Polyvinyl pyrrolidone (PVP) is doped to PbI2 and organic salt during two‐step growth of halideperovskite. It is observed that PVP molecules can interact with both PbI2 and organic salt, reduce the aggregation and crystallization of the two, and then slow down the coarsening rate of perovskite. As doping concentration increases from 0 to 1 mM in organic salt, average crystallite size of perovskite decreases monotonously from 90 to 34 nm; Surface fluctuation reduces from 259.9 to 179.8 nm at first, and then increases; Similarly, surface roughness decreases from 45.55 to 26.64 nm at first, and then rises. Accordingly, a kind of “confinement effect” is resolved to crystallite growth and surface fluctuation/roughness, which helps to build compact and uniform perovskite film. Density of trap states (t‐DOS) is cut down by ≈60% at moderate doping  (0.2 mM). Due to the “confinement effect”, power conversion efficiency of perovskite solar cells is improved from 19.46 (±2.80) % to 21.50 (±0.99) %, and further improved to 24.11% after surface modification. Meanwhile, “confinement effect” strengthens crystallite/grain boundaries and improves thermal stability of both film and device. T80 of device increases to 120 h, compared to 50 h for reference ones.

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This work investigates the photovoltaic properties of polymers that include different carbazole blocks as electron donors (D) but the same benzothiadiazole derivative as the electron acceptor (A). Five D–A copolymers are studied with ultrafast intramolecular exciton splitting and recombination dynamics to acquire the single-molecule structure and their photovoltaic performance relationship. The photovoltaic parameters such as energy level, optical band gap, and light-harvesting ability are highly dependent on the molecular structure of the donor monomer (including their appended flexible alkyl chain). Branched or linear alkyl groups on the same D block obviously vary the polymer steady-state absorption spectra and film morphology. For organic solar cells, this work allows tuning and control of the ultrafast dynamics, implying photovoltaic material design in the future.

Improving efficiency and stability has become an urgent issue in the application of perovskite solar cells (PSCs). Herein, a kind of long‐chain polymer or polymethylmethacrylate (PMMA) is added into the spiro‐OMeTAD matrix to improve the film formation process and hence the device performance. It is observed that, after modification, the spiro‐OMeTAD‐based hole‐transporting layer becomes uniform, continuous, and condensed. Meanwhile, the power conversion efficiency of the devices is upgraded. Compared with the control device, open‐circuit voltage of the modified one (with moderate doping) increases from 1.06 (±0.03) to 1.10 (±0.02) V, fill factor increases from 72.20 (±3.44)% to 75.59 (±3.35)%, and the power conversion efficiency increases from 18.82 (±1.06)% to 20.51 (±0.82)% (highest at 21.78%) under standard test condition (AM 1.5G, 100 mW cm−2). Transient photocurrent/photovoltage decay curves, time‐resolved photoluminance, and impedance spectroscopy studies show that the modification could accelerate charge transfer and retard interfacial recombination. In addition, the modification improves device stability. Due to the strengthened barrier against penetration of “H2O/O2/Ag,” the efficiency of the unsealed device could retain 91.49% (by average) of the initial one after 100 days storage in the dark [relative humidity = 30(±5)%]. This work shows that long‐chain polymer doping could simultaneously improve efficiency and stability of spiro‐OMeTAD‐based PSCs.

SnO2 modified mesoporous ZrO2 is used to replace the mesoporous TiO2 layer and serves as a kind of mesoporous electron-transport layer during the low-temperature fabrication of mesoscopic perovskite solar cells that are based on carbon electrode. X-ray/ultraviolet photoelectron spectroscopy studies and electrical test observe that SnO2 modification brought down the work function while increasing the conductivity of the mesoporous ZrO2. Transient photovoltage/photocurrent decay curves, impedance spectroscopy, and photoluminescence mapping show that after the bottom layer of ZrO2 is modified by SnO2, the charge extraction process is accelerated while recombination is retarded. This modification helps to increase the power conversion efficiency from 4.70 (±0.85)% to 10.15 (±0.35)%, along with the optimized efficiency at 13.37% (AM1.5G, 100 mW/cm2) for the low-temperature devices. In addition, the effects of modification layers of SnO2 on the power conversion properties are carefully studied. This study shows that SnO2 modified mesoporous ZrO2 could serve as an efficient electron-transport layer for the low-temperature mesoscopic devices.