Three azahelicene derivatives with electron-rich bis(4-methoxyphenyl)amino or bis(p-methoxyphenyl)aminophenyl groups at the terminals were deliberately designed, synthesized, and characterized as hole-transporting materials (HTMs) for perovskite solar cells (PSCs). Optical and thermal properties, energy level alignments, film morphologies, hole extraction ability, and hole mobility were studied in detail. PSCs using the newly synthesized molecules as HTMs were fabricated. A maximum power conversion efficiency (PCE) of 17.34% was observed for the bis(p-methoxyphenyl)amino-substituted derivative (SY1) and 16.10% for the bis(p-methoxyphenyl)aminophenyl-substituted derivative (SY2). Longer-chain substituent such as hexyloxy group greatly diminishes the efficiency. In addition, the dopant-free devices fabricated with SY1 as the HTM shows an average PCE of 12.13%, which is significantly higher than that of spiro-OMeTAD (7.61%). The ambient long-term stability test revealed that after 500 h, the devices prepared from SY1 and SY2 retained more than 96% of its initial performance, which is much improved than the reference device with standard spiro-OMeTAD as the HTM under the same conditions. Detailed material cost analysis reveals that the material cost for SY1 is less than 8% of that for spiro-OMeTAD. These results provide a useful direction for designing a new class of HTMs to prepare highly efficient and more durable PSCs.
Three new donor−acceptor−donor type (D−A−D) hole-transporting materials (HTMs), YC-1−YC-3, based on the 4-dicyanomethylene-4Hcyclopenta [2,1-b;3,4-b′]dithiophene (DiCN-CPDT) core structure endowed with two arylamino-based units as peripheral groups were designed, synthesized, and applied in perovskite solar cells (PSCs). Hole mobility, steady-state photoluminescence, thin-film surface morphology on top of the perovskite layer, and photovoltaic performance for the YC series were systematically investigated and compared with those of Spiro-OMeTAD. It was found that YC-1 exhibited more efficient hole transport and extraction characteristics at the perovskite/HTM interface. Meanwhile, the film of YC-1 showed a homogeneous and dense capping layer coverage on the perovskite layer without any pinholes, leading to the improvement of the fill factor and open circuit voltage. The PSC device based on YC-1 as a HTM exhibited a high power conversion efficiency (PCE) of 18.03%, which is comparable to that of the device based on the benchmark Spiro-OMeTAD (18.14%), and also a better long-term stability with 85% of the initial efficiency retained in excess of 500 h under the condition of 30% relative humidity, presumably due to the hydrophobic nature of the material. This work demonstrates that the dicyanomethylene-CPDT-based derivatives are promising HTMs for efficient and stable PSCs.
The
power conversion efficiency (PCE) of perovskite solar cells
has been showing rapid improvement in the last decade. However, still,
there is an unarguable performance deficit compared with the Schockley–Queisser
(SQ) limit. One of the major causes for such performance discrepancy
is surface and grain boundary defects. They are a source of nonradiative
recombination in the devices that not only causes performance loss
but also instability of the solar cells. In this study, we employed
a direct postsurface passivation strategy at mild temperatures to
modify perovskite layer defects using tetraoctylammonium chloride
(TOAC). The passivated perovskite layers have demonstrated extraordinary
improvement in photoluminescence and charge carrier lifetimes compared
to their control counterparts in both Cs0.05(FAPbI3)0.83(MAPbBr3)0.17 and MAPbI3-type perovskite layers. The investigation on electron-only
and hole-only devices after TOAC treatment revealed suppressed electron
and hole trap density of states. The electrochemical study demonstrated
that TOAC treatment improved the charge recombination resistance of
the perovskite layers and reduced the charge accumulation on the surface
of perovskite films. As a result, perovskite solar cells prepared
by TOAC treatment showed a champion PCE of 21.24% for the Cs0.05(FAPbI3)0.83(MAPbBr3)0.17-based device compared to 19.58% without passivation. Likewise, the
PCE of MAPbI3 improved from 18.09 to 19.27% with TOAC treatment.
The long-term stability of TOAC-passivated perovskite Cs0.05(FAPbI3)0.83(MAPbBr3)0.17 devices has retained over 97% of its initial performance after 720
h in air.
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