论文标题
配体的定向自我组装散装有机 - 气门/量子点混合膜可实现三胞胎激子的定量收获
Ligand Directed Self-Assembly of Bulk Organic-Semiconductor/Quantum-Dot Blend Films Enables Near Quantitative Harvesting of Triplet Excitons
论文作者
论文摘要
有机半导体中发生的激子乘法过程Singlet Pission(SF)提供了一种打破单频隙光伏(PV)中的冲击式式式限制的方法。如果可以将SF产生的三胞胎激子转移到无机量子点(QDS)中,则可以将基于SF的光子乘法辐射重组,从而将单个高能光子转换为两个低功能的光子。这样的SF光子乘法膜(SF-PMF)可以将最佳SI-PV的效率从26.7%提高到32.5%。但是,在这样的薄膜中,需要精确的纳米级形态,该薄膜由有机相的适当形态组成,允许有效的SF,其中QD发射器在数十nm长度尺度上很好地分散以实现有效收获三联。然而,由于其大小,形状和表面能的不匹配,有机-QD混合物中的个体组件具有聚集和相分离的趋势,这是一个长期存在的问题。在这里,我们使用具有电子活性的高度溶剂半导体配体的QD表面工程方法,该方法与SF材料相匹配,这使我们能够指导自组装工艺屈服于具有良好的QD和最小聚集的溶液处理膜,如X射线和中子和中子和电子显微镜表征,表现为最小。稳态和时间分辨的光谱表明,在有机相-QD界面上,膜在有机相和定量三重态转移中支持有效的SF(190%的产率),从而导致95%的三胞胎激子被QD收获。我们的结果将SF-PMF建立为一种高度有希望的结构,以利用SF工艺来提高PV效率,并提供了一种高度用途的方法来克服有机半导体与QD的混合在一起的挑战。
Singlet fission (SF), an exciton multiplication process occurring in organic semiconductors, offers a way to break the Shockley-Queisser limit in single-bandgap photovoltaics (PV). If the triplet excitons generated by SF can be transferred to inorganic quantum dots (QDs), where they radiatively recombine, SF based photon multiplication is achieved, converting a single high-energy photon into two low-energy photons. Such a SF photon multiplication film (SF-PMF) could raise the efficiency of the best Si-PV from 26.7% to 32.5%. But a precise nanoscale morphology is required within such a film consisting of the appropriate morphology for the organic phase, allowing for efficient SF, within which the QD emitters are well dispersed on a tens of nm length scale to enable efficient harvesting of the triplets. However, it has been a long-standing problem that the individual components in organic-QD blends have a tendency to aggregate and phase separate, due to a mismatch of their size, shape and surface energies. Here, we demonstrate a QD surface engineering approach using an electronically active, highly soluble semiconductor ligand that is matched to the SF material, which allows us to direct the self-assembly process yielding solution processed films with well-dispersed QDs and minimal aggregation, as characterised by X-ray and neutron scattering and electron microscopy. Steady state and time-resolved optical spectroscopy show that the films support efficient SF (190% yield) in the organic phase and quantitative triplet energy transfer across the organic-QD interface, resulting in 95% of the triplet excitons being harvested by the QDs. Our results establish the SF-PMF as a highly promising architecture to harness the SF process to enhance PV efficiencies, and also provide a highly versatile approach to overcome challenges in the blending of organic semiconductors with QDs.