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Significance Defects in two-dimensional (2D) transition-metal dichalcogenides play a crucial role in controlling the spatiotemporal dynamics of photogenerated charge carriers, which remain poorly understood to date. In this paper, the defect-mediated carrier diffusion and recombination in WS2monolayers are quantitatively investigated by laser-illuminated microwave impedance microscopy. Surprisingly, the photoresponse is in general stronger in the more disordered regions and samples. Such counterintuitive observations are reconciled by spatiotemporally resolved experiments, which indicate that the electron lifetime is prolonged due to the slow release of holes from the trap states. The results reveal the intrinsic time and length scales of photocarriers in van der Waals materials, providing the guidance for implementing nanooptoelectronic devices based on 2D semiconductors.more » « less
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Abstract Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in‐plane ferroelectric material that exhibits a giant nonlinear optical effect, group‐IV monochalcogenide SnSe, is reported. Nanometer‐scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical‐vapor‐deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second‐harmonic fields and the as‐resulted second‐harmonic generation was observed to be 100 times more intense than monolayer WS2. This work demonstrates in‐plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on‐chip nonlinear optical components and nonvolatile memory devices.more » « less
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Abstract 2D transition metal dichalcogenide (TMD) layered materials are promising for future electronic and optoelectronic applications. The realization of large‐area electronics and circuits strongly relies on wafer‐scale, selective growth of quality 2D TMDs. Here, a scalable method, namely, metal‐guided selective growth (MGSG), is reported. The success of control over the transition‐metal‐precursor vapor pressure, the first concurrent growth of two dissimilar monolayer TMDs, is demonstrated in conjunction with lateral or vertical TMD heterojunctions at precisely desired locations over the entire wafer in a single chemical vapor deposition (VCD) process. Owing to the location selectivity, MGSG allows the growth of p‐ and n‐type TMDs with spatial homogeneity and uniform electrical performance for circuit applications. As a demonstration, the first bottom‐up complementary metal‐oxide‐semiconductor inverter based on p‐type WSe2and n‐type MoSe2is achieved, which exhibits a high and reproducible voltage gain of 23 with little dependence on position.more » « less
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