AI 中文总结
研究针对二维材料用于高效光电子学的问题，通过第一性原理计算筛选WS₂/ZnO异质结构，分析其面依赖电子性质与界面缺陷相互作用，确定最佳衬底面，明确不同缺陷影响，为二维/三维混合发光二极管的衬底选择和缺陷工程提供微观框架。
AI 中文摘要
针对用于高效光电子学的二维材料，使用第一性原理混合泛函计算对WS₂/ZnO异质结构的面依赖电子性质和界面缺陷热力学进行了计算筛选。界面比较确定非极性(1010)m面为最佳衬底面，保持2.42 eV的直接带隙和稳健的I型能带排列。孤立的硫（VS）和界面氧（VO）空位会引入深非辐射复合中心。锌空位（VZn）在价带边缘附近充当浅受主，导致无意的p型行为。缺陷对分析表明，由于有利的结合能，中性空位在范德华间隙中聚集。在n型条件下，缺陷稳定为带电物种。虽然层间库仑排斥削弱了(VS - VZn)''对的结合能，但在贫阴离子条件下它们的形成能降至2.61 eV，使-4簇成为界面上热力学上最丰富的缺陷对。此外，原生VZn可防止通常由间隙氢（Hi）引起的费米能级上升，将捐赠电子分布到浅受主状态并保持主体带边刚性。这些发现为二维/三维混合发光二极管中的衬底选择和缺陷工程建立了微观框架。
英文摘要
Aiming at two-dimensional materials for high-efficiency optoelectronics, WS$2$/ZnO heterostructures are computationally screened for their facet-dependent electronic properties and interfacial defect thermodynamics using first-principles hybrid functional calculations. Interface comparison identifies the non-polar ($10\overline{1}0$) $m$-plane as the optimal substrate facet, maintaining a direct 2.42~eV bandgap and a robust type-I band alignment. Isolated sulfur ($\mathrm{V_S}$) and interfacial oxygen ($\mathrm{V_O}$) vacancies introduce deep non-radiative recombination centers. Conversely, zinc vacancies ($\mathrm{V{Zn}}$) act as shallow acceptors near the valence band edge, contributing to unintentional $p$-type behavior. Analysis of defect pairs reveals that neutral vacancies cluster across the van der Waals gap due to favorable binding energies. Under $n$-type conditions, defects stabilize as charged species. Although inter-layer Coulomb repulsion weakens the binding energy of $(\mathrm{V_S} - \mathrm{V_{Zn}})''''$ pairs, their formation energy drops to 2.61~eV under anion-poor conditions, making the $-4$ cluster the most thermodynamically abundant defect pair at the interface. Furthermore, native $\mathrm{V_{Zn}}$ prevents the Fermi level rise typically induced by interstitial hydrogen ($\mathrm{H_i}$), distributing donated electrons into shallow acceptor states and preserving host band edge rigidity. These findings establish a microscopic framework for substrate selection and defect engineering in 2D/3D hybrid light-emitting diodes.
Comments10 pages, 24 figures
