Yinan Chen

Abstract:

Layered organic-inorganic halide perovskites exhibit remarkable structural and chemical diversity and hold great promise for optoelectronic devices. In these materials, excitons are thought to be strongly confined within the inorganic metal halide layers with interlayer coupling generally suppressed by the organic cations. Here, we present an in-depth study of the energy and spatial distribution of the lowest-energy excitons in layered organic-inorganic halide perovskites from first-principles many-body perturbation theory, within the GW approximation and the Bethe-Salpeter equation. We find that the quasiparticle band structures, linear absorption spectra, and exciton binding energies depend strongly on the distance and the alignment of adjacent metal halide perovskite layers. Furthermore, we show that exciton delocalization can be modulated by tuning the interlayer distance and alignment, both parameters determined by the chemical composition and size of the organic cations. Our calculations establish the general intuition needed to engineer excitonic properties in novel halide perovskite nanostructures.

Abstract:

Halogen mixing in lead-halide perovskites is an effective route for tuning the band gap in light emission and multijunction solar cell applications. Here we report the effect of halogen mixing on the optoelectronic properties of lead-halide perovskites from theory and experiment. We applied the virtual crystal approximation within density functional theory, the <i>GW</i> approximation, and the Bethe-Salpeter equation to calculate structural, vibrational, and optoelectronic properties for a series of mixed halide perovskites. We separately perform spectroscopic measurements of these properties and analyze the impact of halogen mixing on quasiparticle band gaps, effective masses, absorption coefficients, charge-carrier mobilities, and exciton binding energies. Our joint theoretical-experimental study demonstrates that iodide-bromide mixed-halide perovskites can be modeled as homovalent alloys, and local structural distortions do not play a significant role for the properties of these mixed species. Our study outlines a general theoretical-experimental framework for future investigations of novel chemically mixed systems.