Cy5染料激子相互作用的从头算研究。

Ab Initio Studies of Exciton Interactions of Cy5 Dyes.

作者信息

Fothergill Jenny W, Hernandez Andres C, Knowlton William B, Yurke Bernard, Li Lan

机构信息

Micron School of Materials Science and Engineering , Boise State University , Boise , Idaho 83725 , United States.

Department of Electrical and Computer Engineering , Boise State University , Boise , Idaho 83725 , United States.

出版信息

J Phys Chem A. 2018 Nov 21;122(46):8989-8997. doi: 10.1021/acs.jpca.8b05237. Epub 2018 Nov 9.

DOI:10.1021/acs.jpca.8b05237

PMID:30380862

Abstract

The excited state properties of cyanine dyes and the orientations of their aggregates were studied using density functional theory (DFT). The effects of exchange-correlation functional and solvent model on the absorption spectrum of Cy5 was investigated. Using the 6-31+G(d,p) basis set and B3LYP exchange-correlation functional with IEF-PCM (water) solvent, the predicted spectrum achieved a maximum absorbance within 0.007 eV of experiment. An in-house program based on the theoretical model of Kühn, Renger, and May (KRM), which predicts the orientation of dyes within an aggregate from its absorbance and circular dichroism (CD) spectra or vice versa, was used to investigate the orientation of an experimentally observed dimer. The absorbance spectrum predicted using the KRM model of the dimer structure optimized with the 6-31+G(d,p) basis set, ωB97XD exchange-correlation functional, and IEF-PCM solvent agrees with experimental data.

摘要

利用密度泛函理论（DFT）研究了花菁染料的激发态性质及其聚集体的取向。研究了交换相关泛函和溶剂模型对Cy5吸收光谱的影响。使用6-31+G(d,p)基组和具有IEF-PCM（水）溶剂的B3LYP交换相关泛函，预测光谱在实验值的0.007 eV范围内达到最大吸光度。基于Kühn、Renger和May（KRM）理论模型的内部程序用于研究实验观察到的二聚体的取向，该程序可根据染料聚集体的吸光度和圆二色性（CD）光谱预测其取向，反之亦然。使用6-31+G(d,p)基组、ωB97XD交换相关泛函和IEF-PCM溶剂优化的二聚体结构的KRM模型预测的吸光光谱与实验数据一致。