Triplet transfer from PbS quantum dots to tetracene ligands: is faster always better?
Triplet transfer from PbS quantum dots to tetracene ligands: is faster always better?
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DOI：
10.1039/d2tc03470k
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发表时间：
2022-11-10
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量子点-有机半导体杂化材料作为自旋混合器正获得越来越多的关注，其应用范围从太阳能收集到自旋存储器。无机量子点（QD）和有机半导体之间的三重态能量转移是开发这些应用的关键步骤。在这里，我们报告的三重态能量转移从PbS量子点到四个能量和结构相似的并四苯配体。即使有类似的配体，我们发现三重态能量转移动力学可以显着变化。对于TIPS-并四苯衍生物与羧酸，乙酸和methanethethylene锚定基团的短pro-cata侧，我们发现，三重态转移发生通过一个逐步的过程中，介导的表面状态，而单取代的TIPS-并四苯衍生物5-（4-苯甲酸）-12-三异丙基甲硅烷基乙炔基并四苯（BAT）三重态转移直接发生，虽然较慢，通过德克斯特交换机制。尽管BAT的三重态转移较慢，但总产率较高，如使用红荧烯发射体从上转换发射测定的。这项工作强调了表面介导的转移机制受到寄生损失途径的困扰，并且具有直接Dexter样三联体转移的材料优选用于高效应用。我们报告了从PbS量子点到四个能量和结构相似的并四苯配体的三重态能量转移，即使具有相似的配体，我们发现三重态能量转移动力学可以显着变化。
Quantum dot-organic semiconductor hybrid materials are gaining increasing attention as spin mixers for applications ranging from solar harvesting to spin memories. Triplet energy transfer between the inorganic quantum dot (QD) and organic semiconductor is a key step to understand in order to develop these applications. Here we report on the triplet energy transfer from PbS QDs to four energetically and structurally similar tetracene ligands. Even with similar ligands we find that the triplet energy transfer dynamics can vary significantly. For TIPS-tetracene derivatives with carboxylic acid, acetic acid and methanethiol anchoring groups on the short pro-cata side we find that triplet transfer occurs through a stepwise process, mediated via a surface state, whereas for monosubstituted TIPS-tetracene derivative 5-(4-benzoic acid)-12-triisopropylsilylethynyl tetracene (BAT) triplet transfer occurs directly, albeit slower, via a Dexter exchange mechanism. Even though triplet transfer is slower with BAT the overall yield is greater, as determined from upconverted emission using rubrene emitters. This work highlights that the surface-mediated transfer mechanism is plagued with parasitic loss pathways and that materials with direct Dexter-like triplet transfer are preferred for high-efficiency applications. We report the triplet energy transfer from PbS QDs to four energetically and structurally similar tetracene ligands, even with similar ligands we find that the triplet energy transfer dynamics can vary significantly.
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