Computer modelling of novel perovskite halides for next-generation solar cells

a) Brief description of the context of the research

Metal halide perovskites are generating enormous excitement for their use in low-cost, high-performance and scalable photovoltaic (PV) devices. These materials have the general ABX3 structure, where A is a mono-cation (methylammonium, MA; formamidinium, FA; and/or cesium, Cs), B is a di-cation (typically Pb), and X is an anion (typically I or an I/Br mixture). In contrast to crystalline silicon, perovskites offer low-temperature processability and band gap tunability through modifications of the chemical composition. Within 10 years, there has been an unprecedented rise in the power conversion efficiency (PCE) of perovskite solar cells from 3% to over 25%. However, there are significant stability issues and a full understanding of the underpinning defect, ion transport and interfacial properties is incomplete. Hence, we have yet to unlock the full performance potential of these materials.

b) Aims and objectives

This project will address critical challenges of this extraordinary class of material through a multi-faceted computational approach led by Prof Saiful Islam (SI) with the following key objectives:
(i) To elucidate the activation energies and diffusion coefficients for ion migration across multiple compositions (partial A-cation substitution vs mixed I/Br) with comparison to the best-in-class perovskite (FA,Cs)PbI3 as an appropriate reference system.
(ii) To compare and contrast how ion accumulation at the interfaces influence current transport and device stability.
(iii) To elucidate how A-site cation doping and 2D structures can mitigate ion migration and surface reactions, and to formulate design guidelines for optimum compositions, enabling industrial relevance.

c) Novelty of the research methodology

Particular strengths of this project will be (i) the ability to harness a range of density functional theory (DFT) and molecular dynamics (MD) methods (e.g. VASP, LAMMPS codes), (ii) the effective...