Contactless Series Resistance Imaging of Perovskite Solar Cells via Inhomogeneous Illumination

A contactless effective series resistance imaging method for large area perovskite solar cells that is based on photoluminescence imaging with non-uniform illumination is introduced and demonstrated experimentally. The proposed technique is applicable to partially and fully processed perovskite solar cells if laterally conductive layers are present. The capability of the proposed contactless method to detect features with high effective series resistance is validated by comparison with various contacted mode luminescence imaging techniques. The method can reliably provide information regarding the severeness of the detected series resistance through photo-excitation pattern manipulation. Application of the method to sub-cells in monolithic tandem devices, without the need for electrical contacting the terminals, appears feasible.Comment: 17 pages, 5 figure

Anomalous structural evolution and glassy lattice in mixed-halide hybrid perovskites

Hybrid halide perovskites have emerged as highly promising photovoltaic materials because of their exceptional optoelectronic properties, which are often optimized via compositional engineering like mixing halides. It is well established that hybrid perovskites undergo a series of structural phase transitions as temperature varies. In this work, the authors find that phase transitions are substantially suppressed in mixed-halide hybrid perovskite single crystals of MAPbI3-xBrx (MA = CH3NH3+ and x = 1 or 2) using a complementary suite of diffraction and spectroscopic techniques. Furthermore, as a general behavior, multiple crystallographic phases coexist in mixed-halide perovskites over a wide temperature range, and a slightly distorted monoclinic phase, hitherto unreported for hybrid perovskites, is dominant at temperatures above 100 K. The anomalous structural evolution is correlated with the glassy behavior of organic cations and optical phonons in mixed-halide perovskites. This work demonstrates the complex interplay between composition engineering and lattice dynamics in hybrid perovskites, shedding new light on their unique properties.Peer ReviewedPostprint (published version

Thermal Disorder-Induced Strain and Carrier Localization Activate Reverse Halide Segregation.

Publication status: PublishedFunder: Australian Government; doi: http://dx.doi.org/10.13039/100015539Funder: Government of Western Australia; doi: http://dx.doi.org/10.13039/501100011025The reversal of halide ions is studied under various conditions. However, the underlying mechanism of heat-induced reversal remains unclear. This work finds that dynamic disorder-induced localization of self-trapped polarons and thermal disorder-induced strain (TDIS) can be co-acting drivers of reverse segregation. Localization of polarons results in an order of magnitude decrease in excess carrier density (polaron population), causing a reduced impact of the light-induced strain (LIS - responsible for segregation) on the perovskite framework. Meanwhile, exposing the lattice to TDIS exceeding the LIS can eliminate the photoexcitation-induced strain gradient, as thermal fluctuations of the lattice can mask the LIS strain. Under continuous 0.1 W cm⁻2 illumination (upon segregation), the strain disorder is estimated to be 0.14%, while at 80 °C under dark conditions, the strain is 0.23%. However, in situ heating of the segregated film to 80 °C under continuous illumination (upon reversal) increases the total strain disorder to 0.25%, where TDIS is likely to have a dominant contribution. Therefore, the contribution of entropy to the system's free energy is likely to dominate, respectively. Various temperature-dependent in situ measurements and simulations further support the results. These findings highlight the importance of strain homogenization for designing stable perovskites under real-world operating conditions