Unraveling the Impact of Hole Transport Materials on Photostability of Perovskite Films and p-i-n Solar Cells

We investigated the impact of a series of hole transport layer (HTL) materials such as Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT: PSS), NiOx, poly[bis(4-phenyl)(2,4,6-trimethylphenyl)-amine (PTAA), and polytriarylamine (PTA) on photostability of thin films and solar cells based on MAPbI(3), Cs(0.15)FA(0.85)PbI(3), Cs(0.1)MA(0.15)FA(0.75)PbI(3), Cs(0.1)MA(0.15)FA(0.75)Pb(Br0.15I0.85)(3), and Cs(0.15)FA(0.85)Pb(Br0.15I0.85)(3) complex lead halides. Mixed halide perovskites showed reduced photostability in comparison with similar iodide-only compositions. In particular, we observed light-induced recrystallization of all perovskite films except MAPbI(3) with the strongest effects revealed for Br-containing systems. Moreover, halide and beta FAPbI(3) phase segregations were also observed mostly in mixed-halide systems. Interestingly, coating perovskite films with the PCBM layer spectacularly suppressed light-induced growth of crystalline domains as well as segregation of Br-rich and I-rich phases or beta FAPbI(3). We strongly believe that all three effects are promoted by the light-induced formation of surface defects, which are healed by adjacent PCBM coating. While comparing different hole-transport materials, we found that NiOx and PEDOT:PSS are the least suitable HTLs because of their interfacial (photo)chemical interactions with perovskite absorbers. On the contrary, polyarylamine-type HTLs PTA and PTAA form rather stable interfaces, which makes them the best candidates for durable p-i-n perovskite solar cells. Indeed, multilayered ITO/PTA(A)/MAPbI(3)/PCBM stacks revealed no aging effects within 1000 h of continuous light soaking and delivered stable and high power conversion efficiencies in solar cells. The obtained results suggest that using polyarylamine-type HTLs and simple single-phase perovskite compositions pave a way for designing stable and efficient perovskite solar cells.