Computational Materials Science最新文献_第6页

CO₂/CH₄ competitive adsorption in MOFs: high-throughput screening and molecular simulation MOFs中CO₂/CH₄竞争性吸附：高通量筛选和分子模拟

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-24 DOI: 10.1016/j.commatsci.2026.114603

Ziheng Wang, Jinchen Cao, Xiaojian Wang, Wenbo Gu

This study conducted high-throughput screening(HTS) of 12,020 MOFs using random forest assistance, combined with SHAP analysis. It identified K_CO2, O%, and ASA as positive descriptors for adsorption performance, while TDU and Density showed negative correlations. Subsequently, six MOFS with the best performance were selected (DUWROE, EJIDUW01, NISBEX, QUQHAM, TIDQIG, and XEHSOT). The results indicates that DUWROE represents thermodynamically dominated high-capacity materials, whose high adsorption capacity stems from larger pores and heterogeneous strong adsorption sites, but exhibits lower diffusion and local distribution selectivity, making it suitable for capacity-dominated processes such as Pressure Swing Adsorption (PSA). NISBEX, on the other hand, represents a kinetically driven, highly selective material. Its pore size distribution, achieved through precise sieving, enables excellent diffusion selectivity and molecular local enrichment. However, its adsorption capacity is limited, making it more suitable for selectivity-driven processes like membrane separation. Further research reveals that differences in adsorption energy and adsorption heat can serve as indicators for distinguishing the distribution of strong and weak adsorption sites within MOFs. This work provides clear structure-property correlation principles and selection guidelines for the rational design of MOFs tailored to diverse separation requirements.

本研究利用随机森林辅助，结合SHAP分析对12020个mof进行了高通量筛选（HTS）。结果表明，KCO2、O%和ASA是吸附性能的正相关描述符，而TDU和密度呈负相关。随后，选择了6个性能最佳的mof （DUWROE、EJIDUW01、NISBEX、QUQHAM、TIDQIG和XEHSOT）。结果表明，DUWROE是一种以热力学为主导的高容量材料，其高吸附容量源于较大的孔隙和非均相强吸附位点，但具有较低的扩散和局部分布选择性，适合于变压吸附（PSA）等以容量为主导的过程。另一方面，NISBEX代表了一种动力学驱动的高选择性材料。它的孔径分布，通过精确的筛分，使出色的扩散选择性和分子局部富集。然而，它的吸附能力是有限的，这使得它更适合于选择性驱动的过程，如膜分离。进一步研究表明，吸附能和吸附热的差异可以作为区分mof内强弱吸附位点分布的指标。为合理设计适合不同分离要求的MOFs提供了明确的结构-性能相关原则和选择指导。

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引用次数: 0

Two-dimensional InAs/GaSb van der Waals heterostructures: interface engineering and infrared optoelectronic properties 二维InAs/GaSb范德华异质结构：界面工程和红外光电特性

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-03-03 DOI: 10.1016/j.commatsci.2026.114595

Guowang Yu , Xiaoning Guan , Yanan Zhang , Yaqi Zhao , Yanchao Zhang , Fan Zhang , Feng Zhou , Pengfei Lu

Two-dimensional InAs/GaSb van der Waals (vdW) heterostructures are of interest for infrared optoelectronic applications, yet the role of interface geometry in determining their stability and electronic properties remains insufficiently clarified. Here, density functional theory (DFT) calculations, as implemented in the Vienna Ab initio Simulation Package (VASP), are carried out for 24 bilayer stacking models with distinct lateral registries. By optimizing the interlayer separation and evaluating formation and binding energies, we identify a subset of thermodynamically stable configurations that remain bound within a characteristic vdW separation window. Hybrid-functional band-structure calculations using the Heyd–Scuseria–Ernzerhof screened hybrid functional (HSE06) reveal pronounced stacking dependence, including semiconducting and metallic cases, and indicate that most semiconducting stackings exhibit type-II band alignment with spatially separated band edges. By jointly considering band-gap magnitude and band alignment, four representative mid-infrared candidates with HSE06 band gaps of 0.1–0.5 eV are selected. The calculated optical-absorption spectra show a clear enhancement in the infrared; for the BB1 stacking, the absorption coefficient remains on the order of 10⁵ cm⁻¹ from the near- to mid-infrared (1–5 μm) and stays appreciable up to about 6 μm, relative to the isolated InAs and GaSb monolayers under the same slab-based computational definition of the absorption coefficient. The present results provide microscopic insight into stacking-dependent stability and electronic structure, and offer practical guidance for interface-stacking selection and first-principles screening of InAs/GaSb and related type-II vdW heterostructures.

二维InAs/GaSb范德华（vdW）异质结构对红外光电应用很有兴趣，但界面几何形状在决定其稳定性和电子性能方面的作用仍然不够明确。在这里，密度泛函理论（DFT）计算，在维也纳从头算模拟包（VASP）中实现，对24个具有不同横向注册的双层叠加模型进行了计算。通过优化层间分离和评估形成能和结合能，我们确定了一个在特征vdW分离窗口内保持结合的热力学稳定构型子集。使用Heyd-Scuseria-Ernzerhof筛选的杂化功能（HSE06）进行的杂化功能带结构计算显示了明显的堆叠依赖性，包括半导体和金属情况，并表明大多数半导体堆叠表现为ii型带排列，带边缘空间分离。通过综合考虑带隙大小和带向，选择了4个具有代表性的中红外候选物，HSE06带隙在0.1 ~ 0.5 eV之间。计算得到的光吸收光谱在红外波段有明显的增强；在相同的板基吸收系数计算定义下，相对于孤立的InAs和GaSb单层，BB1层的吸收系数在近红外到中红外（1 - 5 μm）范围内保持在105 cm−1左右，在6 μm范围内保持可观。本研究结果提供了对层叠依赖稳定性和电子结构的微观洞察，并为InAs/GaSb和相关ii型vdW异质结构的界面层叠选择和第一性原理筛选提供了实用指导。

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引用次数: 0

Stable HCP high-entropy alloys identified by knowledge-based screening and valence electron concentration criteria 利用知识筛选和价电子浓度标准鉴定稳定的HCP高熵合金

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-26 DOI: 10.1016/j.commatsci.2026.114584

Hiroshi Mizuseki , Ryoji Sahara , Kenta Hongo

Although extensive research has been conducted on High-Entropy Alloys (HEAs) with face-centered cubic (FCC) and body-centered cubic (BCC) structures, the formation conditions and stability of HEAs with hexagonal close-packed (HCP) structures remain less explored compared to their cubic counterparts. Comprehensive exploration of HEAs requires efficient and reliable methods to assess structural stability across a vast compositional space comprising multiple metallic elements. In this study, we investigated 40,920 equimolar quaternary alloys, generated by selecting arbitrary combinations of four elements from a pool of 33. Metallurgical screening was performed based on criteria including atomic radius and electronegativity differences among constituent elements, enthalpy–entropy competition, and mixing enthalpy calculated using the semi-empirical Miedema model. This screening identified 1005 compositions with the potential to form random solid solutions (RSS). For these candidates, first-principles calculations were conducted to evaluate the RSS formation energies for FCC, BCC, and HCP structures, thereby determining the most stable crystal structure for each composition. The results revealed a clear correlation between valence electron concentration (VEC) and the distribution of crystal structures. Notably, HCP structures were frequently observed not only in the intermediate VEC range between those favoring BCC and FCC, but also in low-VEC regions around 3 and high-VEC regions exceeding 10. This trend closely mirrors the VEC-dependent structural preferences of individual 4d and 5d transition metals, suggesting that the intrinsic crystal structures of constituent elements may be preserved in HEAs. Our findings provide a systematic dataset of HCP stability within the VEC framework and offer a baseline for the development of multicomponent alloys.

虽然对具有面心立方（FCC）和体心立方（BCC）结构的高熵合金（HEAs）进行了广泛的研究，但与具有立方结构的高熵合金相比，具有六方密堆积（HCP）结构的高熵合金（HEAs）的形成条件和稳定性研究较少。对HEAs的全面探索需要高效可靠的方法来评估由多种金属元素组成的巨大组成空间的结构稳定性。在这项研究中，我们研究了40,920种等摩尔季元合金，这些合金是从33种元素中任意选择四种元素的组合产生的。冶金筛选的标准包括原子半径和组成元素之间的电负性差异、焓-熵竞争以及使用半经验Miedema模型计算的混合焓。该筛选确定了1005种具有形成随机固溶体（RSS）潜力的组合物。对于这些候选化合物，采用第一性原理计算来评估FCC、BCC和HCP结构的RSS形成能，从而确定每种成分最稳定的晶体结构。结果表明，价电子浓度（VEC）与晶体结构的分布有明显的相关性。值得注意的是，HCP结构不仅在有利于BCC和FCC的中间VEC范围内，而且在VEC约为3的低VEC区域和VEC超过10的高VEC区域也经常出现。这一趋势密切反映了单个4d和5d过渡金属的vecc依赖结构偏好，表明组成元素的固有晶体结构可能在HEAs中被保留。我们的研究结果提供了VEC框架内HCP稳定性的系统数据集，并为多组分合金的开发提供了基线。

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引用次数: 0

The role of electron-phonon interactions on the electrical transport properties of metal interconnects 电子-声子相互作用对金属互连电输运性质的影响

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-27 DOI: 10.1016/j.commatsci.2026.114605

Shumin Yan , Ruiling Gao , Shunbo Hu , Runhai Ouyang , Yin Wang

The performance of integrated circuits critically depends on the electrical transport properties of metal interconnect. In this work, we employed the Büttiker probe model and interpretable machine learning to investigate the influence of electron-phonon interactions on the electrical transport properties of metal interconnect. The NEGF-DFT method was utilized to investigate the relationship between the transport properties and the intensity of electron-phonon coupling in the six metals: Ag, Cu, Al, Rh, Ru, and Ir. Results show that as the coupling strength γ increases, the transmission coefficient, current density, and conductance of all metal systems exhibit a decreasing trend. Additionally, we found the presence of vacancy defects leads to a more pronounced reduction of conductance in all systems. To find the quantitative relationship between the electron-phonon interactions and the conductance of the metal interconnect systems, symbolic regression was performed using the SISSO method. An accurate formula was obtained and it reveals that the conductance decreases linearly with increasing electron-phonon coupling constant and temperature. This work provides valuable insights to the influence of electron-phonon interactions on the electrical transport properties of metal interconnects in integrated circuits, and helps reveal how microscopic scattering processes shape the macroscopic transport behavior of interconnect materials.

集成电路的性能在很大程度上取决于金属互连的电输运特性。在这项工作中，我们采用 ttiker探针模型和可解释机器学习来研究电子-声子相互作用对金属互连电输运性质的影响。利用NEGF-DFT方法研究了Ag、Cu、Al、Rh、Ru和Ir六种金属的输运性质与电子-声子耦合强度之间的关系。结果表明：随着耦合强度γ的增大，各金属体系的透射系数、电流密度和电导均呈减小趋势；此外，我们发现空缺缺陷的存在导致所有系统的电导更明显的降低。为了找到电子-声子相互作用与金属互连系统电导之间的定量关系，使用SISSO方法进行了符号回归。结果表明，电导随温度和电子-声子耦合常数的增加而线性减小。这项工作为电子-声子相互作用对集成电路中金属互连电输运特性的影响提供了有价值的见解，并有助于揭示微观散射过程如何塑造互连材料的宏观输运行为。

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引用次数: 0

Layer-locked anomalous valley hall effect in two-dimensional tetragonal trilayers with electrically controllable valley and spin polarizations 具有可控谷极化和自旋极化的二维四边形三层中锁层的反常谷霍尔效应

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-10 DOI: 10.1016/j.commatsci.2026.114570

Bo Chen , Jian Liu , Lin Xue , Zhi Yang , Yong-Jia Zhang

Two-dimensional (2D) multilayer materials with coupled valley, spin, and layer degrees of freedom enable concurrent electrical control of valley and spin polarizations. However, realizing valley-spin-layer coupling (VSLC) in 2D materials remains challenging due to the stringent symmetry requirements. In this work, we show that the VSLC trilayers can be constructed by assembling non-VSLC monolayers, as demonstrated by density functional theory calculations on tetragonal Fe₂I₂/Na₂Cl₂/Fe₂I₂ and V₂Se₂O/Na₂Cl₂/V₂Se₂O trilayer van der Waals heterostructures, as well as a V₂Se₂O trilayer. Furthermore, on the basis of valley-layer coupling, nonzero Berry curvature, and spin splitting, anomalous valley Hall effect (AVHE) and layer-locked AVHE can be achieved in these systems after electron doping and the application of a longitudinal in-plane electric field. Our work proposes a feasible way to build 2D VSLC materials for spin-valleytronic applications and provides a platform for realizing the AVHE and layer-locked AVHE.

二维（2D）多层材料具有耦合的谷、自旋和层自由度，可以同时控制谷和自旋极化。然而，由于具有严格的对称性要求，在二维材料中实现谷-自旋层耦合（VSLC）仍然具有挑战性。通过对Fe2I2/Na2Cl2/Fe2I2和V2Se2O/Na2Cl2/V2Se2O三层van der Waals异质结构以及V2Se2O三层的密度泛函理论计算，我们证明了VSLC三层可以通过组装非VSLC单层来构建。此外，在谷层耦合、非零Berry曲率和自旋分裂的基础上，通过电子掺杂和纵向面内电场的作用，可以在这些体系中实现反常谷霍尔效应（AVHE）和锁层AVHE。我们的工作提出了一种可行的方法来构建自旋谷电子应用的二维VSLC材料，并为实现AVHE和锁层AVHE提供了一个平台。

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引用次数: 0

Synergistic effects of Re and C/O on grain boundary strength in Mo by first-principles calculation 第一性原理计算稀土和碳氧比对Mo晶界强度的协同效应

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-16 DOI: 10.1016/j.commatsci.2026.114563

Cai-Fu Pan , Dong-Jie Wang , Wen-Lue Mao , Li-Xia Jia , Yan-Kun Dou , Jin-Li Cao , Xin-Fu He , Wen Yang

Elements segregation can significantly affect grain boundary (GB) strength, altering the thermal stability and mechanical properties of materials. In this work, we systematically investigate the synergistic effects between solute rhenium (Re) and interstitial carbon and oxygen (C and O) atoms at molybdenum (Mo) GBs and their influence on GB strength through first-principles calculations. Our results demonstrate that both C and Re segregation enhances GB strength, while O segregation significantly deteriorates interfacial cohesion. The co-segregation and co-strengthening energies of ReC and ReO are found to be lower than the sum of their individual values, indicating their repulsive interactions. Notably, ReC co-segregation leads to further GB strengthening, while ReO co-segregation effectively alleviates oxygen-induced embrittlement. Electronic structure analysis reveals that the chemical interactions dominate the repulsive behavior: ReC repulsion originates from direct antibonding states, whereas ReO repulsion is primarily caused by the breaking of MoO bonds. Furthermore, the formation of MoC and MoRe bonds enhances GB cohesion, while oxygen induces the weakening of MoMo metallic bonds. This work provides fundamental understanding of solute-interstitial interactions at atomic scale and offers valuable insights for designing high-performance refractory alloys.

元素偏析会显著影响材料的晶界强度，改变材料的热稳定性和力学性能。在这项工作中，我们通过第一性原理计算系统地研究了钼（Mo） GB中溶质铼（Re）与间隙碳和氧（C和O）原子之间的协同效应及其对GB强度的影响。结果表明，C和Re的偏析均能提高GB的强度，而O的偏析则会显著降低界面的内聚性。ReC和ReO的共偏析和共强化能小于它们各自值的和，表明它们之间存在排斥作用。值得注意的是，ReC共偏析导致了GB的进一步强化，而ReO共偏析则有效地缓解了氧致脆。电子结构分析表明，化学相互作用主导了斥力行为：ReC斥力来源于直接反键状态，而ReO斥力主要是由MoO键断裂引起的。MoC和MoRe键的形成增强了GB的内聚力，而氧导致MoMo金属键的减弱。这项工作提供了在原子尺度上溶质-间隙相互作用的基本理解，并为设计高性能耐火合金提供了有价值的见解。

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引用次数: 0

A computational framework for tracking grain boundaries in 3D image data: Quantifying boundary curvatures and velocities in polycrystalline materials 三维图像数据中跟踪晶界的计算框架：多晶材料中边界曲率和速度的量化

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-09 DOI: 10.1016/j.commatsci.2026.114541

Thomas Wilhelm , Orkun Furat , Jules M. Dake , Carl E. Krill III , Volker Schmidt

Diffraction-based methods for 3D microstructure mapping have revolutionized the investigation of grain growth phenomena in polycrystalline materials. These techniques provide unprecedented experimental access to the location, shape and migration of individual grain boundaries in real samples, together with other relevant boundary parameters, such as misorientation and inclination. However, achieving the ultimate goal of such studies — the identification of physical mechanisms responsible for the observed evolution of microstructure — is impeded by the voxel-based representation of microstructure intrinsic to 3D mapping. The staircase-like discretization of grain boundaries complicates the determination of boundary positions and local curvatures, motivating a transition from a discrete to a continuous representation of the boundary network. This paper introduces an approach based on smoothing thin-plate splines with radial basis functions to represent grain boundaries as continuous surfaces. The method can approximate arbitrarily shaped boundaries while preserving local mean curvatures and, for time-resolved series of images, local boundary velocities. Its accuracy is validated against two datasets: a multiplicatively weighted Laguerre tessellation, where mean curvatures are known analytically, and a Reuleaux tetrahedron evolving under a phase field model, for which local boundary velocities can be determined exactly. The applicability of the method to experimental data is demonstrated using time-resolved 3D maps of grain growth in an Al–Mg alloy.

基于衍射的三维微观结构映射方法已经彻底改变了多晶材料中晶粒生长现象的研究。这些技术提供了前所未有的实验途径来研究真实样品中单个晶界的位置、形状和迁移，以及其他相关的边界参数，如取向偏差和倾角。然而，实现这些研究的最终目标-确定负责观察到的微观结构演变的物理机制-受到三维映射固有的基于体素的微观结构表示的阻碍。晶界的阶梯状离散化使边界位置和局部曲率的确定变得复杂，促使边界网络从离散表示过渡到连续表示。本文介绍了一种基于光滑薄板样条径向基函数的连续晶界表示方法。该方法可以近似任意形状的边界，同时保留局部平均曲率，对于时间分辨的图像序列，保留局部边界速度。它的准确性是通过两个数据集验证的：一个乘法加权拉盖尔镶嵌，其中平均曲率是解析已知的，以及一个在相场模型下进化的勒洛四面体，其局部边界速度可以精确确定。用Al-Mg合金晶粒生长的三维时间分辨图证明了该方法对实验数据的适用性。

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引用次数: 0

Enhancement mechanisms of thermoelectric performance of 2D structures influenced by van der Waals interaction 范德华相互作用对二维结构热电性能增强机制的影响

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-09 DOI: 10.1016/j.commatsci.2026.114557

Eyasu Tadese M. , T.E. Ada , K.N. Nigussa , Cecil N.M. Ouma

Ab initio calculations with the GPAW code were used to analyze the structural, electrical, excitonic, and thermoelectric properties of various bilayer transition metal dichalcogenides. Our work reveals that exciton binding energy plays a decisive role in mechanical strength, carrier separation, electron concentration, carrier conductivity, and van der Waals interactions, thereby giving rise to bipolar, ambipolar, and ohmic-heating effects. The thermoelectric performance of 2H-WS

_{2}

-WSe

_{2}

was found to be most significant, at stable carrier concentration of

\sim 2.1 \times 1 0^{20} {cm}^{3}

near electron–hole symmetry with a peak power factor of

{0.74 mWm}^{- 1} K^{- 2}

, and Seebeck coefficient exceeding

550 μ {VK}^{- 1}

under

n

-type doping, at

800 K

, where the electronic thermal conductivity contributes more than

50%

to the thermoelectric figure of merit. A precise tuning of exciton binding energy along with optimal stacking configurations is critical for utmost enhancement of thermoelectric figure of merit. The outcomes of studies on the selected bilayers shows characteristics that may be suitable for applications in industrial waste heat recovery, automotive exhaust energy harvesting, and power generation in remote environments.

利用GPAW程序进行从头计算，分析了各种双层过渡金属二硫族化合物的结构、电学、激子和热电性质。我们的工作表明，激子结合能在机械强度、载流子分离、电子浓度、载流子电导率和范德华相互作用中起决定性作用，从而产生双极、双极和欧姆加热效应。研究发现，在载流子浓度为~ 2.1×1020cm3时，在电子-空穴对称附近，2H-WS2-WSe2的热电性能最为显著，峰值功率因数为0.74 mWm−1K−2，n型掺杂下的塞贝克系数超过550μVK−1，在800 K时，电子导热系数对热电性能的贡献超过50%。激子结合能的精确调谐以及最佳的堆叠结构是最大限度地提高热电性能的关键。对所选双层材料的研究结果表明，其特性可能适用于工业废热回收、汽车尾气能量收集和偏远环境发电。

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引用次数: 0

Revisiting phonon thermal transport in penta-graphene via a machine-learning potential-driven large-scale molecular dynamics simulation 通过机器学习势能驱动的大规模分子动力学模拟重访五石墨烯中的声子热输运

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-02-25 DOI: 10.1016/j.commatsci.2026.114606

Junwei Che , Xuezhi Wang

Two-dimensional penta-graphene (PG) has emerged as a promising material for electronic, nanoelectromechanical, and energy-related applications, where the lattice thermal conductivity (κ_L) plays a critical role in device performance and reliability. However, reported κ_L values for PG vary significantly in the literature. In this work, we determine the intrinsic κ_L of PG and elucidate the underlying microscopic phonon transport mechanisms using large-scale molecular dynamics simulations enabled by a machine-learning potential. For PG with an effective thickness of 4.6 Å, the intrinsic κ_L is found to decrease from 505 to 94 Wm⁻¹ K⁻¹ over the temperature range of 200–1000 K, following a κ_L ∼ T^-0.92 scaling behavior. Mode-resolved phonon analysis reveals that heat transport in PG is dominated by low- and mid-frequency phonon modes below 22 THz. Notably, the contribution of low-frequency phonons below 10 THz remains weakly affected by temperature due to their large group velocities and long lifetimes. In contrast, increasing temperature significantly suppresses the contribution of high-frequency phonons above 22 THz as a result of enhanced anharmonic scattering, leading to the pronounced temperature dependence of κ_L. This work reconciles disparities among previous κ_L predictions for PG and establishes a key foundation for the thermal management of PG-based technologies.

二维五石墨烯（PG）已成为电子、纳米机电和能源相关应用的一种有前途的材料，其中晶格热导率（κL）在器件性能和可靠性中起着关键作用。然而，文献中报道的PG的κL值差异很大。在这项工作中，我们确定了PG的内在κL，并利用机器学习潜力实现的大规模分子动力学模拟阐明了潜在的微观声子传输机制。对于有效厚度为4.6 Å的PG，在200-1000 K的温度范围内，其本征κL从505下降到94 Wm−1 K−1，表现出κL ~ T-0.92的标化行为。模式分辨声子分析表明，PG中的热输运主要由低于22太赫兹的低频和中频声子模式主导。值得注意的是，低于10太赫兹的低频声子的贡献受温度的影响很小，因为它们的群速度大，寿命长。相反，温度升高显著抑制了22thz以上高频声子的贡献，这是由于非谐波散射增强，导致κL的温度依赖性明显。这项工作调和了先前对PG的κL预测之间的差异，并为基于PG的技术的热管理奠定了关键基础。

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引用次数: 0

A comprehensive DFT–QTAIM study on Mg–H interactions in MgH2 crystal MgH2晶体中Mg-H相互作用的DFT-QTAIM综合研究

IF 3.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Computational Materials Science

Pub Date : 2026-03-10 Epub Date: 2026-03-03 DOI: 10.1016/j.commatsci.2026.114627

Lei Bao , Jun Shi

This study systematically investigates the Mg–H interactions in MgH

_{2}

crystal by combining Density Functional Theory (DFT) and the Quantum Theory of Atoms in Molecules (QTAIM). Crystallographic analysis reveals characteristic structural units: the Mg

_{6}

H

_{2}

octahedra and Mg

_{4}

tetrahedra, and their face-sharing and edge-sharing connectivity. The H atom has been found to be triple coordinated with the three nearest Mg atoms, forming an isosceles triangular configuration. Topological examination of the all-electron density distribution confirms that the Mg–H bond is predominantly ionic (with 82% charge transfer) and follows a closed-shell interaction. An energetic evaluation of the Mg–H bond yielded a dissociation energy of 1.6127 eV, indicating a relatively weak ionic bond. This work provides atomic-level insights into the microscopic characteristics governing MgH

_{2}

’s hydrogen storage performance, which encompass both thermodynamic stability and kinetics. These insights offer a theoretical basis for designing improved MgH

_{2}

-based materials.

本研究结合密度泛函理论（DFT）和分子原子量子理论（QTAIM）系统地研究了MgH2晶体中Mg-H相互作用。晶体学分析揭示了其特征结构单元：Mg6H2八面体和Mg4四面体，以及它们的面共享和边共享连接。H原子已被发现与最近的三个Mg原子三配位，形成等腰三角形构型。全电子密度分布的拓扑检查证实，Mg-H键主要是离子键（82%的电荷转移），并遵循封闭壳层相互作用。对Mg-H键进行能量评价，得到离解能为1.6127 eV，表明其离子键相对较弱。这项工作为控制MgH2储氢性能的微观特征提供了原子水平的见解，包括热力学稳定性和动力学。这些见解为设计改进的mgh2基材料提供了理论基础。

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引用次数: 0