P3HT/钙钛矿异质结构中的组分与表面终止对能带排列的调控

中文摘要 AI 辅助

杂化有机-无机钙钛矿异质结构是能量转换和光电器件的新兴平台，然而组分和表面终止对能带排列的影响仍知之甚少。在此，我们利用高通量第一性原理计算，系统地揭示了组分和表面终止对由聚(3-己基噻吩)(P3HT)变体与常规及混合阳离子金属卤化物钙钛矿形成的820种异质结构能带排列的影响。能带边缘分析预测了浓度依赖的能带排列，大多数基于Pb和Sn的钙钛矿表现出Type II和Type III行为，而混合阳离子CsMASnBr3独特地与所有P3HT变体形成Type-I结。显式界面计算表明，表面终止可以逆转常规锡钙钛矿中预测的排列，而混合阳离子钙钛矿无论终止如何均保持与P3HT的Type-I排列。尽管电荷转移可忽略不计，终止依赖的能带偏移产生了显著不同的载流子限制，为工程化P3HT/钙钛矿界面确立了设计原则。

英文摘要

Hybrid organic-inorganic perovskite heterostructures are emerging platforms for energy conversion and optoelectronic devices, yet the effects of composition and surface terminations on band alignment remain poorly understood. Here, using high-throughput first-principles calculations, we systematically reveal the effect of composition and surface termination on the band alignment of 820 heterostructures formed between poly(3-hexylthiophene) (P3HT) variants and conventional and mixed-cation metal halide perovskites. Band edge analysis predicts concentration dependent band alignments, with most Pb and Sn based perovskites exhibiting Type II and III behavior while mixed-cation CsMASnBr3 uniquely forms Type-I junctions with all P3HT variants. Explicit interface calculations reveal that surface termination can reverse the predicted alignment in conventional tin perovskites, while the mixed cation perovskite preserves Type-I alignment with P3HT regardless of termination. Despite negligible charge transfer, termination dependent band offsets produce markedly different carrier confinement, establishing design principles for engineering P3HT/perovskite interfaces.

发表机构

• Faculty of Engineering and Natural Sciences, Sabanci University（萨班哲大学工程与自然科学学院）
• Materials Science and Nano Engineering Program, Sabanci University（萨班哲大学材料科学与纳米工程项目）

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