Prof Henry Snaith FRS

Abstract:

Hysteresis in the current-voltage characteristics of hybrid organic-inorganic perovskite-based solar cells is one of the fundamental aspects of these cells that we do not understand well. One possible cause, suggested for the hysteresis, is polarization of the perovskite layer under applied voltage and illumination bias, due to ion migration within the perovskite. To study this problem systemically, current-voltage characteristics of both regular (light incident through the electron conducting contact) and so-called inverted (light incident through the hole conducting contact) perovskite cells were studied at different temperatures and scan rates. We explain our results by assuming that the effects of scan rate and temperature on hysteresis are strongly correlated to ion migration within the device, with the rate-determining step being ion migration at/across the interfaces of the perovskite layer with the contact materials. By correlating between the scan rate with the measurement temperature, we show that the inverted and regular cells operate in different hysteresis regimes, with different activation energies of 0.28 ± 0.04 eV and 0.59 ± 0.09 eV, respectively. We suggest that the differences observed between the two architectures are due to different rates of ion migration close to the interfaces, and conclude that the diffusion coefficient of migrating ions in the inverted cells is 3 orders of magnitude higher than in the regular cells, leading to different accumulation rates of ions near the interfaces. Analysis of VOC as a function of temperature shows that the main recombination mechanism is trap-assisted (Shockley-Read Hall, SRH) in the space charge region, similar to what is the case for other thin film inorganic solar cells.

Abstract:

Here we study perovskite solar cells based on mesoporous alumina scaffold infiltrated and capped with a perovskite absorber layer, which are devoid of a discrete n-type electron collection layer. We employ ethoxylated polyethylenimine (PEIE) to modify the interface between the perovskite absorber layer and the metallic transparent fluorine-doped SnO 2 (FTO) electrode. Surprisingly, the PEIE interlayer obviates the requirement for the conventional dense-TiO 2 (d-TiO 2 ) compact layer (or organic fullerene layer), usually required to selectively extract electrons from the perovskite film. The self-organized PEIE interlayer produced a strong induced dipole moment at the perovskite-FTO interface, with our results indicating that electrons accumulate within the perovskite film at this interface. The resultant “n-type” contact region within the perovskite absorber layer, progressing to an intrinsic (i) region within the bulk of the perovskite layer, represents an n-i homojunction and favorably enables selective electron extraction at the FTO electrode. Resulting solar cells deliver current-voltage measured power conversion efficiencies (η) of over 15.0% and a substantial stabilized efficiency (η) of 9.1%. Although our solar cell performance remains lower than the highest reported efficiencies for perovskite solar cells employing discrete charge selective extraction layers, it indicates significant potential for “homo-junction” perovskite solar cells, once the metallic-to-perovskite contact is fully controlled. Additionally, our work identifies the potential impact of modifying the interface between the perovskite absorber and the subsequent contact materials with dipolar organic compounds, which may be applicable to optimizing contact at perovskite-semiconductor heterojunctions.

Abstract:

This paper investigates the effect of adding a 450 nm layer based on porous TiO2 at the interface between a 4.5 μm carbon/TiO2 nanoparticle-based electrode and a polymer electrolyte membrane as a route to improve energy storage performance in solid-state supercapacitors. Electrochemical characterisation showed that adding the interface layer reduced charge transfer resistance, promoted more efficient ion transfer across the interface and significantly improved charge/discharge dynamics in a solid-state supercapacitor, resulting in an increased areal capacitance from 45.3 to 111.1 mF cm^2 per electrode at 0.4 mA cm^2.