Szczuczko Lena, Gałyńska Marta, Kriebel Maximilian H, Tecmer Paweł, Boguslawski Katharina
Institute of Physics, Faculty of Physics, Astronomy, and Informatics, Nicolaus Copernicus University in Toruń, Grudziadzka 5, 87-100 Toruń, Poland.
Faculty of Chemistry, Nicolaus Copernicus University in Toruń, Gagarina 7, 87-100 Toruń, Poland.
J Chem Theory Comput. 2025 May 13;21(9):4506-4519. doi: 10.1021/acs.jctc.5c00186. Epub 2025 Apr 29.
We introduce a new domain-based charge-transfer analysis tool exploiting the locality of pair Coupled Cluster Doubles orbitals. Unique features of the proposed model include the ability to monitor the direction of the charge flow between different parts or moieties of the system and its quantitative evaluation. We assess the predictive power of our new method for selected dye candidates of dye-sensitized solar cells with different doping and structural arrangements and compare our results for excitation and orbital energies to various density functional approximations and the domain-based local pair natural orbital variant of coupled cluster singles doubles. Our work confirms that the dyes with S-doped bridges are the most promising candidates for dye-sensitized solar cells applications, featuring the largest donor → bridge → acceptor directed charge transfer and the most favorable electrodonating and electroaccepting powers.
我们引入了一种新的基于域的电荷转移分析工具，该工具利用了双耦合簇轨道对的局部性。所提出模型的独特特性包括能够监测系统不同部分或基团之间电荷流动的方向及其定量评估。我们评估了我们的新方法对具有不同掺杂和结构排列的染料敏化太阳能电池所选染料候选物的预测能力，并将我们关于激发能和轨道能的结果与各种密度泛函近似以及耦合簇单双激发的基于域的局部对自然轨道变体进行比较。我们的工作证实，具有S掺杂桥的染料是染料敏化太阳能电池应用中最有前景的候选物，具有最大的供体→桥→受体定向电荷转移以及最有利的给电子和吸电子能力。
