Reducing Energy Disorder of Hole Transport Layer by Charge Transfer Complex for High Performance p-i-n Perovskite...

Solution-processed organic semiconductor charge-transport layers (OS-CTLs) with high mobility, low trap density, and energy level alignment have dominated the important progress in p-i-n planar perovskite solar cells (pero-SCs). Unfortunately, their inevitable long chains result in weak molecular stacking, which is likely to generate high energy disorder and deteriorate the charge-transport ability of OS-CTLs. Here, a charge-transfer complex (CTC) strategy to reduce the energy disorder in the OS-CTLs by doping an organic semiconductor, 4,4'-(4,8-bis(5-(trimethylsilyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl)bis(N,N-bis(4-methoxyphenyl)aniline) (BDT-Si), in a commercial hole-transport layer (HTL), poly[bis(4-phenyl) (2,4,6-trimethylphenyl)amine (PTAA), is proposed. The formation of the CTC makes the PTAA conjugated backbone electron-deficient, resulting in a quinoidal and stiffer character, which is likely to planarize the PTAA backbone and enhance the ordering of the film in nanoscale. The resultant HTL exhibits a reduced energy disorder, which simultaneously promotes hole transport in the HTL, hole extraction at the interface, energy level alignment, and quasi-Fermi level splitting in the device. As a result, the p-i-n planar pero-SCs with optimized HTL exhibit the best power conversion efficiency of 21.87% with good operating stability. This finding demonstrates that the CTC strategy is an effective way to reduce the energy disorder in HTLs and to improve the performance of planar pero-SCs.