Motivated by the exploration for high-performable sensitizers, in this work six novel organic donor–acceptor–π–spacer–acceptor (D–A–π–A) dyes were designed by inserting auxiliary electron acceptors into the C220 dye, and their photovoltaic performances were predicted by density functional theory (DFT) and time-dependent DFT (TD-DFT) calculations coupled with the charge hopping model. Results revealed that the insertion of auxiliary electron acceptors can clearly stabilize the LUMO, narrow the HOMO–LUMO gap, and remarkably enhance the dye’s optical absorption. Based on the estimation for the rates and efficiencies in charge injection, recombination, and dye regeneration processes, the photoelectric conversion efficiency (PCE) of C220 dye was predicted to be about 10.39% under standard solar radiation, in line with its measured value of 10.1%, suggesting that our calculation scheme is reliable. With the same strategy, the predicted PCE values for the dye 2, 3, and 4, with BTD, BSD and DPP as auxiliary electron acceptors, are as high as 13.17, 14.05 and 15.70%, respectively; illuminating that these three dyes are potential sensitizers for TiO₂ nanocrystalline solar cells, and worth further study by experiments.

出于对高性能敏化剂探索的推动，在这项工作中，通过将辅助电子受体插入C220染料中，设计了六种新颖的有机供体-受体-π-间隔子-受体（D-A-π-A）染料，并设计了光电通过密度泛函理论（DFT）和时变DFT（TD-DFT）计算以及电荷跳跃模型来预测性能。结果表明，插入辅助电子受体可以明显稳定LUMO，缩小HOMO-LUMO间隙，并显着提高染料的光吸收。根据电荷注入，重组和染料再生过程的速率和效率的估计，预计C220染料在标准太阳辐射下的光电转换效率（PCE）约为10.39％，与测量值10.1一致％，说明我们的计算方案是可靠的。采用相同的策略，以BTD，BSD和DPP作为辅助电子受体的染料2、3和4的预测PCE值分别高达13.17％，14.05和15.70％。说明这三种染料是TiO的潜在敏化剂_2个纳米晶太阳能电池，值得通过实验进一步研究。