Multiscale Modeling of Electronic Excitations in Branched Conjugated Molecules Using an Exciton Scattering Approach

The exciton scattering (ES) approach attributes excited electronic states in quasi-1D branched polymer molecules to standing waves of quantum quasiparticles (excitons) scattered at the molecular vertices. We extract their dispersion and frequency-dependent scattering matrices at termini, ortho, and meta joints for pi-conjugated phenylacetylene-based molecules from atomistic time-dependent density-functional theory (TD DFT) calculations. This allows electronic spectra for any structure of arbitrary size within the considered molecular family to be obtained with negligible numerical effort. The agreement is within 10-20 meV for all test cases, when comparing the ES results with the reference TD DFT calculations.