Low‐cost solution‐processed CdTe nanocrystal (NC) solar cells always suffer from a high interface energy barrier and unbalanced hole/electron transport as well as anisotropic atom diffusion on the CdTe surface due to the limited amount of hole/electron interface materials or the difficulty in interface processing. In this work, a novel strategy is first adopted with gradient electron transport layer (CdS/CdSe) modification in the cathode and a new crosslinkable hole transport polymer (P‐TPA) implantation in the anode. The carrier recombination at interfaces is greatly decreased and thus the carrier collection is increased. Moreover, the light harvesting is improved both in short and long wavelength regions, making Jsc and Voc increase simultaneously. A champion solar cell shows a very high power conversion efficiency of 9.2% and an outstanding Jsc of 25.31 mA cm−2, which are among the highest values for all solution‐processed CdTe NC solar cells with a superstrate structure, and the latter value is even higher than that of traditional thick CdTe thin‐film solar cells (2 µm) via the high temperature close space sublimation method. This work demonstrates that facile surface modifications in both the cathode and anode with stepped extraction and organic–inorganic hybridization are very promising in constructing next‐generation highly efficient NC photovoltaic devices.

Simultaneous enhancement of photoluminescence quantum efficiency (PLQE) and optical gain in semiconducting polymer films is desirable for optically‐ or electrically‐pumped organic solid‐state lasers. In this work, a simple self‐dilution effect is achieved by introducing a small amount (≈10% by weight) of 2,5‐dimethyl‐1,4‐phenylene (DP) units in the backbone of poly(9,9‐dioctylfluorene) (PFO). The resulting copolymers, compared with PFO (PLQE 39%), exhibit a significantly increased PLQE (66%) while keeping similar absorption and photoluminescence profile, concomitant with an enhancement in optical gain properties. The radiative decay rate increases sharply along with a sustaining reduction in the non‐radiative decay rate in these copolymers, following similar principle of physical dilution of a luminescent compound in solution or in a polymer matrix. Among all the copolymers, the one containing 10% DP units exhibits the lowest amplified spontaneous emission/distributed feedback laser threshold (10.9 nJ/1.4 nJ, eightfold reduction), and the highest gain coefficient (54.4 cm−1). The results demonstrate that a moderate DP/fluorene ratio can maximize the beneficial self‐dilution effects. These investigations shed light on new design strategies to achieve conjugated polymers with concurrent high PLQE and large optical gain properties.

Large and rigid substituents may facilitate the improvement of the color purity of polyfluorenes.

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