Experimental and theoretical optical properties of methylammonium lead halide perovskites
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Published version
Author(s)
Type
Journal Article
Abstract
The optical constants of methylammonium lead halide single crystals CH3NH3PbX3 (X = I, Br, Cl) are interpreted with high level ab initio calculations using the relativistic quasiparticle self-consistent GW approximation (QSGW). Good agreement between the optical constants derived from QSGW and those obtained from spectroscopic ellipsometry enables the assignment of the spectral features to their respective inter-band transitions. We show that the transition from the highest valence band (VB) to the lowest conduction band (CB) is responsible for almost all the optical response of MAPbI3 between 1.2 and 5.5 eV (with minor contributions from the second highest VB and the second lowest CB). The calculations indicate that the orientation of [CH3NH3]+ cations has a significant influence on the position of the bandgap suggesting that collective orientation of the organic moieties could result in significant local variations of the optical properties. The optical constants and energy band diagram of CH3NH3PbI3 are then used to simulate the contributions from different optical transitions to a typical transient absorption spectrum (TAS).
Date Issued
2016-03-28
Online Publication Date
2015-10-05
2016-05-17T09:21:47Z
Date Acceptance
2015-09-30
ISSN
2040-3372
Publisher
Royal Society of Chemistry
Start Page
6317
End Page
6327
Journal / Book Title
Nanoscale
Volume
8
Issue
12
Copyright Statement
© The Royal Society of Chemistry 2016. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Source Database
web-of-science
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (E
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (E
Grant Number
EP/J002305/1
EP/M025020/1
J14384
EP/K030671/1
J13361
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Physics, Applied
Chemistry
Science & Technology - Other Topics
Materials Science
Physics
SOLAR-CELLS
CHARGE SEPARATION
ELECTRON
EFFICIENCY
STATE
IODIDE
POLARIZATION
CARRIERS
SPECTRA
LENGTHS
Nanoscience & Nanotechnology
02 Physical Sciences
03 Chemical Sciences
10 Technology
Publication Status
Published
Date Publish Online
2015-10-05