二维半导体中钒掺杂和硫空位行为的理解和控制:走向预测设计

IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ACS Nano Pub Date : 2025-09-19 DOI:10.1021/acsnano.5c10856
Shreya Mathela, , , Zhuohang Yu, , , Zachary D. Ward, , , Nikalabh Dihingia, , , Alex Sredenschek, , , David Sanchez, , , Kyle T. Munson, , , Elizabeth Houser, , , Edgar Dimitrov, , , Arpit Jain, , , Danielle Reifsnyder Hickey, , , Humberto Terrones*, , , Mauricio Terrones*, , and , John B. Asbury*, 
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引用次数: 0

摘要

在过渡金属二硫化物(TMD)单层中掺杂提供了一种强大的方法来精确定制其电子,光学和催化性能,用于先进的技术应用,包括光电子学,催化和量子技术。然而,这些材料的掺杂效率和结果受到引入掺杂剂与本征缺陷(特别是硫空位)之间复杂相互作用的强烈影响。掺杂剂和缺陷之间的耦合可以导致明显不同的行为,这对TMD性能的可预测和可控设计提出了重大挑战。例如,在这项工作中,我们系统地改变了二硫化钨(WS2)单层中的p型钒(V)掺杂密度,并观察到掺杂行为的转变。在低浓度下,v掺杂剂增强了WS2的固有光学性质,这可以通过增加光致发光来证明,而不会引入新的电子态。然而,在较高浓度下,v掺杂剂促进钒-硫空位配合物的形成,产生中隙态,其能量可以通过控制钒浓度来精确调节。利用激发和温度依赖的光致发光显微镜,原子分辨率扫描透射电子显微镜和第一性原理计算的组合,我们确定了p型v掺杂剂和n型单硫空位之间的吸引相互作用。我们的研究结果提供了焓掺杂缺陷相互作用与熵效应如何控制tmd性能增强和扰动之间平衡的机制理解,并为下一代光电、催化和量子器件的掺杂策略的合理设计提供了途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Understanding and Controlling Vanadium Doping and Sulfur Vacancy Behavior in Two-Dimensional Semiconductors: Toward Predictive Design

Understanding and Controlling Vanadium Doping and Sulfur Vacancy Behavior in Two-Dimensional Semiconductors: Toward Predictive Design

Understanding and Controlling Vanadium Doping and Sulfur Vacancy Behavior in Two-Dimensional Semiconductors: Toward Predictive Design

Doping in transition-metal dichalcogenide (TMD) monolayers provides a powerful method to precisely tailor their electronic, optical, and catalytic properties for advanced technological applications, including optoelectronics, catalysis, and quantum technologies. However, the doping efficiency and outcomes in these materials are strongly influenced by the complex interactions between introduced dopants and intrinsic defects, particularly sulfur vacancies. This coupling between dopants and defects can lead to distinctly different behaviors depending on the doping concentration, presenting significant challenges in the predictable and controlled design of TMD properties. For example, in this work we systematically varied the p-type vanadium(V) doping density in tungsten disulfide (WS2) monolayers and observed a transition in doping behavior. At low concentrations, V-dopants enhance the native optical properties of WS2, as evidenced by increased photoluminescence, without introducing new electronic states. However, at higher concentrations, V-dopants promote the formation of vanadium–sulfur vacancy complexes that generate midgap states, with energies that can be precisely tuned by controlling the vanadium concentration. Using a combination of excitation- and temperature-dependent photoluminescence microscopy, atomic-resolution scanning transmission electron microscopy, and first-principles calculations, we identify attractive interactions between p-type V-dopants and n-type monosulfur vacancies. Our results provide a mechanistic understanding of how enthalpic dopant–defect interactions versus entropic effects govern the balance between property enhancement and perturbation of TMDs and suggest a pathway toward the rational design of doping strategies for next-generation optoelectronic, catalytic, and quantum devices.

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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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