Temperature dependent reversal of phase segregation in mixed-halide perovskites
Abstract:
Understanding the mechanism of light-induced halide segregation in mixed-halide perovskites is essential for their application in multijunction solar cells. Here, photoluminescence spectroscopy is used to uncover how both increases in temperature and light intensity can counteract the halide segregation process. It is observed that, with increasing temperature, halide segregation in CH3NH3Pb(Br0.4I0.6)3 first accelerates toward ≈290 K, before slowing down again toward higher temperatures. Such reversal is attributed to the trade-off between the temperature activation of segregation, for example through enhanced ionic migration, and its inhibition by entropic factors. High light intensities meanwhile can also reverse halide segregation; however, this is found to be only a transient process that abates on the time scale of minutes. Overall, these observations pave the way for a more complete model of halide segregation and aid the development of highly efficient and stable perovskite multijunction and concentrator photovoltaics.Open-circuit and short-circuit loss management in wide-gap perovskite p-i-n solar cells
Abstract:
In this work, we couple theoretical and experimental approaches to understand and reduce the losses of wide bandgap Br-rich perovskite pin devices at open-circuit voltage (VOC) and short-circuit current (JSC) conditions. A mismatch between the internal quasi-Fermi level splitting (QFLS) and the external VOC is detrimental for these devices. We demonstrate that modifying the perovskite top-surface with guanidinium-Br and imidazolium-Br forms a low-dimensional perovskite phase at the n-interface, suppressing the QFLS-VOC mismatch, and boosting the VOC. Concurrently, the use of an ionic interlayer or a self-assembled monolayer at the p-interface reduces the inferred field screening induced by mobile ions at JSC, promoting charge extraction and raising the JSC. The combination of the n- and p-type optimizations allows us to approach the thermodynamic potential of the perovskite absorber layer, resulting in 1 cm2 devices with performance parameters of VOCs up to 1.29 V, fill factors above 80% and JSCs up to 17 mA/cm2, in addition to a thermal stability T80 lifetime of more than 3500 h at 85 °C.