Electronic Properties and Carrier Dynamics at the Alloy Interfaces of WS_2xSe_2−2x Spiral Nanosheets

Abstract Electronic properties at the interfaces between different‐composition domains of 2D‐alloys are key for their optical, electronic, and optoelectronic applications. Understanding the interfacial electronic structures and carrier dynamics is essential for designing and fabricating devices that use these alloys. Here, WS_2xSe_2−2x spiral nanosheets are prepared using the physical vapor deposition method, and the nonlinear optical and electronic properties, as well as the carrier dynamics at the interfaces between the WS and WSe domains, are studied. Second‐harmonic generation tests demonstrate that these nanosheets exhibit a very strong layer‐dependent nonlinear optical effect. Atomic‐resolution scanning tunneling microscopy (STM) and spectroscopy (STS) measurements reveal that S and Se atoms are non‐uniformly distributed, forming WS domains, WSe domains, and defect‐related areas. Atomic STM images and STS maps reveal enhanced local density of states by electron scattering at the WS/WSe interfaces, providing a detailed nanoscale interpretation of the S/Se‐ratio‐dependent lifetimes observed in pump–probe spectroscopy measurements. This work provides valuable interfacial characterization of 2D‐alloy materials, using state‐of‐the‐art methods with high temporal and spatial resolutions. The obtained insights are likely to be useful for prospective applications.