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Title: Efficient carrier transport in halide perovskites: theoretical perspectives

Abstract

Recently, halide perovskites have been shown to exhibit excellent carrier transport properties. Density functional calculations are performed to study the electronic structure, dielectric properties, and defect properties of β-CH 3NH 3PbI 3. Our results show that Pb chemistry plays an important role in a wide range of material properties, i.e., small effective masses, enhanced Born effective charges and lattice polarization, and the suppression of the formation of deep defect levels, all of which contribute to the exceptionally good carrier transport properties observed in CH 3NH 3PbI 3. Defect calculations show that, among native point defects (including vacancies, interstitials, and antisites), only iodine vacancy is a low-energy deep trap and non-radiative recombination centre. Finaly, alloying iodide with chloride reduces the lattice constant of the iodide and significantly increases the formation energy of interstitial defects, which explains the observed substantial increase in carrier diffusion length in mixed halide CH 3NH 3PbI 3Cl compared to that in CH 3NH 3PbI 3.

Authors:
 [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1154829
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 2; Journal Issue: 24; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Du, M. H. Efficient carrier transport in halide perovskites: theoretical perspectives. United States: N. p., 2014. Web. doi:10.1039/c4ta01198h.
Du, M. H. Efficient carrier transport in halide perovskites: theoretical perspectives. United States. doi:10.1039/c4ta01198h.
Du, M. H. Thu . "Efficient carrier transport in halide perovskites: theoretical perspectives". United States. doi:10.1039/c4ta01198h.
@article{osti_1154829,
title = {Efficient carrier transport in halide perovskites: theoretical perspectives},
author = {Du, M. H.},
abstractNote = {Recently, halide perovskites have been shown to exhibit excellent carrier transport properties. Density functional calculations are performed to study the electronic structure, dielectric properties, and defect properties of β-CH3NH3PbI3. Our results show that Pb chemistry plays an important role in a wide range of material properties, i.e., small effective masses, enhanced Born effective charges and lattice polarization, and the suppression of the formation of deep defect levels, all of which contribute to the exceptionally good carrier transport properties observed in CH3NH3PbI3. Defect calculations show that, among native point defects (including vacancies, interstitials, and antisites), only iodine vacancy is a low-energy deep trap and non-radiative recombination centre. Finaly, alloying iodide with chloride reduces the lattice constant of the iodide and significantly increases the formation energy of interstitial defects, which explains the observed substantial increase in carrier diffusion length in mixed halide CH3NH3PbI3Cl compared to that in CH3NH3PbI3.},
doi = {10.1039/c4ta01198h},
journal = {Journal of Materials Chemistry. A},
issn = {2050-7488},
number = 24,
volume = 2,
place = {United States},
year = {2014},
month = {4}
}

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Enhanced Born charges in III-VII, IV-VII 2 , and V-VII 3 compounds
journal, July 2010


First-principles calculations for defects and impurities: Applications to III-nitrides
journal, April 2004

  • Van de Walle, Chris G.; Neugebauer, Jörg
  • Journal of Applied Physics, Vol. 95, Issue 8
  • DOI: 10.1063/1.1682673

Electronic band structure, phonons, and exciton binding energies of halide perovskites CsSnCl 3 , CsSnBr 3 , and CsSnI 3
journal, October 2013


Low-temperature processed meso-superstructured to thin-film perovskite solar cells
journal, January 2013

  • Ball, James M.; Lee, Michael M.; Hey, Andrew
  • Energy & Environmental Science, Vol. 6, Issue 6
  • DOI: 10.1039/c3ee40810h

Projector augmented-wave method
journal, December 1994


Electronic structure and defect properties of Tl 6 SeI 4 : Density functional calculations
journal, October 2012


All-solid-state dye-sensitized solar cells with high efficiency
journal, May 2012

  • Chung, In; Lee, Byunghong; He, Jiaqing
  • Nature, Vol. 485, Issue 7399, p. 486-489
  • DOI: 10.1038/nature11067

Unusual defect physics in CH 3 NH 3 PbI 3 perovskite solar cell absorber
journal, February 2014

  • Yin, Wan-Jian; Shi, Tingting; Yan, Yanfa
  • Applied Physics Letters, Vol. 104, Issue 6
  • DOI: 10.1063/1.4864778

Influence of the exchange screening parameter on the performance of screened hybrid functionals
journal, December 2006

  • Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F.
  • The Journal of Chemical Physics, Vol. 125, Issue 22
  • DOI: 10.1063/1.2404663

Orbital-dependent density functionals: Theory and applications
journal, January 2008


Small Photocarrier Effective Masses Featuring Ambipolar Transport in Methylammonium Lead Iodide Perovskite: A Density Functional Analysis
journal, November 2013

  • Giorgi, Giacomo; Fujisawa, Jun-Ichi; Segawa, Hiroshi
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 24
  • DOI: 10.1021/jz4023865

DFT and k · p modelling of the phase transitions of lead and tin halide perovskites for photovoltaic cells : DFT and
journal, October 2013

  • Even, Jacky; Pedesseau, Laurent; Jancu, Jean-Marc
  • physica status solidi (RRL) - Rapid Research Letters, Vol. 8, Issue 1
  • DOI: 10.1002/pssr.201308183

Thallium Chalcohalides for X-ray and γ-ray Detection
journal, July 2011

  • Johnsen, Simon; Liu, Zhifu; Peters, John A.
  • Journal of the American Chemical Society, Vol. 133, Issue 26
  • DOI: 10.1021/ja202540t

Enhanced Born charge and proximity to ferroelectricity in thallium halides
journal, April 2010


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Thallium Bromide Nuclear Radiation Detector Development
journal, August 2009

  • Churilov, Alexei V.; Ciampi, Guido; Kim, Hadong
  • IEEE Transactions on Nuclear Science, Vol. 56, Issue 4
  • DOI: 10.1109/TNS.2009.2021424

Mesoscopic CH3NH3PbI3/TiO2 Heterojunction Solar Cells
journal, October 2012

  • Etgar, Lioz; Gao, Peng; Xue, Zhaosheng
  • Journal of the American Chemical Society, Vol. 134, Issue 42, p. 17396-17399
  • DOI: 10.1021/ja307789s

Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013

  • Stranks, S. D.; Eperon, G. E.; Grancini, G.
  • Science, Vol. 342, Issue 6156, p. 341-344
  • DOI: 10.1126/science.1243982

Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
journal, October 2013


Overcoming the doping bottleneck in semiconductors
journal, August 2004


Synthesis and crystal chemistry of the hybrid perovskite (CH3NH3)PbI3 for solid-state sensitised solar cell applications
journal, January 2013

  • Baikie, Tom; Fang, Yanan; Kadro, Jeannette M.
  • Journal of Materials Chemistry A, Vol. 1, Issue 18
  • DOI: 10.1039/c3ta10518k

Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013

  • Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J.
  • Nature, Vol. 501, Issue 7467, p. 395-398
  • DOI: 10.1038/nature12509

Crystal Growth of the Perovskite Semiconductor CsPbBr 3 : A New Material for High-Energy Radiation Detection
journal, June 2013

  • Stoumpos, Constantinos C.; Malliakas, Christos D.; Peters, John A.
  • Crystal Growth & Design, Vol. 13, Issue 7
  • DOI: 10.1021/cg400645t

Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012


Origin of ferroelectricity in perovskite oxides
journal, July 1992


Structural and electronic properties of hybrid perovskites for high-efficiency thin-film photovoltaics from first-principles
journal, October 2013

  • Brivio, Federico; Walker, Alison B.; Walsh, Aron
  • APL Materials, Vol. 1, Issue 4
  • DOI: 10.1063/1.4824147

Importance of Spin–Orbit Coupling in Hybrid Organic/Inorganic Perovskites for Photovoltaic Applications
journal, August 2013

  • Even, Jacky; Pedesseau, Laurent; Jancu, Jean-Marc
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 17
  • DOI: 10.1021/jz401532q

Giant LO-TO splittings in perovskite ferroelectrics
journal, May 1994


Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells
journal, April 2014

  • Frost, Jarvist M.; Butler, Keith T.; Brivio, Federico
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl500390f

Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties
journal, July 2013

  • Stoumpos, Constantinos C.; Malliakas, Christos D.; Kanatzidis, Mercouri G.
  • Inorganic Chemistry, Vol. 52, Issue 15, p. 9019-9038
  • DOI: 10.1021/ic401215x

Dynamical atomic charges: The case of AB O 3 compounds
journal, September 1998


First-Principles Modeling of Mixed Halide Organometal Perovskites for Photovoltaic Applications
journal, July 2013

  • Mosconi, Edoardo; Amat, Anna; Nazeeruddin, Md. K.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 27
  • DOI: 10.1021/jp4048659

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


First-principles study of native defects in TlBr: Carrier trapping, compensation, and polarization phemomenon
journal, September 2010