Strong Structural and Electronic Coupling in Metavalent PbS Moiré Superlattices

Wang, Yu; Song, Zhigang; Wan, Jiawei; Betzler, Sophia; Xie, Yujun; Ophus, Colin; Bustillo, Karen C.; Ercius, Peter; Wang, Lin-Wang; Zheng, Haimei

doi:10.1021/jacs.2c09947

Strong Structural and Electronic Coupling in Metavalent PbS Moiré Superlattices

Journal Article · Tue Dec 13 00:00:00 EST 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c09947· OSTI ID:1972946

^[1]; Song, Zhigang ^[2]; Wan, Jiawei ^[3]; ^[4]; Xie, Yujun ^[4]; Ophus, Colin ^[5]; ^[5]; ^[5]; ^[4]; ^[3]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; South China Univ. of Technology (SCUT), Guangzhou (China)
Harvard Univ., Cambridge, MA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry

Moiré superlattices are twisted bilayer materials in which the tunable interlayer quantum confinement offers access to new physics and novel device functionalities. Previously, moiré superlattices were built exclusively using materials with weak van der Waals interactions, and synthesizing moiré superlattices with strong interlayer chemical bonding was considered to be impractical. Here, in this study, using lead sulfide (PbS) as an example, we report a strategy for synthesizing moiré superlattices coupled by strong chemical bonding. We use water-soluble ligands as a removable template to obtain free-standing ultrathin PbS nanosheets and assemble them into direct-contact bilayers with various twist angles. Atomic-resolution imaging shows the moiré periodic structural reconstruction at the superlattice interface due to the strong metavalent coupling. Electron energy loss spectroscopy and theoretical calculations collectively reveal the twist-angle-dependent electronic structure, especially the emergent separation of flat bands at small twist angles. The localized states of flat bands are similar to well-arranged quantum dots, promising an application in devices. This study opens a new door to the exploration of deep energy modulations within moiré superlattices alternative to van der Waals twistronics.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1972946

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 51 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Strong Structural and Electronic Coupling in Metavalent PbS Moiré Superlattices

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