We report the origin of the strong UV-irradiation dependence, generally known as a “light-soaking” process, in inverted polymer solar cells (I-PSCs) using the interface of an sol-gel processed titanium sub-oxide (TiOx) and indium tin oxide (ITO) cathode. When I-PSCs incorporating TiOx as an electron-selecting layer were fabricated, the as-prepared devices exhibited an anomalous J-V curve with a kink shape, resulting in an extremely low efficiency. However, the kink shape disappeared after white light irradiation for considerable duration, after which the device parameters recovered the normal values expected for this class of devices. By using electrochemical impedance spectroscopy and by measuring the contact potential difference and transient photoconductivity of the TiOx layer, we found that the light-soaking process in I-PSCs originates from the photoinduced “rearrangement of the Fermi levels” at the sol-gel processed TiOx and ITO cathode interface together with trap sites existing in the TiOx layer. Based on our data, we optimized I-PSC devices with a high fill factor (FF) of ∼70%.
Additional post-processing techniques, such as post-thermal annealing and UV illumination, were found to be required to obtain desirable values of the cell parameters in a tandem polymer solar cell incorporated with solution-processed basic n-type titanium sub-oxide (TiO(x))/acidic p-type poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) interlayers. Subsequent to the fabrication of the tandem polymer solar cells, the open-circuit voltage (V(OC)) of the cells exhibited half of the expected value. Only after the application of the post-treatments, the V(OC) of a tandem cell increased from the initial half-cell value (∼0.6 V) to its full-cell value (∼1.2 V). The selective light-biased incident photon-to-current efficiency (IPCE) measurements indicated that the initial V(OC) originated from the back subcell and that the application of the post-processing treatments revived the front subcell, such that the net photocurrent of the tandem cell was finally governed by a recombination process of holes from the back subcell and electrons from the front subcell. Based on our experimental results, we suggest that a V(OC) enhancement could be ascribed to two types of subsequent junction formations at the interface between the TiO(x) and PEDOT:PSS interlayers: an 'ion-mediated dipole junction', resulting from the electro-kinetic migration of cationic ions in the interlayers during post-thermal annealing in the presence of a low-work-function metal cathode, and a 'photoinduced Schottky junction', formed by increasing the charge carrier density in the n-type TiO(x) interlayer during UV illumination process. The two junctions separately contributed to the formation of a recombination junction through which the electrons in TiO(x) and the holes in PEDOT:PSS were able to recombine without substantial voltage drops.
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