Kim Minseong, Seo Jihyung, Kim Jihyun, Moon Jong Sung, Lee Junghyun, Kim Je-Hyung, Kang Joohoon, Park Hyesung
Department of Materials Science and Engineering, Perovtronics Research Center, Low Dimensional Carbon Materials Center, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea.
School of Advanced Materials Science and Engineering, Sungkyunkwan University (SKKU), Suwon 16419, Republic of Korea.
ACS Nano. 2021 Feb 23;15(2):3038-3046. doi: 10.1021/acsnano.0c09430. Epub 2021 Jan 29.
Chemical vapor deposition (CVD) using liquid-phase precursors has emerged as a viable technique for synthesizing uniform large-area transition metal dichalcogenide (TMD) thin films. However, the liquid-phase precursor-assisted growth process typically suffers from small-sized grains and unreacted transition metal precursor remainders, resulting in lower-quality TMDs. Moreover, synthesizing large-area TMD films with a monolayer thickness is also quite challenging. Herein, we successfully synthesized high-quality large-area monolayer molybdenum diselenide (MoSe) with good uniformity via promoter-assisted liquid-phase CVD process using the transition metal-containing precursor homogeneously modified with an alkali metal halide. The formation of a reactive transition metal oxyhalide and reduction of the energy barrier of chalcogenization by the alkali metal promoted the growth rate of the TMDs along the in-plane direction, enabling the full coverage of the monolayer MoSe film with negligible few-layer regions. Note that the fully selenized monolayer MoSe with high crystallinity exhibited superior electrical transport characteristics compared with those reported in previous works using liquid-phase precursors. We further synthesized various other monolayer TMD films, including molybdenum disulfide, tungsten disulfide, and tungsten diselenide, to demonstrate the broad applicability of the proposed approach.
使用液相前驱体的化学气相沉积(CVD)已成为一种可行的技术,用于合成均匀的大面积过渡金属二硫属化物(TMD)薄膜。然而,液相前驱体辅助生长过程通常存在晶粒尺寸小和未反应的过渡金属前驱体残留的问题,导致TMD的质量较低。此外,合成具有单层厚度的大面积TMD薄膜也颇具挑战性。在此,我们通过使用用碱金属卤化物均匀改性的含过渡金属前驱体的促进剂辅助液相CVD工艺,成功合成了高质量、大面积且均匀性良好的单层二硒化钼(MoSe₂)。反应性过渡金属卤氧化物的形成以及碱金属对硫化过程能垒的降低促进了TMD沿面内方向的生长速率,使得单层MoSe₂薄膜能够完全覆盖,几乎没有少层区域。值得注意的是,与先前使用液相前驱体的工作报道相比,具有高结晶度的完全硒化单层MoSe₂表现出优异的电输运特性。我们进一步合成了各种其他单层TMD薄膜,包括二硫化钼、二硫化钨和二硒化钨,以证明所提出方法的广泛适用性。