Organic light emitting diodes (OLED) exhibit remarkable energy efficiency in applications ranging from urban lighting to large-screen display panels. The goal of this research is to eliminate the need for heavy-metal ions by developing a fundamentally new class of all-organic phosphorescent molecules. The principal task is to design molecules in which the juxtaposition of electronic orbitals promotes the processes underlying phosphorescence while at the same time the chemical bonding patterns provide the structural rigidity needed to minimize the non-radiative decay of electronic excitations. To this end an integrative computational-experimental approach is employed, in which molecular simulations, chemical synthesis, and materials characterization are combined in a synergistic and iterative sequence. The expected outcomes of this project are novel environmentally benign phosphorescent materials that are based on sustainable chemistries and that are immediately deployable for lighting applications. The new insights into the functional response of molecular materials gained while perfecting metal-free OLED benefits organic electronics in general, and advance technologies such as photovoltaics, sensors, and displays. Finally, software toolkits, data management utilities, and workflows for simulation-based predictive materials design are established as a new paradigm for materials development.