The rational control of the nucleation and growth kinetics to enable the high-quality growth of two-dimensional (2D) semiconducting metal chalcogenide heterostructures is a key step for the realization of their applications in nanoelectronics and optoelectronics. Here, we report a facile one-step chemical vapor deposition synthesis of 2D SnS–SnS₂ heterostructures with controlled interfacial structures and stacking configurations via tuning S-precursor concentration during the growth. We demonstrate that the change of S-precursor concentration can drive growth transition from vertically stacking SnS₂/SnS van der Waals heterostructures to SnS/SnS₂ core–shell structures with both the lateral and vertical interfaces. Such a transition originates from a delicate competition between the nucleation of SnS and SnS₂. High-resolution spectroscopy measurements and density functional theory (DFT) calculations reveal these SnS–SnS₂ heterostructures with the type-II band alignment, and the measured valence and conduction band offsets are 1.33 and 0.34 eV for vertical SnS₂/SnS heterostructures and 1.43 and 0.54 eV for SnS/SnS₂ core–shell ones, respectively. This work provides an efficient strategy to control the growth of 2D SnS–SnS₂ heterostructures for optoelectronic applications, such as photodetectors and solar cells.

中文翻译：

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硫驱动的二维SnS–SnS ₂异质结构及其能带排列从垂直生长到横向生长

合理控制成核和生长动力学，以实现二维（2D）半导体金属硫族化物异质结构的高质量生长，是实现其在纳米电子学和光电子学中应用的关键一步。在这里，我们报告了通过控制生长过程中S的前体浓度，实现了2D SnS–SnS ₂异质结构的简便一步化学气相沉积合成，该结构具有受控的界面结构和堆叠构型。我们证明，S前体浓度的变化可以驱动生长从垂直堆叠的SnS ₂ / SnS van der Waals异质结构向SnS / SnS _2的转变具有横向和纵向界面的核壳结构。这种转变源自SnS和SnS ₂的成核之间的微妙竞争。高分辨率光谱测量和密度泛函理论（DFT）计算揭示了这些II型带对准的SnS–SnS ₂异质结构，垂直SnS ₂ / SnS异质结构的化合价和导带偏移为1.33和0.34 eV ，1.43 SnS / SnS ₂核-壳型分别为0.54 eV和。这项工作为控制光电检测器和太阳能电池等光电应用中2D SnS–SnS ₂异质结构的生长提供了有效的策略。