杂原子掺杂原型有机染料的前沿轨道工程：用于染料敏化太阳能电池
摘要
杂原子掺杂有机染料的计算设计对于染料敏化太阳能电池 (DSSC) 仍具有挑战性，因为预测方法必须准确描述远程电荷转移 (CT) 激发，同时在系统性材料筛选中保持计算效率。在本工作中，我们使用范围分离混合泛函 LC-PBE 结合线性响应时序密度泛函理论 (TDDFT) 于 Tamm-Dancoff 近似 (TDA) 内，考察其电子结构和激发态性质。我们采用简化且物理动机明确的有效调谐协议 () 以实现有机染料电子性质的快速可靠筛选。通过针对 -桥或链路的三个位置进行目标杂原子 (N、O 和 B) 掺杂，分析关键影响光吸收和电子注入的 CT 激发能和前沿轨道对齐。基于卡中乌烃供电器和氰乙烆酸接受器，设计了 27 个单掺、二掺和三掺原型有机染料。 Distinct design trends emerge: electron-rich nitrogen and oxygen dopants increase the HOMO-LUMO gap and blue-shift CT excitations, with nitrogen exhibiting the strongest effect, whereas electron-deficient boron substitution narrows the gap and induces pronounced red shifts. Notably, the BBN-doped dye exhibits the smallest gap and lowest excitation energy, highlighting boron-rich motifs as promising candidates for enhanced solar light harvesting. Overall, this study establishes transferable heteroatom-doping guidelines and introduces an efficient, reliable, and cost-effective tuned DFT-TDDFT framework for high-throughput computational discovery and optimization of DSSC sensitizers.
引用
@article{arxiv.2601.03394,
title = {Frontier Orbital Engineering in Heteroatom-Doped Prototypical Organic Dyes for Dye-Sensitized Solar Cells},
author = {Aditi Singh and Ram Dhari Pandey and Subrata Jana and Prasanjit Samal and Paweł Tecmer and Szymon Śmiga},
journal= {arXiv preprint arXiv:2601.03394},
year = {2026}
}