π-stacked organic electronic materials are tunable light absorbers with many potential applications in optoelectronics. The optical properties of such molecules are highly dependent on the nature and energy of electron–hole pairs or excitons formed upon light absorption, which in turn are determined by intra- and intermolecular electronic and vibrational excitations. Here, we present a first-principles approach for describing the optical spectrum of stacked organic molecules with strong vibronic coupling. For stacked perylene tetracarboxylic acid diimides, we describe optical excitations by using the time-dependent density functional theory with a Franck–Condon Herzberg–Teller approximation of vibronic effects and validate our approach with comparison to experimental ultraviolet–visible (UV–vis) absorption measurements of solvated model systems. We determine that for larger macromolecules, unlike for single molecules, the sampling of the ground-state potential energy surface significantly influences the optical absorption spectrum. We account for this effect by applying our analysis to ∼100 structures extracted from equilibrated molecular dynamics simulations and averaging the optical spectrum over the entire ensemble. Additionally, we demonstrate that intermolecular electronic coupling within the stacks results in multiple low-energy electronically excited states that all contribute to the optical spectrum. This study provides a computationally feasible recipe for describing the spectroscopic properties of stacked organic chromophores via first-principles density functional theory.

We report a general, modular, and high yield route to quinoline-based functional materials for applications in organic electronics.

This study describes the synthesis of modular diquinolineanthracene and polydiquinolineanthracene derivatives. The reported facile and scalable aza-Diels-Alder-based approach requires mild conditions, proceeds in two steps, uses commercially available starting materials, and accommodates varying functionalities. Given the known utility of the acene and quinoline motifs, the synthesized molecules and polymers hold promise for organic electronics applications.

Advanced molecular electronic components remain vital for the next generation of miniaturized integrated circuits. Thus, much research effort has been devoted to the discovery of lossless molecular wires, for which the charge transport rate or conductivity is not attenuated with length in the tunneling regime. Herein, we report the synthesis and electrochemical interrogation of DNA-like molecular wires. We determine that the rate of electron transfer through these constructs is independent of their length and propose a plausible mechanism to explain our findings. The reported approach holds relevance for the development of high-performance molecular electronic components and the fundamental study of charge transport phenomena in organic semiconductors.

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Advanced molecular electronic components remain vital for the next generation of miniaturized integrated circuits. Thus,muchresearcheffort has been devoted to the discovery of lossless molecular wires,for whichthe charge transport rate or conductivity is not attenuated with length in the tunneling regime.H erein, we report the synthesis and electrochemical interrogation of DNA-like molecular wires.W edetermine that the rate of electron transfer through these constructs is independent of their length and propose aplausible mechanism to explain our findings.The reported approach holds relevance for the development of high-performance molecular electronic components and the fundamental study of charge transport phenomena in organic semiconductors.