发表机构
Technical University of Denmark（丹麦技术大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
提出无校准的拓扑-谱渗流描述符（TSPD），从静态晶体结构快速确定离子传输机制，经八种材料验证，能正确识别路径受限传输。
AI 中文摘要
离子传输控制着固态电解质、电池电极、离子选择性膜、电解陶瓷、混合导体、多孔吸附剂和生物通道的宏观性能。在每种情况下，离子传输由结构特征决定，即可利用的扩散路径和限制离子跳跃的特定瓶颈原子。这些是晶体框架的固有属性，而温度、载流子浓度和关联运动则控制传输速率。从头算分子动力学（AIMD）直接解析机制，但对于材料筛选而言成本过高，且大多数替代模型仅给出单一传输数。这里我们提出一种基于拓扑-谱渗流描述符（TSPD）的无校准机制确定方法。TSPD在数秒内从单个静态结构获得传输机制。它构建周期性迁移网络，其边势垒由基于物理的能量学计算得出。然后我们分析该网络的势垒阈值拓扑及其势垒加权图拉普拉斯谱。为验证其在计算固态离子学中的有效性，我们针对八种材料（包括阴极和固态电解质，其传输维度从一维到三维）将TSPD与AIMD离子密度和中子衍射数据进行比较。TSPD在每种情况下均重现已确立的机制，并正确识别出几何开放性并不意味着可行离子渗流的结构。该方法对于路径受限、方向依赖的传输最具信息量，并补充了针对强协同或近各向同性传输的完整动力学模拟。
英文摘要
Ion transport controls the macroscopic performance of solid electrolytes, battery electrodes, ion-selective membranes, electrolysis ceramics, mixed conductors, porous sorbents, and biological channels. In each case, ion transport is determined by structural characteristics, namely the available diffusion pathways and the specific bottleneck atoms that limit the ionic jumps. These are intrinsic properties of the crystalline framework, whereas temperature, carrier concentration, and correlated motion govern the transport rate. Ab initio molecular dynamics (AIMD) resolves the mechanism directly but is too costly for materials screening, and most surrogate models give only a single transport number. Here we present a calibration-free method for determining the mechanism, based on Topo-Spectral Percolation Descriptors (TSPD). TSPD obtains the transport mechanism from a single static structure in seconds. It constructs a periodic migration network whose edge barriers are computed from physics-based energetics. We then analyze the barrier-threshold topology of this network and the spectrum of its barrier-weighted graph Laplacian. To establish its validity for computational solid-state ionics, we test TSPD against AIMD ion densities and neutron diffraction data for eight materials, including cathodes and solid electrolytes, whose transport ranges from one- to three-dimensional. TSPD reproduces the established mechanism in every case and correctly identifies structures in which geometric openness does not imply viable ion percolation. The method is most informative for pathway-limited, direction-dependent transport, and it complements full dynamical simulations for strongly cooperative or nearly isotropic transport.
