| Abstract Scope |
Dye molecules can absorb and emit light, demonstrating biomedical imaging, organic photovoltaics, non-linear optics, and quantum information applications. These applications can be manipulated by dye structure features, properties, and aggregation ability. Dye aggregate networks via deoxyribonucleic acid (DNA) templating exhibit exciton delocalization, energy transport, and fluorescence emission. To control the process and optimize the dye structures and properties, we have combined density functional theory-based methods and molecular dynamics. The ground- and excited-state properties of the dyes, such as transition dipole moment, static dipole difference, absorption spectrum, and solvation energy, were calculated. The dye aggregate-DNA interactions and dye orientations were predicted. We found the effects of varying hydrophobic substituents (i.e., functional groups) on the dyes. Substitution can also impact the resultant performance of the DNA-templated dye aggregate through augmenting the electron withdrawing or donating strength of the substituents on the dye. The computational results were validated with experimental observations. |