Photo-Carrier Multi-Dynamical Imaging at the Nanometer Scale in Organic and Inorganic Solar Cells

Investigating the photocarrier dynamics in nanostructured and heterogeneous energy materials is of crucial importance from both fundamental and technological points of view. Here, we demonstrate how noncontact atomic force microscopy combined with Kelvin probe force microscopy under frequency-modulated illumination can be used to simultaneously image the surface photopotential dynamics at different time scales with a sub-10 nm lateral resolution. The basic principle of the method consists in the acquisition of spectroscopic curves of the surface potential as a function of the illumination frequency modulation on a two-dimensional grid. We show how this frequency-spectroscopy can be used to probe simultaneously the charging rate and several decay processes involving short-lived and long-lived carriers. With this approach, dynamical images of the trap-filling, trap-delayed recombination and nongeminate recombination processes have been acquired in nanophase segregated organic donor-acceptor bulk heterojunction thin films. Furthermore, the spatial variation of the minority carrier lifetime has been imaged in polycrystalline silicon thin films. These results establish two-dimensional multidynamical photovoltage imaging as a universal tool for local investigations of the photocarrier dynamics in photoactive materials and devices.