Snaith group

Abstract:

Metal halide perovskites have emerged as one of the most promising materials for photovoltaics (PVs), with power conversion efficiency of over 22% already demonstrated. In order to compete with traditional crystalline silicon PV, cost and stability are equally important issues that need to be considered besides efficiency. Copper thiocyanate (CuSCN) is an interesting candidate to be used as an inexpensive, thermally stable p-type charge conducting material in perovskite solar cells. Here, we report 13% efficient perovskite solar cells employing CuSCN as the hole-transport material. We compare the stability of cells employing CuSCN with those employing the archetypical organic hole-transporter 2,2′,7,7′-Tetrakis (N,N-di-p-methoxyphenyl-amine) 9,9′-Spirobifluorene (Spiro-OMeTAD), under elevated temperature in ambient atmosphere. Surprisingly, we find that the devices employing CuSCN degrade faster under elevated temperatures than the devices employing Spiro-OMeTAD. We discover that an interfacial degradation mechanism occurs at the heterojunction between the perovskite absorber and the CuSCN, even in a dry nitrogen atmosphere, identifying the presence of a critical instability. Interestingly, with the additional coating of the completed cells with a thin film of insulating poly(methyl methacrylate) (PMMA), functioning as a rudimentary “on-cell” encapsulation, we significantly alleviate this issue and deliver efficient perovskite solar cells which survive for more than 1000 hours at 85 °C in air with only 25% degradation in performance. Beyond identifying a critical area to address in order to enable CuSCN to be useful for long term operation in perovskite solar cells, our findings indicate that the role of the “encapsulant” is to both keep the environment out, and keep degradation products within the cell.

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.