Unraveling the Charge-Carrier Dynamics from the Femtosecond to the Microsecond Time Scale in Double-Cable Polymer-Based Single-Component Organic Solar Cells

Single-component organic solar cells (SCOSCs) have witnessed great improvement during the last few years with the champion efficiency jumping from the previous 2-3% to currently 6-11% for the representative material classes. However, the photophysics in many of these materials has not been sufficiently investigated, lacking essential information regarding charge-carrier dynamics as a function of microstructure, which is highly demanded for a better understanding and potential guidance for further improvements. In this work, for the first time, the charge-carrier dynamics of a representative double-cable polymer, which achieves efficiencies of over 6% as an active layer in SCOSCs, is investigated across seven orders of magnitude in time scale, from fs-ps charge generation to ns-mu s charge recombination processes. Specific emphasis is placed on understanding the impact of thermal post-treatment on the charge dissociation and recombination dynamics. Annealing the photoactive layer at 230 degrees C results in the highest photovoltaic performance because of efficient charge generation in parallel to suppressed recombination. This work intends to present a complete picture of the charge-carrier dynamics in SCOSCs using the representative double-cable polymer PBDBPBI-Cl.