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Two-dimensional (2D) Ruddlesden-Popper hybrid organic-inorganic perovskites are the most promising candidates for highly efficient optoelectronic devices due to their remarkable exciton characteristics, adjustable band structure and long-term environmental stability. However, excitons emission behavior of 2D Ruddlesden-Popper perovskites is still unclear. Here we theoretically-experimentally decoupled the excitons behavior in 2D Ruddlesden-Popper PEA 2 PbI 4 nanosheets. Theoretically, the Elliott theory was used to separate exciton and band edge absorptions of PEA 2 PbI 4 nanosheets and determine an exciton binding energy of about 274 meV. Experimentally, spectral-dependent photoluminescence lifetime and excitation powder density-dependent photoluminescence spectra revealed that a distinct photoluminescence tail emission should be derived from localized excitons with lower emission energy than free excitons. Further, the luminescent component of the free excitons and localized excitons with their corresponding densities of states was theoretically decoupled by line-shape analysis of PEA 2 PbI 4 nanosheets photoluminescence spectra, which is consistent with the experimental results demonstrating the existence of localized excitons. Hence, our work provides understanding on the exciton behavior and luminescence mechanism of 2D Ruddlesden-Popper perovskites, which would benefit the prediction of high-performance excitonic devices based on 2D Ruddlesden-Popper perovskites. • Excitons behavior in 2D Ruddlesden-Popper PEA 2 PbI 4 nanosheets was decoupled. • A band tail state emission derived from localized excitons. • The luminescent component of the free excitons and localized excitons was separated. [ABSTRACT FROM AUTHOR]

• The electron injection of ETL/perovskite of PeLEDs at molecular level is studied. • The molecular planarity bridging effects are discovered. • Superior molecular planarity of ETL enhances electron transport ability of ETL. • Superior molecular planarity of ETL improves carrier injection of ETL/perovskite. • Superior molecular planarity of ETL leads to superior performances of PeLEDs. Effectively balancing carrier injection of perovskite LEDs (PeLEDs) for next-generation display and illumination urgently needs for molecularly understanding carrier injection behavior of electron transport layer (ETL)/perovskite toward further developing high performance PeLEDs. Here, we molecularly reveal the electron injection behaviors of PeLEDs by theoretically-experimentally decoupling the electron transport of ETLs and electron injection of TmPyPB/perovskite and TPBi/perovskite. Resulted, the better molecular planarity bridging effect (MPBE) of TmPyPB than TPBi can effectively increase electronic-coupling for the improved electron transport ability and significantly decrease injection barrier for the enhanced electron injection capability, intrinsically leading to a more balanced carrier injection and a less electron accumulation of PeLEDs. Compared to TPBi-based PeLEDs, the TmPyPB-based PeLEDs present the obviously-increased average EQE, current efficiency, power efficiency and luminance by 44 %, 63 %, 43 % and 100 %, respectively. Meanwhile, this PeLED shows a higher voltage tolerance characteristic of 7.5 V than that of TPBi-based PeLEDs (6.25 V). Therefore, this work may provide a fundamental insight into carrier injection behavior of PeLEDs for effectively-regulating its carrier injection balance and further for its greatly-facilitated commercialization. [ABSTRACT FROM AUTHOR]