Strategy to Boost the Efficiency of Mixed-Ion Perovskite Solar Cells: Changing Geometry of the Hole Transporting Material

The hole transporting material (HTM) is an essential component in perovskite solar cells (PSCs) for efficient extraction and collection of the photoinduced charges. Triphenylamine- and carbazole-based derivatives have extensively been explored as alternative and economical HTMs for PSCs. However, the improvement of their power conversion efficiency (PCE), as well as further investigation of the relationship between the chemical structure of the HTMs and the photovoltaic performance, is imperatively needed. In this respect, a simple carbazole-based HTM X25 was designed on the basis of a reference HTM, triphenylamine-based X2, by simply linking two neighboring phenyl groups in a triphenylamine unit through a carbon-carbon single bond. It was found that a lowered highest occupied molecular orbital (HOMO) energy level was obtained for X25 compared to that of X2. Besides, the carbazole moiety in X25 improved the molecular planarity as well as conductivity property in comparison with the triphenylamine unit in X2. Utilizing the HTM X25 in a solar cell with mixed-ion perovskite [HC(NH2)(2)](0.85)(CH3NH3)(0.15)Pb(I0.85Br0.15)(3), a highest reported PCE of 17.4% at 1 sun (18.9% under 0.46 sun) for carbazole-based HTM in PSCs was achieved, in comparison of a PCE of 14.7% for triphenylamine-based HTM X2. From the steady-state photoluminescence and transient photocurrent/photovoltage measurements, we conclude that (1) the lowered HOMO level for X25 compared to X2 favored a higher open-circuit voltage (V-oc) in PSCs; (2) a more uniform formation of X25 capping layer than X2 on the surface of perovskite resulted in more efficient hole transport and charge extraction in the devices. In addition, the long-term stability of PSCs with X25 is significantly enhanced compared to X2 due to its good uniformity of HTM layer and thus complete coverage on the perovskite. The results provide important information to further develop simple and efficient small molecular HTMs applied in solar cells.