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Interfacial Trap-Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid-State Upconversion

机译:铅卤化物钙玻璃溶剂辅助三联体产生敏感的固态上变化

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摘要

Photon upconversion via triplet-triplet annihilation (TTA) has promise for overcoming the Shockley-Queisser limit for single-junction solar cells by allowing the utilization of sub-bandgap photons. Recently, bulk perovskites have been employed as sensitizers in solid-state upconversion devices to circumvent poor exciton diffusion in previous nanocrystal (NC)-sensitized devices. However, an in-depth understanding of the underlying photophysics of perovskite-sensitized triplet generation is still lacking due to the difficulty of precisely controlling interfacial properties of fully solution-processed devices. In this study, interfacial properties of upconversion devices are adjusted by a mild surface solvent treatment, specifically altering perovskite surface properties without perturbing the bulk perovskite. Thermal evaporation of the annihilator precludes further solvent contamination. Counterintuitively, devices with more interfacial traps show brighter upconversion. Approximately an order of magnitude difference in upconversion brightness is observed across different interfacial solvent treatments. Sequential charge transfer and interfacial trap-assisted triplet sensitization are demonstrated by comparing upconversion performance, transient photoluminescence dynamics, and magnetic field dependence of the devices. Incomplete triplet conversion from transferred charges and consequent triplet-charge annihilation (TCA) are also observed. The observations highlight the importance of interfacial control and provide guidance for further design and optimization of upconversion devices using perovskites or other semiconductors as sensitizers.
机译:通过Triollet-Triollinni穿剂(TTA)的光子上转换具有克服单结太阳能电池的震撼批次限制,允许利用子带隙光子。最近,散装钙酯已在固态上变化装置中作为敏化剂,以在先前的纳米晶(NC) - 敏化装置中规避不良的激子扩散。然而,由于难以精确地控制完全解决方案处理装置的界面性能,仍然缺乏对钙钛矿敏化三联代代产生的潜在光学药物的深入了解。在该研究中,通过温和的表面溶剂处理调节上变化装置的界面性能,特别是改变钙钛矿表面性质而不会对散装钙钛进行扰动。 Annihilator的热蒸发排除了进一步的溶剂污染。违反直觉地,具有更多界面陷阱的设备显示更明亮的上变化。在不同的界面溶剂处理中观察到升高亮度的大约幅度差异。通过比较升高的性能,瞬态光致发光动态和器件的磁场依赖性,证明了顺序电荷转移和界面陷阱辅助三重态致敏。来自转移电荷的不完全三态转换和随后的三态电荷湮灭(TCA)也被观察到。观察结果突出了界面控制的重要性,并提供了使用Perovskites或其他半导体作为敏感剂的进一步设计和优化的指导。

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