Excess/unreacted lead iodide (PbI2) has been commonly used in perovskite films for the state‐of‐the‐art solar cell applications. However, an understanding of intrinsic degradation mechanisms of perovskite solar cells (PSCs) containing unreacted PbI2 has been still insufficient and, therefore, needs to be clarified for better operational durability. Here, it is shown that degradation of PSCs is hastened by unreacted PbI2 crystals under continuous light illumination. Unreacted PbI2 undergoes photodecomposition under illumination, resulting in the formation of lead and iodine in films. Thus, this photodecomposition of PbI2 is one of the main reasons for accelerated device degradation. Therefore, this work reveals that carefully controlling the formation of unreacted PbI2 crystals in perovskite films is very important to improve device operational stability for diverse opto‐electronic applications in the future.

In the conventional molecular design of thermally activated delayed fluorescence (TADF) organic emitters, simultaneously achieving a fast rate of reverse intersystem crossing (RISC) from the triplet to the singlet manifold and a fast rate of radiative decay is a challenging task. A number of recent experimental data, however, point to TADF emitters with intramolecular π–π interactions as a potential pathway to overcome the issue. Here, we report a comprehensive investigation of TADF emitters with intramolecular π···π or lone-pair···π noncovalent interactions. We uncover the impact of those intramolecular noncovalent interactions on the TADF properties. In particular, we find that folded geometries in TADF molecules can trigger lone-pair···π interactions, introduce a n → π* character of the relevant transitions, enhance the singlet–triplet spin–orbit coupling, and ultimately greatly facilitate the RISC process. This work provides a robust foundation for the molecular design of a novel class of highly efficient TADF emitters in which intramolecular noncovalent interactions play a critical function.

This work investigates the feasibility of using lowdimensional perovskites for electrically driven lasers given the current status of perovskite light-emitting diodes and optically pumped lasers. In our progress toward electrically driven lasers, we performed a variety of measurements on bulk and lowdimensional perovskite films to give a baseline for expectations. This included the measurement of amplified spontaneous emission, lasing, and near-infrared light-emitting diodes operated at low and high current density. We considered power density thresholds needed for amplified spontaneous emission and lasing and compared this to light-emitting diodes operated at high current density to speculate on the future of electrically driven perovskite lasers. We concluded that our current perovskite devices will need current densities of ∼4 to 10 kA/cm 2 to achieve lasing. Future devices will most significantly benefit from architectures that accommodate higher current, but meaningful reductions in threshold may also come from improved film quality and confinement.

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Three thermally activated delayed fluorescence (TADF) molecules, namely PQ1, PQ2, and PQ3, are composed of electron‐accepting (A) tetrabenzo[a,c]phenazine (TBPZ) and electron‐donating (D) phenoxazine (PXZ) units are designed and characterized. The combined effects of planar acceptor manipulation and high steric hindrance between D and A units endow high molecular rigidity that suppresses nonradiative decay of the excitons with improved photoluminescence quantum yields (PLQYs). Particularly, the well‐aligned excited states involving a singlet and a triplet charge‐transfer excited states and a localized excited triplet state in PQ3 enhances the reverse intersystem crossing rate constant (kRISC) with a short delay lifetime (τd). The orange–red OLED based on PQ3 displays a maximum external EL quantum efficiency (EQE) of 27.4 % with a well‐suppressed EL efficiency roll‐off owing to a completely horizontal orientation of the transition dipole moment in the film state.