Prof Henry Snaith FRS

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.

Abstract:

Direct bandgap perovskite and indirect bandgap Si, which form the two active layers in a tandem solar cell configuration, have different optoelectronic properties and thicknesses. The charge-carrier dynamics of the two-terminal perovskite-on-Si tandem solar cell in response to a supercontinuum light pulse is studied using transient photocurrent (TPC) measurements. Spectral dependence of TPC lifetime is observed and can be classified into two distinct timescales based on their respective carrier generation regions. The faster timescale (∼500 ns) corresponding to the spectral window (300-750 nm) represents the top-perovskite sub-cell, while the slower timescale regime of ∼25 μs corresponds to the bottom-Si sub-cell (>700 nm). Additionally, under light-bias conditions, the transient carrier dynamics of the perovskite sub-cell is observed to be coupled with that of the Si sub-cell. A sharp crossover from the fast-response to a slow-response of the device as a function of the light-bias intensity is observed. These results along with a model based on transfer matrix formulation highlight the role of charge-carrier dynamics in accessing higher efficiencies in tandem solar cells. The carrier transit times and lifetimes in addition to their optical properties need to be taken into account for optimizing the performance.