Enhanced Carrier Diffusion Enables Efficient Back-Contact Perovskite Photovoltaics.

Back-contact architectures offer a promising route to improve the record efficiencies of perovskite solar cells (PSCs) by eliminating parasitic light absorption. However, the performance of back-contact PSCs is limited by inadequate carrier diffusion in perovskite. Here, we report that perovskite films with a preferred out-of-plane orientation show improved carrier dynamic properties. With the addition of guanidine thiocyanate, the films exhibit carrier lifetimes and mobilities increased by 3-5 times, leading to diffusion lengths exceeding 7 µm. The enhanced carrier diffusion results from substantial suppression of nonradiative recombination and improves charge collection. Devices using such films achieve reproducible efficiencies reaching 11.2 %, among the best performances for back-contact PSCs. Our findings demonstrate the impact of carrier dynamics on back-contact PSCs and provide the basis for a new route to high-performance back-contact perovskite optoelectronic devices at low cost.

Solvent Engineering of a Dopant-Free Spiro-OMeTAD Hole-Transport Layer for Centimeter-Scale Perovskite Solar Cells with High Efficiency and Thermal Stability.

High efficiency and environmental stability are mandatory performance requirements for commercialization of perovskite solar cells (PSCs). Herein, efficient centimeter-scale PSCs with improved stability were achieved by incorporating an additive-free 2,2',7,7'-tetrakis[N,N-di(p-methoxyphenyl)amino]-9,9'-spirobifluorene (spiro-OMeTAD) hole-transporting material (HTM) through simply substituting the usual chlorobenzene solvent with pentachloroethane (PC). A stabilized power conversion efficiency (PCE) of 16.1% under simulated AM 1.5G 1 sun illumination with an aperture of 1.00 cm2 was achieved for PSCs using an additive-free spiro-OMeTAD layer cast from PC. X-ray analysis suggested that chlorine radicals from PC transfer partially to spiro-OMeTAD and are retained in the HTM layer, resulting in conductivity improvement. Moreover, unencapsulated PSCs with a centimeter-scale active area cast from PC retained >70% of their initial PCE after ageing at 80 °C for 500 h, in contrast with less than 20% retention for control devices. Morphological and X-ray analyses of the aged cells revealed that the perovskite and HTM layers remain almost unchanged in the cells with a spiro-OMeTAD layer cast from PC whereas serious degradation occurred in the control cells. This study not only reveals the decomposition mechanism of PSCs in the presence of HTM additives but also opens up a broad range of organic semiconductors for radical doping.

Multiple Roles of Cobalt Pyrazol-Pyridine Complexes in High-Performing Perovskite Solar Cells.

Chemical doping is a ubiquitously applied strategy to improve the charge-transfer and conductivity characteristics of spiro-OMeTAD, a hole-transporting material (HTM) used widely in solution-processed perovskite solar cells (PSCs). Cobalt(III) complexes are commonly employed HTM dopants, whose major role is to oxidize spiro-OMeTAD to provide p-doping for improved conductivity. The present work discloses additional, previously unknown important functions of cobalt complexes in the HTM films that influence the photovoltaic performance. Specifically, it is demonstrated that commercial p-dopant FK269 (bis(2,6-di(1H-pyrazol-1-yl)pyridine) cobalt(III) tris(bis(trifluoromethylsulfonyl)imide)) reduces the interfacial recombination and alleviates the decomposition of the perovskite layer under the action of tert-butylpyridine and lithium bis(trifluoromethanesulfonyl)imide. These effects are demonstrated for 1 cm2 perovskite solar cells that achieve a stabilized power conversion efficiency of 19% under 1 sun irradiation.