A σ-Hole''-Containing Volatile Solid Additive Enabling 16.5% Efficiency Organic Solar Cells

Here we introduce a sigma-hole-containing volatile solid additive, 1, 4-diiodotetrafluorobenzene (A3), in PM6:Y6-based OSCs. Aside from the appropriate volatility of A3 additive, the synergetic halogen interactions between A3 and photoactive matrix contribute to more condensed and ordered molecular arrangement in the favorable interpenetrating donor/acceptor domains. As a result, greatly accelerated charge transport process with suppressed charge recombination possibility is observed and ultimately a champion PCE value of 16.5% is achieved. Notably, the A3 treated OSCs can maintain a high efficiency of over 16.0% in a wide concentration range of A3 additive between 10 and 35 mg/mL. The A3-treated device shows excellent stability with an efficiency of 15.9% after 360-h storage. This work demonstrates that the sigma-hole interaction can be applied to enhance the OSC performance and highlights the importance of non-covalent interactions in the optoelectronic materials.