquid phase in the embedded nanoparticles can further increase the maximum values of superheating, but the detailed understanding of the kinetics and mechanisms of melting under confinement by the matrix material is still lacking. In this study, the melting of an octahedral 20 nm Pb nanoparticle embedded into a 30-nm-thick Al film and irradiated by a 110 fs laser pulse is investigated in a series of molecular dynamics simulations. The heating of the embedded Pb nanoparticle is found to be a multi-stage process controlled by the relative strength of the electron–phonon coupling of the nanoparticle and matrix material. The compression of the nanoparticle due to the confined thermal expansion and volume increase upon melting has a strong effect on the equilibrium melting temperature. When this effect is accounted for, the maximum level of superheating achievable prior to melting is consistent with that required for the onset of homogeneous melting in bulk systems. The key factors that define the kinetics of melting at moderate laser fluences are (1) the negative feedback to the melting process provided by the compressive stresses generated due to the volume expansion upon melting of the Pb nanoparticle, (2) the stabilization of the crystal structure in the vicinity of semicoherent {1<!--> <!-->1<!--> <!-->1} interfaces with the matrix, and (3) the gradual resupply of the thermal energy transformed to the heat of melting by the heat transfer from the Al matrix. As a result, the laser fluence range where the melting proceeds slowly, on the timescale of hundreds of picoseconds, is substantially expanded as compared to free-standing nanoparticles or films irradiated by ultrashort laser pulses.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"251 ","pages":"Article 113786"},"PeriodicalIF":3.1,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444357","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":"The spin–orbit coupling induced stereochemical activity and nonlinear optical response in Pb2BO3X (X = Cl, Br, I)","authors":"Jialong Wang,&nbsp;Mei Hu,&nbsp;Yaru Wang,&nbsp;Qun Jing,&nbsp;Haiming Duan,&nbsp;Zhaohui Chen","doi":"10.1016/j.commatsci.2025.113783","DOIUrl":"10.1016/j.commatsci.2025.113783","url":null,"abstract":"<div><div>Spin-orbit coupling (SOC) has gained significant attention for its ability to modify electronic structures and optical properties. In this study, first-principles calculations are employed to investigate the electronic structures and optical properties of Pb₂BO₃X (X = Cl, Br, I) induced by SOC. The results reveal that SOC induces band downshifting and splitting at the top of the valence band (VB) and the bottom of conduction band (CB), leading to decreasement of GGA-PBE and HSE06 bandgaps. The GGA-PBE bandgaps of Pb₂BO₃X (X = Cl, Br, I) decrease from 3.55, 3.33, and 3.00 eV to 3.42, 3.11, and 2.70 eV, respectively, and the reduced HSE06 bandgaps (4.27, 3.88, and 3.50 eV for Pb₂BO₃Cl, Pb₂BO₃Br, and Pb₂BO₃I) are closer to experimental values. It is also observed that the stereochemical activity of lone pairs around the Pb atoms is enhanced with the inclusion of SOC. Furthermore, SOC leads to attenuated second harmonic generation (SHG) coefficients for Pb₂BO₃X (X = Cl, Br, I), with values of 9.00, 10.00, 11.34 × KDP (KH₂PO₄), which are in closer agreement with experimental values. Using the “<em>shifting of conduction band</em>” method, we find that the band splitting and downshifting induced by SOC contribute to a reduction in the effective SHG response. These findings provide valuable insights into the role of SOC in tuning the electronic and optical properties of Pb₂BO₃X (X = Cl, Br, I), offering potential pathways for designing materials with enhanced nonlinear optical responses.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"251 ","pages":"Article 113783"},"PeriodicalIF":3.1,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143437482","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}