Journal
CHEM
Volume 7, Issue 7, Pages 1887-1902Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2021.03.022
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Funding
- United States Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering [DE-SC0018828]
- Office of Naval Research [N00014-18-1-2491]
- Czech Science Foundation through GACR [20-16124J]
- International Scientific Partnership Program at King Saud University [ISPP-147]
- United States Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- National Science Foundation through the UC Irvine Materials Research Science and Engineering Center [DMR-2011967]
- U.S. Department of Energy (DOE) [DE-SC0018828] Funding Source: U.S. Department of Energy (DOE)
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A unique intercalation and separation chemistry has been proposed to successfully overcome the self-retarding effect and achieve complete intercalation of bulk crystals. This method enables high-yield preparation of highly pure 2D semiconductor monolayers and the assembly of large-area organic/inorganic hybrid superlattices, creating a new field of artificial superlattice materials.
The scalable preparation of high-purity monolayers is essential for practically integrating two-dimensional (2D) semiconductors in diverse technologies but remains a persistent challenge. Previous efforts to exfoliate 2D layered crystals by the organic ammonium intercalation usually produce few-layer nanosheets owing to a self-retarding effect that hinders the complete intercalation in neighboring layers. Herein, we report a unique intercalation and separation'' chemistry with a constant self-refreshing crystal surface that mitigates the self-retarding effect to ensure a complete intercalation of the bulk crystal, ultimately enabling high-yield solution-phase exfoliation of 2D semiconductor monolayers in excellent purity (e.g., monolayer purity of >95% for In2Se3 and InSe). Furthermore, we have assembled large-area organic/inorganic hybrid superlattices with diverse organic molecules and inorganic 2D monolayer crystals, thus creating a family of artificial superlattice materials with atomically modulated chemical compositions, widely tunable superlattice periodicities, and specifically tailorable electronic and thermal properties.
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