Abstract

Abstract The unique structural and physical properties of two-dimensional (2D) atomic layer semiconductors render them promising candidates for electronic or optoelectronic devices. However, the lack of efficient and stable approaches to synthesize large-area thin films with excellent uniformity hinders their realistic applications. In this work, we reported a method involving atomic layer deposition and a chemical vapor deposition chamber to produce few-layer 2H-MoSe2 thin films with wafer-level uniformity. The reduction of MoO3 was found indispensable for the successful synthesis of MoSe2 films due to the low vaporization temperature. Moreover, a metal-semiconductor-metal photodetector (PD) was fabricated and investigated systematically. We extracted an ultrahigh photoresponsivity approaching 101 A/W with concomitantly high external quantum efficiency up to 19,668% due to the produced gain arising from the holes trapped at the metal/MoSe2 interface, the band tail state contribution, and the photogating effect. A fast response time of 22 ms was observed and attributed to effective nonequilibrium carrier recombination. Additionally, the ultrahigh photoresponsivity and low dark current that originated from Schottky barrier resulted in a record-high specific detectivity of up to 2×1013 Jones for 2D MoSe2/MoS2 PDs. Our findings revealed a pathway for the development of high-performance PDs based on 2D MoSe2 that are inexpensive, large area, and suitable for mass production and contribute to a deep understanding of the photoconductivity mechanisms in atomically thin MoSe2. We anticipate that these results are generalizable to other layer semiconductors as well.

Highlights

  • Nanomaterials are gaining intense interest in photodetection due to their large surface-to-volume ratios and low dimensions, which can yield higher light sensitivity than their bulk counterparts

  • We reported a method involving atomic layer deposition and a chemical vapor deposition chamber to produce few-layer 2H-MoSe2 thin films with wafer-level uniformity

  • We extracted an ultrahigh photoresponsivity approaching 101 A/W with concomitantly high external quantum efficiency up to 19,668% due to the produced gain arising from the holes trapped at the metal/MoSe2 interface, the band tail state contribution, and the photogating effect

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Summary

Introduction

Nanomaterials are gaining intense interest in photodetection due to their large surface-to-volume ratios and low dimensions, which can yield higher light sensitivity than their bulk counterparts. By employing quantum dots (QDs) [2] and one-dimensional (1D) semiconducting nanostructures of ZrS2, CdS, and ZnO as sensitizers [3,4,5], high-performance photodetectors (PDs) have been demonstrated. Benefiting from the quantum confinement effects in the out-of-plane direction, two-dimensional (2D) materials are highly promising for high-performance optoelectronic devices, which are compatible with current thin-film microfabrication techniques appropriately. The extremely high electrical mobility (up to 200,000 cm2/v/s for both electrons and holes) [6] and vanishing effective mass render graphene a promising candidate for high-speed photodetection, the responsivity of graphene-based PDs is far from satisfactory (~10−3 A/W) mainly due to its short photocarrier lifetime [7], low absorption ratio of incident light (~2%) [8, 9], and external quantum efficiency (EQE; 0.1–0.2%) [10].

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