Controlling the nature and transfer of excited states in organic photovoltaic (OPV) devices is of critical concern due to the fact that exciton transport and separation can dictate the final performance of the system. One effective method to accomplish improved charge separation in organic electronic materials is to control the spin state of the photogenerated charge-carrying species. To this end, nanoparticles with unique iron oxide (Fe3O4) cores and zinc oxide (ZnO) shells were synthesized in a controlled manner. Then, the structural and magnetic properties of these core-shell nanoparticles (Fe3O4@ZnO) were tuned to ensure superior performance when they were incorporated into the active layers of OPV devices. Specifically, small loadings of the core-shell nanoparticles were blended with the previously well-characterized OPV active layer of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM). Upon addition of the core-shell nanoparticles, the performance of the OPV devices was increased up to 25% relative to P3HT-PCBM active layer devices that contained no nanoparticles; this increase was a direct result of an increase in the short-circuit current densities of the devices. Furthermore, it was demonstrated that the increase in photocurrent was not due to enhanced absorption of the active layer due to the presence of the Fe3O4@ZnO core-shell nanoparticles. In fact, this increase in device performance occurred because of the presence of the superparamagnetic Fe3O4 in the core of the nanoparticles as incorporation of ZnO only nanoparticles did not alter the device performance. Importantly, however, the ZnO shell of the nanoparticles mitigated the negative optical effect of Fe3O4, which have been observed previously. This allowed the core-shell nanoparticles to outperform bare Fe3O4 nanoparticles when the single-layer nanoparticles were incorporated into the active layer of OPV devices. As such, the new materials described here present a tangible pathway toward the development of enhanced design schemes for inorganic nanoparticles such that magnetic and energy control pathways can be tailored for flexible electronic applications.
Keywords: controlled nanoparticle synthesis; core−shell nanoparticles; inverted organic solar cells; nanostructural characterization; photocurrent enhancement; superparamagnetic cores.