Abstract
Self-assembled molecules (SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells (PSCs) due to their low material consumption and simple processing. Herein, we design and synthesize a series of donor-acceptor (D-A) type SAMs (MPA-BT-CA, MPA-BT-BA, and MPA-BT-RA, where MPA is 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline; BT is benzo[c][1,2,5]-thiadiazole; CA is 2-cyanoacrylic acid, BA is benzoic acid, RA is rhodanine-3-propionic acid) with distinct anchoring groups, which show dramatically different properties. MPA-BT-CA with CA anchoring groups exhibited stronger dipole moments and formed a homogeneous monolayer on the indium tin oxide (ITO) surface by adopting an upstanding self-assembling mode. However, the MPA-BT-RA molecules tend to aggregate severely in solid state due to the sp3 hybridization of the carbon atom on the RA group, which is not favorable for achieving a long-range ordered self-assembled layer. Consequently, benefiting from high dipole moment, as well as dense and uniform self-assembled film, the device based on MPA-BT-CA yielded a remarkable power conversion efficiency (PCE) of 21.81%. Encouragingly, an impressive PCE approaching 20% can still be obtained for the MPA-BT-CA-based PSCs as the device area is increased to 0.80 cm2. Our work sheds light on the design principles for developing hole selecting SAMs, which will pave a way for realizing highly efficient, flexible, and large-area PSCs.
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