Can Pb-free halide double perovskites support high-efficiency solar cells?
File(s)acsenergy_doubleperovskite_16.pdf (4.06 MB)
Published version
Author(s)
Savory, CN
Walsh, A
Scanlon, DO
Type
Journal Article
Abstract
The methylammonium lead halides have become champion photoactive semiconductors for solar cell applications; however, issues still remain with respect to chemical instability and potential toxicity. Recently, the Cs2AgBiX6 (X = Cl, Br) double perovskite family has been synthesized and investigated as stable nontoxic replacements. We probe the chemical bonding, physical properties, and cation anti-site disorder of Cs2AgBiX6 and related compounds from first-principles. We demonstrate that the combination of Ag(I) and Bi(III) leads to the wide indirect band gaps with large carrier effective masses owing to a mismatch in angular momentum of the frontier atomic orbitals. The spectroscopically limited photovoltaic conversion efficiency is less than 10% for X = Cl or Br. This limitation can be overcome by replacing Ag with In or Tl; however, the resulting compounds are predicted to be unstable thermodynamically. The search for nontoxic bismuth perovskites must expand beyond the Cs2AgBiX6 motif.
Date Issued
2016-10-12
Date Acceptance
2016-10-12
Citation
ACS Energy Letters, 2016, 1 (5), pp.949-955
ISSN
2380-8195
Publisher
American Chemical Society
Start Page
949
End Page
955
Journal / Book Title
ACS Energy Letters
Volume
1
Issue
5
Copyright Statement
© 2016 The Authors. This is an open access article published under a Creative Commons Attribution (CC-BY) License (http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html), which permits unrestricted use, distribution and reproduction in any medium,
provided the author and source are cited.
provided the author and source are cited.
Sponsor
The Royal Society
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000390085700009&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Grant Number
UF150657
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Electrochemistry
Energy & Fuels
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Chemistry
Science & Technology - Other Topics
Materials Science
INITIO MOLECULAR-DYNAMICS
TOTAL-ENERGY CALCULATIONS
QUASI-RANDOM STRUCTURES
WAVE BASIS-SET
PHOTOVOLTAIC APPLICATIONS
ELECTRONIC-PROPERTIES
HYBRID PEROVSKITES
SEMICONDUCTORS
STABILITY
ABSORBER
Publication Status
Published