Thesis advisor: Torsten Fiebig / This dissertation introduces a new field of DNA photonics centering on the electronic properties of DNA, which emerges after the initial controversies regarding the long-range conductivity and wire-type behavior of DNA have been widely settled. DNA photonics study is not solely focused on charge transfer phenomena but encompasses all possible photophysical processes and their potentially complex interplays. For instance, ultrafast electronic energy migration, dissipation, and (de)localization on the femtosecond time scale are shown to be crucial for the description of light-induced dynamics in DNA and have been thoroughly investigated in this dissertation. In addition to measurements on natural single and double-stranded DNA, this dissertation also presents experimental data on a series of functionalized DNA systems (derivatized by stilbene, ethidium, 2-aminopurine, etc.), obtained by state-of-the-art femtosecond broadband pump–probe spectroscopy. The results illustrate the distance dependence of charge transfer, emphasize the role of the initial electronic excitation on energy transfer dynamics, and highlight the influence of structural factors on both processes in DNA. Finally, as one initial step towards DNA electronics application, a DNA mimicking system of tertiary arylureas were employed to demonstrate molecular wire behavior, implying its potential use in molecular electronics. Thus, both the experimental and theoretical research accumulated for DNA π–π coupling can be translated into designing and testing various molecular systems with similar π-stacked structures. / Thesis (PhD) — Boston College, 2008. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Chemistry.