Enhanced Interface Compatibility by Ionic Dendritic Molecules To Achieve Efficient and Stable Perovskite Solar Cells.

Poly(3-hexylthiophene) (P3HT) represents a promising hole transport material for emerging perovskite solar cells (PSCs) due to its appealing merits of high thermal stability and appropriate hydrophobicity. Nonetheless, large energy losses at the P3HT/perovskite interface lead to unsatisfied efficiency and stability of the devices. Herein, two ionic dendritic molecules, 3,3'-(2,7-bis(3,6-bis(bis(4-methoxyphenyl)amino)-9H-carbazol-9-yl)-9H-fluorene-9,9-diyl)bis(N,N,N-trimethylpropan-1-aminium) iodide and 3,3'-(2,7-bis(bis(4-(bis(4-methoxyphenyl)amino)phenyl)amino)-9H-fluorene-9,9-diyl)bis(N,N,N-trimethylpropan-1-aminium) iodide, namely, MPA-Cz-FAI and MPA-PA-FAI, are rationally designed as the interlayer to enhance interfacial compatibility. The dendritic backbone with conjugated structure endows the hole transport layer with high conductivity, derived from the more ordered microstructure with larger crystallization and higher connectivity of domain zones. Besides, a better energy level alignment is established between P3HT and perovskite, which enhances the charge extraction and transport yield. In addition, the peripheral methoxy groups enable effective defect passivation at the interface to suppress nonradiative recombination and the quaternary ammonium iodide serving as side chains enable efficient interfacial hole extraction contributing to enhanced charge collection yield. As a result, the dopant-free P3HT-based PSCs modified with MPA-Cz-PAI deliver a champion efficiency of 19.7%, significantly higher than that of the control devices (15.4%). More encouragingly, the unencapsulated devices demonstrate competitive environmental stability by retaining over 85% of its initial efficiency after 1500 h of storage under humid conditions (70% relative humidity). This work provides an effective molecular design strategy for interface engineering, envisaging a bright prospect for the further development of efficient and stable perovskite solar cells.

Sequential Molecule-Doped Hole Conductor to Achieve >23% Perovskite Solar Cells with 3000-Hour Operational Stability.

Although hole transport layers (HTLs) based on solution-processed doped Spiro-OMeTAD are extremely popular and effective for their remarkable performance in n-i-p perovskite solar cells (PSCs), their scalable application is still being held back by poor chemical stability and unsatisfied scalability. Essentially, the volatile components and hygroscopic nature of ionic salts often cause morphological deformation that deteriorate both device efficiency and stability. Herein, a simple and effective molecular implantation-assisted sequential doping (MISD) approach is strategically introduced to modulate spatial doping uniformity of organic films and fabricate all evaporated Spiro-OMeTAD layer in which phase-segregation free HTL is achieved accompanied with high molecular density, uniform doping composition, and superior optoelectronic characteristics. The resultant MISD-based devices attain a record power conversion efficiency (PCE) of 23.4%, which represents the highest reported value among all the PSCs with evaporated HTLs. Simultaneously, the unencapsulated devices realize considerably enhanced stability by maintaining over 90% of their initial PCEs in the air for 5200 h and after working at maximum power point under illumination for 3000 h. This method provides a facile way to fabricate robust and reliable HTLs toward developing efficient and stable perovskite solar cells.