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Title: Two-Dimensional Halide Perovskites: Tuning Electronic Activities of Defects

Abstract

Two-dimensional (2D) halide perovskites are emerging as promising candidates for nanoelectronics and optoelectronics. To realize their full potential, it is important to understand the role of those defects that can strongly impact material properties. In contrast to other popular 2D semiconductors (e.g., transition metal dichalcogenides MX2) for which defects typically induce harmful traps, we show that the electronic activities of defects in 2D perovskites are significantly tunable. For example, even with a fixed lattice orientation one can change the synthesis conditions to convert a line defect (edge or grain boundary) from electron acceptor to inactive site without deep gap states. Here, we show that this difference originates from the enhanced ionic bonding in these perovskites compared with MX2. The donors tend to have high formation energies and the harmful defects are difficult to form at a low halide chemical potential. Thus, we unveil unique properties of defects in 2D perovskites and suggest practical routes to improve them.

Authors:
 [1];  [2];  [2]
+ Show Author Affiliations
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center and the Resnick Sustainability Inst.
  2. California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center
Publication Date:
Research Org.:
California Institute of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1250031
Alternate Identifier(s):
OSTI ID: 1435806
Grant/Contract Number:  
SC0004993; CBET-1512759; FOA 0001276; AC02-05CH11231; ACI-1053575
Resource Type:
Published Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Name: Nano Letters Journal Volume: 16 Journal Issue: 5; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 30 DIRECT ENERGY CONVERSION; defects; first-principle calculations; Halide perovskites; two-dimensional materials

Citation Formats

Liu, Yuanyue, Xiao, Hai, and Goddard, William A. Two-Dimensional Halide Perovskites: Tuning Electronic Activities of Defects. United States: N. p., 2016. Web. doi:10.1021/acs.nanolett.6b00964.
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Liu, Yuanyue, Xiao, Hai, & Goddard, William A. Two-Dimensional Halide Perovskites: Tuning Electronic Activities of Defects. United States. https://doi.org/10.1021/acs.nanolett.6b00964
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Liu, Yuanyue, Xiao, Hai, and Goddard, William A. Thu . "Two-Dimensional Halide Perovskites: Tuning Electronic Activities of Defects". United States. https://doi.org/10.1021/acs.nanolett.6b00964.
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@article{osti_1250031,
title = {Two-Dimensional Halide Perovskites: Tuning Electronic Activities of Defects},
author = {Liu, Yuanyue and Xiao, Hai and Goddard, William A.},
abstractNote = {Two-dimensional (2D) halide perovskites are emerging as promising candidates for nanoelectronics and optoelectronics. To realize their full potential, it is important to understand the role of those defects that can strongly impact material properties. In contrast to other popular 2D semiconductors (e.g., transition metal dichalcogenides MX2) for which defects typically induce harmful traps, we show that the electronic activities of defects in 2D perovskites are significantly tunable. For example, even with a fixed lattice orientation one can change the synthesis conditions to convert a line defect (edge or grain boundary) from electron acceptor to inactive site without deep gap states. Here, we show that this difference originates from the enhanced ionic bonding in these perovskites compared with MX2. The donors tend to have high formation energies and the harmful defects are difficult to form at a low halide chemical potential. Thus, we unveil unique properties of defects in 2D perovskites and suggest practical routes to improve them.},
doi = {10.1021/acs.nanolett.6b00964},
journal = {Nano Letters},
number = 5,
volume = 16,
place = {United States},
year = {Thu Apr 21 00:00:00 EDT 2016},
month = {Thu Apr 21 00:00:00 EDT 2016}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acs.nanolett.6b00964
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