Frontiers in Materials Modelling of Hybrid Perovskites: Electrons, Phonons and Dynamic Disorder
Aron Walsh a
a Imperial College London, United Kingdom, South Kensington, Londres, Reino Unido, United Kingdom
Proceedings of Perovskite Thin Film Photovoltaics (ABXPV17)
València, Spain, 2017 March 1st - 2nd
Organizers: Henk Bolink and David Cahen
Invited Speaker, Aron Walsh, presentation 091
Publication date: 18th December 2016

The first report on quantum mechanical calculations of methylammonium lead iodide was in 2004[1]. Since then, many millions of processing hours have been spent calculating the properties of these intriguing compounds.

I will critically review the contribution of materials modelling to the field of hybrid perovskite solar cells and assess the current status and challenges. This will include research from my group, where we have been developing and applying from multi-scale simulation techniques [2-5]. The temporal behaviour of hybrid perovskites predicted by theory has recently been validated through a combination of neutron scattering, time-resolved vibrational spectroscopy, and kinetic measurements of the current-voltage response. The implications for achieving high-efficiency stable photovoltaic devices will be discussed.

This research has been supported by the ERC, Royal Society and ESPRC, with a wide collaboration network including simulations by Jarvist Frost, Jonathan Skelton, Federico Brivio and Keith Butler.

1. "First-principles study of the structural and the electronic properties of the lead-halide-based inorganic-organic perovskites (CH3NH3)PbX3 and CsPbX3 (X = Cl, Br, I)" J. Korean Phys. Soc. 44, 889 (2004)

2. “Atomistic origins of high-performance in hybrid halide perovskite solar cells” Nano Letters, 14, 2584 (2014)

3. “Molecular ferroelectric contributions to anomalous hysteresis in hybrid perovskite solar cells” APL Materials 2, 081506 (2014)

4. "Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites" Phys. Chem. Chem. Phys. 18, 27051 (2016)

5. "Direct observation of dynamic symmetry breaking above room temperature in methylammonium lead iodide perovskite" ACS Energy Lett. 1, 880 (2016)

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