Modifed Becke-Johnson exchange potential: improved modelling of lead halides for solar cell applications

TL;DR

This paper demonstrates that using a modified Becke-Johnson exchange potential in density functional theory yields highly accurate predictions of lead halide properties relevant for solar cells, and explores how cation substitution can enhance their optical absorption.

Contribution

It introduces a modified Becke-Johnson exchange potential for improved modeling of lead halides and predicts beneficial effects of cation substitution on solar cell materials.

Findings

Excellent agreement with experimental data for lead halides.

Cation substitution can significantly reduce band gaps.

Potential for near-infrared absorption in modified compounds.

Abstract

We report first-principles calculations, within density functional theory, on the lead halide compounds PbCl2, PbBr2, and CH3NH3PbBr3-xClx, taking into account spin-orbit coupling. We show that, when the modified Becke-Johnson exchange potential is used with a suitable choice of defining parameters, excellent agreement between calculations and experiment is obtained. The computational model is then used to study the effect of replacing the methylammonium cation in CH3NH3PbI3 and CH3NH3PbBr3 with either N2H+5 or N2H+3, which have slightly smaller ionic radii than methylammonium. We predict that a considerable downshift in the values of the band gaps occurs with this replacement. The resulting compounds would extend optical absorption down to the near-infrared region, creating excellent light harvesters for solar cells.