Where Next for Atomistic Modelling of Halide Perovskites?
Aron Walsh a
a Department of Materials, Imperial College London, Prince Consort Rd, South Kensington, London, United Kingdom
International Conference on Hybrid and Organic Photovoltaics
Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Online, Spain, 2021 May 24th - 28th
Organizers: Marina Freitag, Feng Gao and Sam Stranks
Invited Speaker, Aron Walsh, presentation 117
Publication date: 11th May 2021

As technologies based on metal halide perovskites have rapidly developed, so too has our understanding of the underpinning chemistry and physics. There has been close collaboration and interplay between measurement and modelling throughout this process. The impact of in silico methods has ranged from understanding the microscopic nature of chemical bonding to the macroscopic responses of the crystal. These include studies involving lattice vibrations and molecular rotations, charged point defects and dielectric response, to describing complex emergent behavior including current-voltage hysteresis, ferroelectricity, and photoinstabilities. In this talk, beyond covering some of my own research [1-5], I will give a perspective on current directions and future challenges for modelling soft crystalline semiconductors.


1. “Atomistic origins of high-performance in hybrid halide perovskite solar cells” Nano Letters, 14, 2584 (2014); https://pubs.acs.org/doi/10.1021/nl500390f

2. "Direct observation of dynamic symmetry breaking above room temperature in methylammonium lead iodide perovskite" ACS Energy Lett. 1, 880 (2016); https://doi.org/10.1021/acsenergylett.6b00381

3. "Slow cooling of hot polarons in halide perovskite solar cells" ACS Energy Letters 2, 2647 (2017); https://doi.org/10.1021/acsenergylett.7b00862

4. "Dynamic symmetry breaking and spin splitting in metal halide perovskites" Physical Review B 98, 085108 (2018); https://doi.org/10.1103/PhysRevB.98.085108

5. "Performance-limiting nanoscale trap clusters at grain junctions in halide perovskites" Nature 580, 360 (2020); https://doi.org/10.1038/s41586-020-2184-1

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