Core/Shell Nanocrystal Tailored Carrier Dynamics in Hysteresisless Perovskite Solar Cells with ∼20% Efficiency and Long Operational Stability.

The ambient stability, hysteresis, and trap states in organo-halide perovskite solar cells (PSCs) are correlated to the influence of interlayer interfaces and grain boundaries. Astute incorporation of Cu2ZnSnS4 (CZTS) and Au/CZTS core/shell nanocrystals (NCs) can realize the goal of simultaneously achieving better performance and ambient stability of the PSCs. With optimized Au/CZTS NC size and concentration in the photoactive layer, power conversion efficiency can be increased up to 19.97 ± 0.6% with ambient air stability >800 h, as compared to 14.46 ± 1.02% for the unmodified devices. Through efficient carrier generation by CZTS and perovskite, accompanied by the plasmonic effect of Au, carrier density is sufficiently increased as validated by transient absorption spectroscopy. NCs facilitate the interfacial charge transfer by suitable band alignment and removal of recombination centers such as metallic Pb0, surface defects, or impurity sites. NC embedding also increases the perovskite grain size and assists in pinhole filling, reducing the trap state density.

All-inorganic quantum dot assisted enhanced charge extraction across the interfaces of bulk organo-halide perovskites for efficient and stable pin-hole free perovskite solar cells.

In spite of achieving high power conversion efficiency (PCE), organo-halide perovskites suffer from long term stability issues. Especially the grain boundaries of polycrystalline perovskite films are considered as giant trapping sites for photo-generated carriers and therefore play an important role in charge transportation dynamics. Surface engineering via grain boundary modification is the most promising way to resolve this issue. A unique antisolvent-cum-quantum dot (QD) assisted grain boundary modification approach has been employed for creating monolithically grained, pin-hole free perovskite films, wherein the choice of all-inorganic CsPbBr x I3-x (x = 1-2) QDs is significant. The grain boundary filling by QDs facilitates the formation of compact films with 1-2 µm perovskite grains as compared to 300-500 nm grains in the unmodified films. The solar cells fabricated by CsPbBr1.5I1.5 QD modification yield a PCE of ∼16.5% as compared to ∼13% for the unmodified devices. X-ray photoelectron spectral analyses reveal that the sharing of electrons between the PbI6 - framework in the bulk perovskite and Br- ions in CsPbBr1.5I1.5 QDs facilitates the charge transfer process while femtosecond transient absorption spectroscopy (fs-TAS) suggests quicker trap filling and enhanced charge carrier recombination lifetime. Considerable ambient stability up to ∼720 h with <20% PCE degradation firmly establishes the strategic QD modification of bulk perovskite films.