Titanium oxide (TiO2) has been commonly used as an electron transport layer (ETL) of regular‐structure perovskite solar cells (PSCs), and so far the reported PSC devices with power conversion efficiencies (PCEs) over 21% are mostly based on mesoporous structures containing an indispensable mesoporous TiO2 layer. However, a high temperature annealing (over 450 °C) treatment is mandatory, which is incompatible with low‐cost fabrication and flexible devices. Herein, a facile one‐step, low‐temperature, nonhydrolytic approach to in situ synthesizing amino‐functionalized TiO2 nanoparticles (abbreviated as NH2‐TiO2 NPs) is developed by chemical bonding of amino (‐NH2) groups, via TiN bonds, onto the surface of TiO2 NPs. NH2‐TiO2 NPs are then incorporated as an efficient ETL in n‐i‐p planar heterojunction (PHJ) PSCs, affording PCE over 21%. Cs0.05FA0.83MA0.12PbI2.55Br0.45 (abbreviated as CsFAMA) PHJ PSC devices based on NH2‐TiO2 ETL exhibit the best PCE of 21.33%, which is significantly higher than that of the devices based on the pristine TiO2 ETL (19.82%) and is close to the record PCE for devices with similar structures and fabrication procedures. Besides, due to the passivation of the surface trap states of perovskite film, the hysteresis of current–voltage response is significantly suppressed, and the ambient stability of devices is improved upon amino functionalization.

Organo-metal halide perovskite solar cells based on planar architecture have been reported to achieve remarkably high power conversion efficiency (PCE, >16%), rendering them highly competitive to the conventional silicon based solar cells. A thorough understanding of the role of each component in solar cells and their effects as a whole is still required for further improvement in PCE. In this work, the planar heterojunction-based perovskite solar cells were simulated with the program AMPS (analysis of microelectronic and photonic structures)-1D. Simulation results revealed a great dependence of PCE on the thickness and defect density of the perovskite layer. Meanwhile, parameters including the work function of the back contact as well as the hole mobility and acceptor density in hole transport materials were identified to significantly influence the performance of the device. Strikingly, an efficiency over 20% was obtained under the moderate simulation conditions.

.36%, and 9.18%, which are enhanced by ≈17.5%, 11.6%, and 11.8%, respectively, compared to that of the reference (undoped) devices. The PCE enhancement of the C 3 N 4 QDs doped BHJ-PSC device is found to be primarily attributed to the increase of short-circuit current ( J sc ), and this is confi rmed by external quantum effi ciency (EQE) measurements. The effects of C 3 N 4 QDs on the surface morphology, optical absorption and photoluminescence (PL) properties of the active layer fi lm as well as the charge transport property of the device are investigated, revealing that the effi ciency enhancement of the BHJ-PSC devices upon C 3 N 4 QDs doping is due to the conjunct effects including the improved interfacial contact between the active layer and the hole transport layer due to the increase of the roughness of the active layer fi lm, the facilitated photoinduced electron transfer from the conducting polymer donor to fullerene acceptor, the improved conductivity of the active layer, and the improved charge (hole and electron) transport.