Dataset of "Tuning the morphology and energy levels in organic solar cells with metal- organic framework nanosheets"

Metal-organic framework nanosheets (MONs) have proved themselves to be usefuladditives for enhancing the performance of a variety of thin film solar cell devices. However,to date only isolated examples have been reported. In this work we take advantage of themodular structure of MONs in order to resolve the effect of their different structural andoptoelectronic features on the performance of organic photovoltaic (OPV) devices. Threedifferent MONs were synthesized using different combinations of two porphyrin-based ligandsmeso-tetracarboxyphenyl porphyrin (TCPP) or tetrapyridyl-porphyrin (TPyP) with either zincand/or copper ions and the effect of their addition to polythiophene-fullerene (P3HT-PCBM)OPV devices was investigated. The power conversion efficiency (PCE) of devices was found toapproximately double with the addition of MONs of Zn2(ZnTCPP), but was unchanged withthe addition of Cu2(ZnTPyP) and halved upon the addition of Cu2(CuTCPP) compared todevices without nanosheets. Our analysis indicates that there are three different mechanismsby which MONs can influence the photoactive layer – light absorption, energy level alignment,and morphological changes. Analysis of external quantum efficiency, UV-vis photoelectronspectroscopy data found that MONs have similar effects on light absorption and energy levelalignment. However, atomic force and Raman microscopy studies revealed that the nanosheetthickness and lateral size are crucial parameters in enabling the MONs to act as beneficialadditives resulting in an improvement of the OPV device performance. We anticipate thisstudy will aid in the design of MONs and other 2D materials for future use in other lightharvesting and emitting devices.

金属有机框架纳米片（Metal-organic framework nanosheets, MONs）已被证实可作为有效添加剂，用于提升各类薄膜太阳能电池器件的性能。然而截至目前，相关研究仅报道过孤立的案例。本研究利用MONs的模块化结构，旨在阐明其不同结构与光电子特性对有机光伏（Organic Photovoltaic, OPV）器件性能的影响。本研究通过两种卟啉基配体——介四羧基苯基卟啉（meso-tetracarboxyphenyl porphyrin, TCPP）与四吡啶基卟啉（tetrapyridyl-porphyrin, TPyP）——分别与锌、铜离子或其组合，合成了三种不同的MONs，并探究了将其掺入聚噻吩-富勒烯（P3HT-PCBM）型OPV器件后对器件性能的影响。研究发现，相较于未添加纳米片的器件，掺入Zn₂(ZnTCPP)型MONs的器件的功率转换效率（Power Conversion Efficiency, PCE）提升约一倍；掺入Cu₂(ZnTPyP)型MONs的器件性能无明显变化；而掺入Cu₂(CuTCPP)型MONs的器件性能则下降一半。本研究分析表明，MONs可通过三种不同机制影响器件活性层：光吸收调控、能级对齐调控与形貌调控。对外量子效率、紫外-可见光电子能谱数据的分析显示，MONs对光吸收与能级对齐的影响较为相似。但原子力显微镜与拉曼显微镜研究表明，纳米片的厚度与横向尺寸是决定MONs能否作为有益添加剂并提升OPV器件性能的关键参数。本研究有望为MONs及其他二维材料的设计提供指导，助力其未来应用于各类光捕获与发光器件中。