Abstract

Two-dimensional transition metal dichalcogenides (2D TMDs) have gained great interest due to their unique tunable bandgap as a function of the number of layers. Especially, single-layer tungsten disulfides (WS2) is a direct band gap semiconductor with a gap of 2.1 eV featuring strong photoluminescence and large exciton binding energy. Although synthesis of MoS2 and their layer dependent properties have been studied rigorously, little attention has been paid to the formation of single-layer WS2 and its layer dependent properties. Here we report the scalable synthesis of uniform single-layer WS2 film by a two-step chemical vapor deposition (CVD) method followed by a laser thinning process. The PL intensity increases six-fold, while the PL peak shifts from 1.92 eV to 1.97 eV during the laser thinning from few-layers to single-layer. We find from the analysis of exciton complexes that both a neutral exciton and a trion increases with decreasing WS2 film thickness; however, the neutral exciton is predominant in single-layer WS2. The binding energies of trion and biexciton for single-layer WS2 are experimentally characterized at 35 meV and 60 meV, respectively. The tunable optical properties by precise control of WS2 layers could empower a great deal of flexibility in designing atomically thin optoelectronic devices.

Highlights

  • During the laser thinning from few-layers to single-layer

  • We introduce a large-scale single-layer WS2 film synthesis by using the two-step method followed by a laser thinning process

  • The synthesized WS2 film was characterized by atomic force microscopy (AFM), Raman spectroscopy, PL, and X-ray photoelectron spectroscopy (XPS)

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Summary

Introduction

During the laser thinning from few-layers to single-layer. We find from the analysis of exciton complexes that both a neutral exciton and a trion increases with decreasing WS2 film thickness; the neutral exciton is predominant in single-layer WS2. Recent studies have shown that single-layer TMDs exhibit direct band gap property that is accompanied by strong photoluminescence (PL) emission and large exciton binding energy; they are promising materials for fundamental studies as well as next-generation ultra-thin opto-electronic devices[4,5]. Song et al.[9] presented fabrication of layer-controlled WS2 by sulfurization of WO3 film using atomic layer deposition (ALD), and Yun et al.[10] reported centimeter-scale single-layer WS2 on gold foil by using chemical vapor deposition (CVD). Their PL spectra within the single-layer WS2 film were spatially nonuniform. The exact values for the binding energy of the excitons in WS2 are still debated and the behavior of exciton complexes with respect to the WS2 layers remains unexplored

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