Hybrid perovskites incorporating conjugated organic cations enable unusual charge carrier interactions among organic and inorganic structural components, but are difficult to prepare as films due to disparate component chemical/physical characteristics (e.g., solubility, thermal stability). Here we demonstrate that resonant infrared matrix-assisted pulsed laser evaporation (RIR-MAPLE) mitigates these challenges, enabling facile deposition of lead-halide-based perovskite films incorporating variable-length oligothiophene cations. Density functional theory (DFT) predicts suitable organic and inorganic moieties that form quantum-well-like structures with targeted luminescence or exciton separation/quenching. RIR-MAPLE-deposited films enable confirmation of these predictions by optical measurements, which further display excited state behavior transcending traditional quantum-well models—i.e., with appropriate selection of specially synthesized organic/inorganic moieties, intercomponent carrier transfer efficiently converts excitons from singlet to triplet states in organics for which intersystem crossing cannot ordinarily compete with recombination. These observations demonstrate the uniquely versatile excited-state behavior in hybrid perovskite quantum wells, and the value of integrating DFT, organic synthesis, RIR-MAPLE and spectroscopy for screening/preparing rationally devised complex structures.

中文翻译：

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通过共振红外矩阵辅助脉冲激光蒸发沉积的合理设计的基于低聚物的钙钛矿薄膜中的可调谐内部量子阱对准†

掺入共轭有机阳离子的钙钛矿杂化物使有机和无机结构组分之间发生异常的载流子相互作用，但由于组分的化学/物理特性不同（例如，难于制备成膜），溶解度，热稳定性）。在这里，我们证明了共振红外矩阵辅助脉冲激光蒸发（RIR-MAPLE）减轻了这些挑战，使掺入可变长度的低聚噻吩阳离子的基于卤化铅的钙钛矿薄膜的沉积变得容易。密度泛函理论（DFT）预测合适的有机和无机部分，这些部分形成具有定向发光或激子分离/猝灭的量子阱状结构。使用RIR-MAPLE沉积的薄膜可以通过光学测量来确认这些预测，从而进一步显示超越传统量子阱模型的激发态行为，即与专门合成的有机/无机部分的适当选择，组件间载体传输有效地转换从单线到三重态激子中的有机物为其中间窜越不能通常与重组竞争。这些观察结果证明了在混合钙钛矿量子阱中独特的通用激发态行为，以及集成DFT，有机合成，RIR-MAPLE和光谱学对于筛选/制备合理设计的复杂结构的价值。