Halide Perovskite Heteroepitaxy: Bond Formation and Carrier Confinement at the PbS-CsPbBr3 Interface

Young Kwang Jung; Keith T. Butler; Aron Walsh

doi:10.1021/acs.jpcc.7b10000

Halide Perovskite Heteroepitaxy: Bond Formation and Carrier Confinement at the PbS-CsPbBr₃ Interface

Young Kwang Jung, Keith T. Butler, Aron Walsh

Department of Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

35 Citations (Scopus)

Abstract

Control of the stability, transport, and confinement of charge carriers (electrons and holes) at interfaces is a key requirement to realize robust halide perovskite devices. The PbS-CsPbBr₃ interface is atomically matched with low lattice strain, opening the potential for epitaxial growth. We assess the atomic nature of the interface using first-principles density functional theory calculations to identify (1) the thermodynamically stable (100) surface termination of the halide perovskite; (2) the most favorable (100)|(100) contact geometry; (3) the strong interfacial chemical bonding between PbS and CsPbBr₃; (4) the type I (straddling) band alignment that enables electron and hole confinement in the lead sulfide layer. The combination of metal halide perovskites and IV-VI semiconductors represents an important platform for probing interfacial chemical processes and realizing new functionality.

Original language	English
Pages (from-to)	27351-27356
Number of pages	6
Journal	Journal of Physical Chemistry C
Volume	121
Issue number	49
DOIs	https://doi.org/10.1021/acs.jpcc.7b10000
Publication status	Published - 2017 Dec 14

Bibliographical note

Funding Information:
We thank A. Soon for fruitful discussions. The work at ICL was supported by the EPSRC (Grant No. EP/K016288/1 and EP/ M009580/1) and the ERC (Grant No. 277757). A.W. is supported by a Royal Society University Research Fellowship. Via our membership of the U.K.’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202), this work used the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk).

Publisher Copyright:
© 2017 American Chemical Society.

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
Energy(all)
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

Access to Document

10.1021/acs.jpcc.7b10000

Cite this

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abstract = "Control of the stability, transport, and confinement of charge carriers (electrons and holes) at interfaces is a key requirement to realize robust halide perovskite devices. The PbS-CsPbBr3 interface is atomically matched with low lattice strain, opening the potential for epitaxial growth. We assess the atomic nature of the interface using first-principles density functional theory calculations to identify (1) the thermodynamically stable (100) surface termination of the halide perovskite; (2) the most favorable (100)|(100) contact geometry; (3) the strong interfacial chemical bonding between PbS and CsPbBr3; (4) the type I (straddling) band alignment that enables electron and hole confinement in the lead sulfide layer. The combination of metal halide perovskites and IV-VI semiconductors represents an important platform for probing interfacial chemical processes and realizing new functionality.",

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