Impact of Precursor Concentration on Perovskite Crystallization for Efficient Wide-Bandgap Solar Cells.

High-crystalline-quality wide-bandgap metal halide perovskite materials that achieve superior performance in perovskite solar cells (PSCs) have been widely explored. Precursor concentration plays a crucial role in the wide-bandgap perovskite crystallization process. Herein, we investigated the influence of precursor concentration on the morphology, crystallinity, optical property, and defect density of perovskite materials and the photoelectric performance of solar cells. We found that the precursor concentration was the key factor for accurately controlling the nucleation and crystal growth process, which determines the crystallization of perovskite materials. The precursor concentration based on Cs0.05FA0.8MA0.15Pb(I0.84Br0.16)3 perovskite was controlled from 0.8 M to 2.3 M. The perovskite grains grow larger with the increase in concentration, while the grain boundary and bulk defect decrease. After regulation and optimization, the champion PSC with the 2.0 M precursor concentration exhibits a power conversion efficiency (PCE) of 21.13%. The management of precursor concentration provides an effective way for obtaining high-crystalline-quality wide-bandgap perovskite materials and high-performance PSCs.

A Cost-Effective Alpha-Fluorinated Bithienyl Benzodithiophene Unit for High-Performance Polymer Donor Material.

To reduce synthetic cost of the classic fluorinated bithienyl benzodithiophene (BDTT-F) unit, here, an alpha-fluorinated bithienyl benzodithiophene unit, namely, α-BDTT-F (F atom in the α position of the lateral thiophene unit), is developed by the isomerization strategy of exchanging the positions of the F atom and flexible alkyl chain on the lateral thiophene unit of the BDTT-F unit. The α-BDTT-F unit was synthesized with less synthetic steps, higher synthetic yield, and less purification times from the same raw materials as those of the BDTT-F unit, thus with low synthetic cost. Theoretical calculation indicates that the α-BDTT-F unit possesses a similar twisted conformation and electronic structures as those of the BDTT-F unit. The α-BDTT-F-based polymer α-PBQ10 exhibits similar light absorption and energy levels as those of the corresponding BDTT-F-based polymer PBQ10 but marginally increased molecular aggregation and stronger hole transport than PBQ10. In consequence, the α-PBQ10:Y6-based polymer solar cell demonstrates a slightly enhanced power conversion efficiency (PCE) of 16.26% compared with that of the PBQ10:Y6-based device (PCE = 16.23%). Also, the PCE is further improved to 16.77% through subtle microscopic morphology regulation of the photoactive layer with the fullerene derivative indene-C60 bisadduct as the third component. This work provides new ideas for the design of low-cost and high-efficiency photovoltaic molecules.

High Efficiency Polymer Solar Cells with Efficient Hole Transfer at Zero Highest Occupied Molecular Orbital Offset between Methylated Polymer Donor and Brominated Acceptor.

Achieving efficient charge transfer at small frontier molecular orbital offsets between donor and acceptor is crucial for high performance polymer solar cells (PSCs). Here we synthesize a new wide band gap polymer donor, PTQ11, and a new low band gap acceptor, TPT10, and report a high power conversion efficiency (PCE) PSC (PCE = 16.32%) based on PTQ11-TPT10 with zero HOMO (the highest occupied molecular orbital) offset (ΔEHOMO(D-A)). TPT10 is a derivative of Y6 with monobromine instead of bifluorine substitution, and possesses upshifted lowest unoccupied molecular orbital energy level (ELUMO) of -3.99 eV and EHOMO of -5.52 eV than Y6. PTQ11 is a derivative of low cost polymer donor PTQ10 with methyl substituent on its quinoxaline unit and shows upshifted EHOMO of -5.52 eV, stronger molecular crystallization, and better hole transport capability in comparison with PTQ10. The PSC based on PTQ11-TPT10 shows highly efficient exciton dissociation and hole transfer, so that it demonstrates a high PCE of 16.32% with a higher Voc of 0.88 V, a large Jsc of 24.79 mA cm-2, and a high FF of 74.8%, despite the zero ΔEHOMO(D-A) value between donor PTQ11 and acceptor TPT10. The PCE of 16.32% is one of the highest efficiencies in the PSCs. The results prove the feasibility of efficient hole transfer and high efficiency for the PSCs with zero ΔEHOMO(D-A), which is highly valuable for understanding the charge transfer process and achieving high PCE of PSCs.

Achieving Fast Charge Separation and Low Nonradiative Recombination Loss by Rational Fluorination for High-Efficiency Polymer Solar Cells.

Four low-cost copolymer donors of poly(thiophene-quinoxaline) (PTQ) derivatives are demonstrated with different fluorine substitution forms to investigate the effect of fluorination forms on charge separation and voltage loss (Vloss ) of the polymer solar cells (PSCs) with the PTQ derivatives as donor and a A-DA'D-A-structured molecule Y6 as acceptor. The four PTQ derivatives are PTQ7 without fluorination, PTQ8 with bifluorine substituents on its thiophene D-unit, PTQ9, and PTQ10 with monofluorine and bifluorine substituents on their quinoxaline A-unit respectively. The PTQ8- based PSC demonstrates a low power conversion efficiency (PCE) of 0.90% due to the mismatch in the highest occupied molecular orbital (HOMO) energy levels alignment between the donor and acceptor. In contrast, the devices based on PTQ9 and PTQ10 show enhanced charge-separation behavior and gradually reduced Vloss , due to the gradually reduced nonradiative recombination loss in comparison with the PTQ7-based device. As a result, the PTQ10-based PSC demonstrates an impressive PCE of 16.21% with high open-circuit voltage and large short-circuit current density simultaneously, and its Vloss is reduced to 0.549 V. The results indicate that rational fluorination of the polymer donors is a feasible method to achieve fast charge separation and low Vloss simultaneously in the PSCs.