Dynamic symmetry breaking and spin splitting in metal halide perovskites

Scott McKechnie, Jarvist M. Frost, Dimitar Pashov, Pooya Azarhoosh, Aron Walsh, Mark Van Schilfgaarde

Research output: Contribution to journalArticle

12 Citations (Scopus)

Abstract

Metal halide perovskites exhibit a materials physics that is distinct from traditional semiconductors. While materials such as CH3NH3PbI3 are nonmagnetic, the presence of heavy elements (Pb and I) in a noncentrosymmetric crystal environment result in a spin splitting of the frontier electronic bands through the Rashba-Dresselhaus effect. We show, from a combination of ab initio molecular dynamics, density-functional theory, and quasiparticle GW theory, that the nature (magnitude and orientation) of the band splitting depends on the local asymmetry around the Pb and I sites in the perovskite structure. The potential fluctuations vary in time as a result of thermal disorder. We show that the same physics emerges both for the organic-inorganic CH3NH3PbI3 and the inorganic CsPbI3 compound. The results are relevant to the photophysics of these compounds and are expected to be general to other lead iodide containing perovskites.

Original languageEnglish
Article number085108
JournalPhysical Review B
Volume98
Issue number8
DOIs
Publication statusPublished - 2018 Aug 6

Fingerprint

Metal halides
metal halides
perovskites
broken symmetry
Physics
Inorganic compounds
inorganic compounds
physics
Iodides
heavy elements
Perovskite
iodides
Density functional theory
Molecular dynamics
Lead
asymmetry
disorders
Semiconductor materials
molecular dynamics
density functional theory

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Cite this

McKechnie, S., Frost, J. M., Pashov, D., Azarhoosh, P., Walsh, A., & Van Schilfgaarde, M. (2018). Dynamic symmetry breaking and spin splitting in metal halide perovskites. Physical Review B, 98(8), [085108]. https://doi.org/10.1103/PhysRevB.98.085108
McKechnie, Scott ; Frost, Jarvist M. ; Pashov, Dimitar ; Azarhoosh, Pooya ; Walsh, Aron ; Van Schilfgaarde, Mark. / Dynamic symmetry breaking and spin splitting in metal halide perovskites. In: Physical Review B. 2018 ; Vol. 98, No. 8.
@article{115f6cd3db3c4e60b7118d2fc8b893e9,
title = "Dynamic symmetry breaking and spin splitting in metal halide perovskites",
abstract = "Metal halide perovskites exhibit a materials physics that is distinct from traditional semiconductors. While materials such as CH3NH3PbI3 are nonmagnetic, the presence of heavy elements (Pb and I) in a noncentrosymmetric crystal environment result in a spin splitting of the frontier electronic bands through the Rashba-Dresselhaus effect. We show, from a combination of ab initio molecular dynamics, density-functional theory, and quasiparticle GW theory, that the nature (magnitude and orientation) of the band splitting depends on the local asymmetry around the Pb and I sites in the perovskite structure. The potential fluctuations vary in time as a result of thermal disorder. We show that the same physics emerges both for the organic-inorganic CH3NH3PbI3 and the inorganic CsPbI3 compound. The results are relevant to the photophysics of these compounds and are expected to be general to other lead iodide containing perovskites.",
author = "Scott McKechnie and Frost, {Jarvist M.} and Dimitar Pashov and Pooya Azarhoosh and Aron Walsh and {Van Schilfgaarde}, Mark",
year = "2018",
month = "8",
day = "6",
doi = "10.1103/PhysRevB.98.085108",
language = "English",
volume = "98",
journal = "Physical Review B",
issn = "2469-9950",
publisher = "American Physical Society",
number = "8",

}

McKechnie, S, Frost, JM, Pashov, D, Azarhoosh, P, Walsh, A & Van Schilfgaarde, M 2018, 'Dynamic symmetry breaking and spin splitting in metal halide perovskites', Physical Review B, vol. 98, no. 8, 085108. https://doi.org/10.1103/PhysRevB.98.085108

Dynamic symmetry breaking and spin splitting in metal halide perovskites. / McKechnie, Scott; Frost, Jarvist M.; Pashov, Dimitar; Azarhoosh, Pooya; Walsh, Aron; Van Schilfgaarde, Mark.

In: Physical Review B, Vol. 98, No. 8, 085108, 06.08.2018.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Dynamic symmetry breaking and spin splitting in metal halide perovskites

AU - McKechnie, Scott

AU - Frost, Jarvist M.

AU - Pashov, Dimitar

AU - Azarhoosh, Pooya

AU - Walsh, Aron

AU - Van Schilfgaarde, Mark

PY - 2018/8/6

Y1 - 2018/8/6

N2 - Metal halide perovskites exhibit a materials physics that is distinct from traditional semiconductors. While materials such as CH3NH3PbI3 are nonmagnetic, the presence of heavy elements (Pb and I) in a noncentrosymmetric crystal environment result in a spin splitting of the frontier electronic bands through the Rashba-Dresselhaus effect. We show, from a combination of ab initio molecular dynamics, density-functional theory, and quasiparticle GW theory, that the nature (magnitude and orientation) of the band splitting depends on the local asymmetry around the Pb and I sites in the perovskite structure. The potential fluctuations vary in time as a result of thermal disorder. We show that the same physics emerges both for the organic-inorganic CH3NH3PbI3 and the inorganic CsPbI3 compound. The results are relevant to the photophysics of these compounds and are expected to be general to other lead iodide containing perovskites.

AB - Metal halide perovskites exhibit a materials physics that is distinct from traditional semiconductors. While materials such as CH3NH3PbI3 are nonmagnetic, the presence of heavy elements (Pb and I) in a noncentrosymmetric crystal environment result in a spin splitting of the frontier electronic bands through the Rashba-Dresselhaus effect. We show, from a combination of ab initio molecular dynamics, density-functional theory, and quasiparticle GW theory, that the nature (magnitude and orientation) of the band splitting depends on the local asymmetry around the Pb and I sites in the perovskite structure. The potential fluctuations vary in time as a result of thermal disorder. We show that the same physics emerges both for the organic-inorganic CH3NH3PbI3 and the inorganic CsPbI3 compound. The results are relevant to the photophysics of these compounds and are expected to be general to other lead iodide containing perovskites.

UR - http://www.scopus.com/inward/record.url?scp=85051538375&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85051538375&partnerID=8YFLogxK

U2 - 10.1103/PhysRevB.98.085108

DO - 10.1103/PhysRevB.98.085108

M3 - Article

VL - 98

JO - Physical Review B

JF - Physical Review B

SN - 2469-9950

IS - 8

M1 - 085108

ER -

McKechnie S, Frost JM, Pashov D, Azarhoosh P, Walsh A, Van Schilfgaarde M. Dynamic symmetry breaking and spin splitting in metal halide perovskites. Physical Review B. 2018 Aug 6;98(8). 085108. https://doi.org/10.1103/PhysRevB.98.085108