Two-Dimensional Palladium Diselenide with Strong In-Plane Optical Anisotropy and High Mobility Grown by Chemical Vapor Deposition

Gu, Yiyi; Cai, Hui; Dong, Jichen; Yu, Yiling; Hoffmann, Anna; Liu, Chenze; Oyedele, Akinola; Lin, Yu-Chuan; Ge, George; Puretzky, Alexander; Duscher, Gerd; Chisholm, Matthew; Rack, Philip D.; Rouleau, Christopher; Gai, Zheng; Meng, Xiangmin; Ding, Feng; Geohegan, David; Xiao, Kai

doi:10.1002/adma.201906238

Two-Dimensional Palladium Diselenide with Strong In-Plane Optical Anisotropy and High Mobility Grown by Chemical Vapor Deposition

Journal Article · Mon Mar 16 00:00:00 EDT 2020 · Advanced Materials

DOI:https://doi.org/10.1002/adma.201906238· OSTI ID:1649489

Gu, Yiyi ^[1]; Cai, Hui ^[2]; Dong, Jichen ^[3]; ^[2]; Hoffmann, Anna ^[4]; Liu, Chenze ^[4]; Oyedele, Akinola ^[2]; ^[2]; Ge, George ^[2]; ^[2]; Duscher, Gerd ^[4]; ^[2]; ^[5]; ^[2]; ^[2]; Meng, Xiangmin ^[6]; Ding, Feng ^[7]; ^[2]; ^[2]

Chinese Academy of Sciences (CAS), Beijing (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Ulsan National Inst. of Science and Technology (UNIST) (South Korea)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Chinese Academy of Sciences (CAS), Beijing (China)
Ulsan National Inst. of Science and Technology (UNIST) (South Korea); Inst. for Basic Science (IBS), Ulsan (South Korea)

Two-dimensional (2D) palladium diselenide (PdSe₂) has strong interlayer coupling and a puckered pentagonal structure, leading to remarkable layer-dependent electronic structures and highly anisotropic in-plane optical and electronic properties. However, the lack of high-quality, 2D PdSe₂ crystals grown by bottom-up approaches limits the study of their exotic properties and practical applications. In this work, chemical vapor deposition growth of highly crystalline few-layer (≥2 layers) PdSe₂ crystals on various substrates is reported. The high quality of the PdSe₂ crystals is confirmed by low-frequency Raman spectroscopy, scanning transmission electron microscopy, and electrical characterization. In addition, strong in-plane optical anisotropy is demonstrated via polarized Raman spectroscopy and second-harmonic generation maps of the PdSe₂ flakes. A theoretical model based on kinetic Wulff construction theory and density functional theory calculations is developed and described the observed evolution of “square=like” shaped PdSe₂ crystals into rhombus due to the higher nucleation barriers for stable attachment on the (1,1) and (1,-1) edges, which results in their slower growth rates. Finally, few-layer PdSe₂ field-effect transistors reveal tunable ambipolar charge carrier conduction with an electron mobility up to ≈294 cm² V^-1 s^-1, which is comparable to that of exfoliated PdSe₂, indicating the promise of this anisotropic 2D material for electronics.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: China Scholarship Council; Institute for Basic Science; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1649489

Alternate ID(s):: OSTI ID: 1604823

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 19 Vol. 32; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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