Dative Epitaxy of Commensurate Monocrystalline Covalent van der Waals Moiré Supercrystal

Bian, Mengying; Zhu, Liang; Wang, Xiao; Choi, Junho; Chopdekar, Rajesh V.; Wei, Sichen; Wu, Lishu; Huai, Chang; Marga, Austin; Yang, Qishuo; Li, Yuguang C.; Yao, Fei; Yu, Ting; Crooker, Scott A.; Cheng, Xuemei M.; Sabirianov, Renat F.; Zhang, Shengbai; Lin, Junhao; Hou, Yanglong; Zeng, Hao

doi:10.1002/adma.202200117

Dative Epitaxy of Commensurate Monocrystalline Covalent van der Waals Moiré Supercrystal

Journal Article · Wed Mar 02 00:00:00 EST 2022 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202200117· OSTI ID:1880504

Bian, Mengying ^[1]; Zhu, Liang ^[2]; Wang, Xiao ^[3]; Choi, Junho ^[4]; Chopdekar, Rajesh V. ^[5]; Wei, Sichen ^[6]; Wu, Lishu ^[7]; Huai, Chang ^[6]; Marga, Austin ^[6]; Yang, Qishuo ^[2]; Li, Yuguang C. ^[6]; Yao, Fei ^[6]; Yu, Ting ^[7]; ^[4]; Cheng, Xuemei M. ^[3]; Sabirianov, Renat F. ^[8]; Zhang, Shengbai ^[9]; Lin, Junhao ^[2]; Hou, Yanglong ^[10]; ^[6]

Peking Univ., Beijing (China); State Univ. of New York (SUNY), Buffalo, NY (United States)
Southern University of Science and Technology (SUSTech), Shenzhen (China)
Bryn Mawr College, PA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
State Univ. of New York (SUNY), Buffalo, NY (United States)
Nanyang Technological Univ. (Singapore)
Univ. of Nebraska, Omaha, NE (United States)
Rensselaer Polytechnic Inst., Troy, NY (United States)
Peking Univ., Beijing (China)

Realizing van der Waals (vdW) epitaxy in the 1980s represents a breakthrough that circumvents the stringent lattice matching and processing compatibility requirements in conventional covalent heteroepitaxy. However, due to the weak vdW interactions, there is little control over film qualities by the substrate. Typically, discrete domains with a spread of misorientation angles are formed, limiting the applicability of vdW epitaxy. In this study, the epitaxial growth of monocrystalline, covalent Cr₅Te₈ 2D crystals on monolayer vdW WSe₂ by chemical vapor deposition is reported, driven by interfacial dative bond formation. The lattice of Cr₅Te₈, with a lateral dimension of a few tens of micrometers, is fully commensurate with that of WSe₂ via 3 × 3 (Cr₅Te₈)/7 × 7 (WSe₂) supercell matching, forming a single-crystalline moiré superlattice. This work establishes a conceptually distinct paradigm of thin-film epitaxy, termed “dative epitaxy”, which takes full advantage of covalent epitaxy with chemical bonding for fixing the atomic registry and crystal orientation, while circumventing its stringent lattice matching and processing compatibility requirements; conversely, it ensures the full flexibility of vdW epitaxy, while avoiding its poor orientation control. Cr₅Te₈ 2D crystals grown by dative epitaxy exhibit square magnetic hysteresis, suggesting minimized interfacial defects that can serve as pinning sites.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: China Postdoctoral Science Foundation; China–German Collaboration Project; Guangdong International Science Collaboration Project; National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); Science, Technology and Innovation Commission of Shenzhen Municipality; State Univ. of New York (SUNY) at Buffalo; State University of New York (SUNY) at Buffalo; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: 89233218CNA000001; AC02-05CH11231

OSTI ID:: 1880504

Alternate ID(s):: OSTI ID: 1925188

Report Number(s):: LA-UR-22-21038

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 17 Vol. 34; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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