Upconversion at Solid/Liquid Interfaces Using Perovskite Single Crystal Triplet Sensitizers
Upconversion at Solid/Liquid Interfaces Using Perovskite Single Crystal Triplet Sensitizers
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DOI：
10.1021/acs.chemmater.3c02778
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发表时间：
2024-02-06
影响因子：
8.6
通讯作者：
Nienhaus，Lea
中科院分区：
文献类型：
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作者：
Moller，Gregory;Sullivan，Colette M.;Nienhaus，Lea
钙钛矿敏化的光子上转换（UC）具有通过将两个低能量光子转换成较高能量的单个光子来改进包括光子晶体学和光子晶体学的广泛技术的潜力。迄今为止，钙钛矿敏化UC已经通过使用溶液中的纳米晶体和使用多晶钙钛矿膜的固态薄膜双层进行了研究。虽然在薄膜双层中已经实现了有效的UC，但是由于单个钙钛矿晶粒和晶界引起的表面不均匀性和缺陷可能限制整体性能。然而，固态UC中的主要问题之一是由于不利的分子间相互作用和竞争弛豫途径，固态中可行的三重态零化子的数量有限。在这里，我们调查的混合阳离子甲基铵甲脒三碘化铅钙钛矿单晶的性质，使用X射线衍射和光谱学和随后的掺入和性能作为三重态敏化剂的三重态-三重态湮灭在溶液基红荧烯。与混合固态/溶液的方法，这里提出的，广泛的潜在的零化子可以迅速被筛选。此外，钙钛矿单晶的更高的表面均匀性和数量级更低的缺陷密度和更高的稳定性允许对界面电荷转移过程的潜在改进和由于减少的载流子捕获而增加的UC性能。
Perovskite-sensitized photon upconversion (UC) has the potential to improve a wide range of technologies including photocatalysis and photovoltaics, by converting two low energy photons into a single photon of higher energy. To date, perovskite-sensitized UC has been studied by using nanocrystals in solution and solid-state thin film bilayers using polycrystalline perovskite films. While efficient UC has been achieved in thin film bilayers, surface inhomogeneities and defects due to individual perovskite crystal grains and grain boundaries may limit the overall performance. However, one of the main issues in solid-state UC is a limited number of viable triplet annihilators in the solid-state due to unfavorable intermolecular interactions and competing relaxation pathways. Here, we investigate the properties of mixed cation methylammonium formamidinium lead triiodide perovskite single crystals using X-ray diffraction and optical spectroscopy and their subsequent incorporation and performance as triplet sensitizers for triplet–triplet annihilation in solution-based rubrene. With the hybrid solid-state/solution approach presented here, a wide number of potential annihilators can be rapidly be screened. In addition, the higher surface homogeneity and orders of magnitude lower defect densities and higher stability of perovskite single crystals allow for potential improvements to interfacial charge transfer processes and increases in UC performance due to reduced carrier trapping.