Bart Roose

Migration of cations induces reversible performance losses over day/night cycling in perovskite solar cells

Perovskites have been demonstrated in solar cells with a power conversion efficiency of well above 20%, which makes them one of the strongest contenders for next generation photovoltaics. While there are no concerns about their efficiency, very little is known about their stability under illumination and load. Ionic defects and their migration in the perovskite crystal lattice are some of the most alarming sources of degradation, which can potentially prevent the commercialization of perovskite solar cells (PSCs). In this work, we provide direct evidence of electric field-induced ionic defect migration and we isolate their effect on the long-term performance of state-of-the-art devices. Supported by modelling, we demonstrate that ionic defects, migrating on timescales significantly longer (above 103 s) than what has so far been explored (from 10−1 to 102 s), abate the initial efficiency by 10–15% after several hours of operation at the maximum power point. Though these losses are not negligible, we prove that the initial efficiency is fully recovered when leaving the device in the dark for a comparable amount of time. We verified this behaviour over several cycles resembling day/night phases, thus probing the stability of PSCs under native working conditions. This unusual behaviour reveals that research and industrial standards currently in use to assess the performance and the stability of solar cells need to be adjusted for PSCs. Our work paves the way for much needed new testing protocols and figures of merit specifically designed for PSCs.

Identifying and suppressing interfacial recombination to achieve high open-circuit voltage in perovskite solar cells

With close to 100% internal quantum efficiency over the absorption spectrum, photocurrents in perovskite solar cells (PSCs) are at their practical limits. It is therefore imperative to improve open-circuit voltages (VOC) in order to go beyond the current 100 mV loss-in-potential. Identifying and suppressing recombination bottlenecks in the device stack will ultimately drive the voltages up. In this work, we investigate in depth the recombination at the different interfaces in a PSC, including the charge selective contacts and the effect of grain boundaries. We find that the density of grain boundaries and the use of tunneling layers in a highly efficient PSC do not modify the recombination dynamics at 1 sun illumination. Instead, the recombination is strongly dominated by the dopants in the hole transporting material (HTM), spiro-OMeTAD and PTAA. The reduction of doping concentrations for spiro-OMeTAD yielded VOCs as high as 1.23 V in contrast to PTAA, which systematically showed slightly lower voltages. This work shows that a further suppression of non-radiative recombination is possible for an all-low-temperature PSC, to yield a very low loss-in-potential similar to GaAs, and thus paving the way towards higher than 22% efficiencies.

A Ga-doped SnO2 mesoporous contact for UV stable highly efficient perovskite solar cells

Increasing the stability of perovskite solar cells is a major challenge for commercialization. The highest efficiencies so far have been achieved in perovskite solar cells employing mesoporous TiO2 (m-TiO2). One of the major causes of performance loss in these m-TiO2-based perovskite solar cells is induced by UV-radiation. This UV instability can be solved by replacing TiO2 with SnO2; thus developing a mesoporous SnO2 (m-SnO2) perovskite solar cell is a promising approach to maximise efficiency and stability. However, the performance of mesoporous SnO2 (m-SnO2) perovskite solar cells has so far not been able to rival the performance of TiO2 based perovskite solar cells. In this study, for the first time, high-efficiency m-SnO2 perovskite solar cells are fabricated, by doping SnO2 with gallium, yielding devices that can compete with TiO2 based devices in terms of performance. We found that gallium doping severely decreases the trap state density in SnO2, leading to a lower recombination rate. This, in turn, leads to an increased open circuit potential and fill factor, yielding a stabilised power conversion efficiency of 16.4%. The importance of high-efficiency m-SnO2 based perovskite solar cells is underlined by stability data, showing a marked increase in stability under full solar spectrum illumination.