Selective Oxidation of WS2 Defect Domain with Sub‐Monolayer Thickness Leads to Multifold Enhancement in Photoluminescence,Advanced Materials Interfaces

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Selective Oxidation of WS2 Defect Domain with Sub‐Monolayer Thickness Leads to Multifold Enhancement in Photoluminescence
Advanced Materials Interfaces ( IF 4.3 ) Pub Date : 2019-08-27 , DOI: 10.1002/admi.201900962
Pawan Kumar _{1,

2} , Jayeeta Biswas ₃ , Juhi Pandey ₄ , Kartikey Thakar ₃ , Ajay Soni ₄ , Saurabh Lodha ₃ , Viswanath Balakrishnan ₁

Affiliation

Stabilizing defective domains of sub‐monolayer thickness in 2D materials plays a significant role in tuning the electronic and optical properties. The chemical vapor deposition growth of WS₂ monolayers with control over phase and uniformly nucleated defect domains is reported. Multifold photoluminescence (PL) enhancement (≈20‐fold) is achieved by stabilizing defect‐dominated domains toward design of nanoscale optical devices. While the observed luminescence variation in the form of alternating triangles arises from planar heterostructure (1H–1T′) formation, defect domain present at the center of WS₂ heterophase monolayer causes 20‐fold enhancement in photoluminescence. The observed luminescence enhancement is correlated with sulfur defects and confirmed by site‐specific spatial X‐ray photoemission spectroscopy and in situ PL measurements at cryogenic temperatures. Detailed microstructural and spectroscopic observations indicate the partial stripping of monolayers by removal of sulfur and incorporation of oxygen leading to increased excitonic emissions. The demonstrated atomic‐scale manipulation to stabilize defect domains over large area with enhanced luminescence behavior is relevant for developing next‐generation nanoscale photonic devices.

中文翻译：

具有亚单分子层厚度的WS2缺陷域的选择性氧化导致光致发光的多重增强

稳定2D材料中亚单层厚度的缺陷区域在调节电子和光学性能方面起着重要作用。据报道，WS ₂单层的化学气相沉积生长具有对相和均匀成核缺陷域的控制。通过稳定缺陷占主导地位的域以实现纳米级光学器件的设计，可以实现多倍的光致发光（PL）增强（≈20倍）。虽然观察到的交替三角形形式的发光变化是由平面异质结构（1H-1T'）形成引起的，但在WS ₂的中心存在缺陷域异相单层导致光致发光增强20倍。观测到的发光增强与硫缺陷相关，并通过特定位置的空间X射线光电子能谱和低温下的原位PL测量得到了证实。详细的微观结构和光谱观察表明，通过除去硫和掺入氧气导致单分子层的部分剥离，导致激子发射增加。事实证明，通过原子级操纵来稳定大面积缺陷域并具有增强的发光性能，这与开发下一代纳米级光子器件有关。

更新日期：2019-08-27

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