Epitaxial Growth of Centimeter-Scale Single-Crystal MoS2 Monolayer on Au (111).

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) have emerged as attractive platforms in next-generation nanoelectronics and optoelectronics for reducing device sizes down to ten nanometer scale. To achieve this, the controlled synthesis of wafer-scale single-crystal TMDs with high crystallinity has been a continuous pursuit. However, previous efforts to epitaxially grow TMD films on insulating substrates (e.g., mica and sapphire) failed to eliminate the evolution of antiparallel domains and twin boundaries, leading to the formation of polycrystalline films. Herein, we report the epitaxial growth of wafer-scale single-crystal MoS2 monolayers on vicinal Au (111) thin films, as obtained by melting and resolidifying commercial Au foils. The unidirectional alignment and seamless stitching of the MoS2 domains were comprehensively demonstrated using atomic- to centimeter-scale characterization techniques. By utilizing onsite scanning tunneling microscope characterizations combined with first-principles calculations, it was revealed that, the nucleation of MoS2 monolayer is dominantly guided by the steps on Au (111), which leads to highly-oriented growth of MoS2 along the <110> step edges. This work, thereby, makes a significant step towards the practical applications of semiconducting 2D materials and the large-scale integration of 2D electronics.

[1]  Q. Fu,et al.  Single-crystal hexagonal boron nitride monolayer epitaxially grown on Cu (111) thin film across a wafer , 2021, 2105.15040.

[2]  Yu Huang,et al.  Van der Waals thin-film electronics , 2019, Nature Electronics.

[3]  Lei Yin,et al.  Recent Progress in CVD Growth of 2D Transition Metal Dichalcogenides and Related Heterostructures , 2019, Advanced materials.

[4]  Enge Wang,et al.  Epitaxial growth of a 100-square-centimetre single-crystal hexagonal boron nitride monolayer on copper , 2019, Nature.

[5]  James Hone,et al.  Disorder in van der Waals heterostructures of 2D materials , 2019, Nature Materials.

[6]  H. Jeong,et al.  Van der Waals contacts between three-dimensional metals and two-dimensional semiconductors , 2019, Nature.

[7]  Ksenia V. Bets,et al.  How the Complementarity at Vicinal Steps Enables Growth of 2D Monocrystals. , 2019, Nano letters.

[8]  D. Muller,et al.  Additive manufacturing of patterned 2D semiconductor through recyclable masked growth , 2019, Proceedings of the National Academy of Sciences of the United States of America.

[9]  T. Booth,et al.  A universal approach for the synthesis of two-dimensional binary compounds , 2018, Nature Communications.

[10]  Young Hee Lee,et al.  Wafer-scale single-crystal hexagonal boron nitride film via self-collimated grain formation , 2018, Science.

[11]  Bin Wang,et al.  Colossal grain growth yields single-crystal metal foils by contact-free annealing , 2018, Science.

[12]  Chuanghan Hsu,et al.  A library of atomically thin metal chalcogenides , 2018, Nature.

[13]  Zhongfan Liu,et al.  Batch production of 6-inch uniform monolayer molybdenum disulfide catalyzed by sodium in glass , 2018, Nature Communications.

[14]  D. Lizzit,et al.  Epitaxial growth of single-orientation high-quality MoS2 monolayers , 2018, 1802.02220.

[15]  Guodong Liu,et al.  Wafer-Scale Growth and Transfer of Highly-Oriented Monolayer MoS2 Continuous Films. , 2017, ACS nano.

[16]  L. Gu,et al.  Two-dimensional metallic tantalum disulfide as a hydrogen evolution catalyst , 2017, Nature Communications.

[17]  Zhenhua Ni,et al.  Ultrafast Growth of High‐Quality Monolayer WSe2 on Au , 2017, Advanced materials.

[18]  R. Ruoff,et al.  Ultrafast epitaxial growth of metre-sized single-crystal graphene on industrial Cu foil. , 2017, Science Bulletin.

[19]  Zijing Ding,et al.  Molecular Beam Epitaxy of Highly Crystalline Monolayer Molybdenum Disulfide on Hexagonal Boron Nitride. , 2017, Journal of the American Chemical Society.

[20]  Qiyuan He,et al.  Recent Advances in Ultrathin Two-Dimensional Nanomaterials. , 2017, Chemical reviews.

[21]  Wei Liu,et al.  Chemical Vapor Deposition of Large-Size Monolayer MoSe2 Crystals on Molten Glass. , 2017, Journal of the American Chemical Society.

[22]  Tao Zhang,et al.  Twinned growth behaviour of two-dimensional materials , 2016, Nature Communications.

[23]  L. Gu,et al.  Temperature‐Mediated Selective Growth of MoS2/WS2 and WS2/MoS2 Vertical Stacks on Au Foils for Direct Photocatalytic Applications , 2016, Advanced materials.

[24]  S. Chae,et al.  Misorientation-angle-dependent electrical transport across molybdenum disulfide grain boundaries , 2016, Nature Communications.

[25]  Jing Zhao,et al.  Oxygen-Assisted Chemical Vapor Deposition Growth of Large Single-Crystal and High-Quality Monolayer MoS2. , 2015, Journal of the American Chemical Society.

[26]  N. Xu,et al.  All Chemical Vapor Deposition Synthesis and Intrinsic Bandgap Observation of MoS2/Graphene Heterostructures , 2015, Advanced materials.

[27]  Lianmao Peng,et al.  Large-area synthesis of high-quality and uniform monolayer WS2 on reusable Au foils , 2015, Nature Communications.

[28]  M. Ge,et al.  Step-Edge-Guided Nucleation and Growth of Aligned WSe2 on Sapphire via a Layer-over-Layer Growth Mode. , 2015, ACS nano.

[29]  Zhongfan Liu,et al.  Substrate Facet Effect on the Growth of Monolayer MoS2 on Au Foils. , 2015, ACS nano.

[30]  Gang Hee Han,et al.  Seeded growth of highly crystalline molybdenum disulphide monolayers at controlled locations , 2015, Nature Communications.

[31]  Qiang Sun,et al.  Unravelling orientation distribution and merging behavior of monolayer MoS2 domains on sapphire. , 2015, Nano letters.

[32]  Oriol López Sánchez,et al.  Large-Area Epitaxial Monolayer MoS2 , 2015, ACS nano.

[33]  Jingyu Sun,et al.  Controllable growth and transfer of monolayer MoS2 on Au foils and its potential application in hydrogen evolution reaction. , 2014, ACS nano.

[34]  Yu Zhang,et al.  Controlled growth of high-quality monolayer WS2 layers on sapphire and imaging its grain boundary. , 2013, ACS nano.

[35]  Jun Lou,et al.  Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers. , 2013, Nature materials.

[36]  Xiaolong Zou,et al.  Predicting dislocations and grain boundaries in two-dimensional metal-disulfides from the first principles. , 2013, Nano letters.

[37]  Timothy C. Berkelbach,et al.  Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide. , 2013, Nature Materials.

[38]  J. Shan,et al.  Tightly bound trions in monolayer MoS2. , 2012, Nature materials.

[39]  Qing Hua Wang,et al.  Electronics and optoelectronics of two-dimensional transition metal dichalcogenides. , 2012, Nature nanotechnology.

[40]  Bin Wang,et al.  Single terrace growth of graphene on a metal surface. , 2011, Nano letters.

[41]  G. Kresse,et al.  Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set , 1996 .