Experimental and theoretical optical properties of methylammonium lead halide perovskites

Aurélien M A Leguy, Pooya Azarhoosh, M Isabel Alonso, Mariano Campoy-Quiles, Oliver J Weber, Jizhong Yao, Daniel Bryant, Mark T Weller, Jenny Nelson, Aron Walsh, Mark van Schilfgaarde, Piers R F Barnes

Research output: Contribution to journalArticle

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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).

Original languageEnglish
JournalNanoscale
Early online date5 Oct 2015
DOIs
Publication statusPublished - 19 Oct 2015

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Optical constants
Optical properties
Valence bands
Conduction bands
Optical transitions
Spectroscopic ellipsometry
Electron transitions
Band structure
Cations
Absorption spectra
Energy gap
Lead
Positive ions
Single crystals
methylamine

Cite this

Leguy, A. M. A., Azarhoosh, P., Alonso, M. I., Campoy-Quiles, M., Weber, O. J., Yao, J., ... Barnes, P. R. F. (2015). Experimental and theoretical optical properties of methylammonium lead halide perovskites. Nanoscale. https://doi.org/10.1039/c5nr05435d

Experimental and theoretical optical properties of methylammonium lead halide perovskites. / Leguy, Aurélien M A; Azarhoosh, Pooya; Alonso, M Isabel; Campoy-Quiles, Mariano; Weber, Oliver J; Yao, Jizhong; Bryant, Daniel; Weller, Mark T; Nelson, Jenny; Walsh, Aron; van Schilfgaarde, Mark; Barnes, Piers R F.

In: Nanoscale, 19.10.2015.

Research output: Contribution to journalArticle

Leguy, AMA, Azarhoosh, P, Alonso, MI, Campoy-Quiles, M, Weber, OJ, Yao, J, Bryant, D, Weller, MT, Nelson, J, Walsh, A, van Schilfgaarde, M & Barnes, PRF 2015, 'Experimental and theoretical optical properties of methylammonium lead halide perovskites', Nanoscale. https://doi.org/10.1039/c5nr05435d
Leguy AMA, Azarhoosh P, Alonso MI, Campoy-Quiles M, Weber OJ, Yao J et al. Experimental and theoretical optical properties of methylammonium lead halide perovskites. Nanoscale. 2015 Oct 19. https://doi.org/10.1039/c5nr05435d
Leguy, Aurélien M A ; Azarhoosh, Pooya ; Alonso, M Isabel ; Campoy-Quiles, Mariano ; Weber, Oliver J ; Yao, Jizhong ; Bryant, Daniel ; Weller, Mark T ; Nelson, Jenny ; Walsh, Aron ; van Schilfgaarde, Mark ; Barnes, Piers R F. / Experimental and theoretical optical properties of methylammonium lead halide perovskites. In: Nanoscale. 2015.
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AB - 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).

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