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Suppressing charge recombination is key for organic solar cells to become commercial reality. However, there is still no conclusive picture of how recombination losses are influenced by the complex nanoscale morphology. Here, new insight is provided by revisiting the P3HT:PCBM blend, which is still one of the best performers regarding reduced recombination. By changing small details in the annealing procedure, two model morphologies were prepared that vary in phase separation, molecular order and phase purity, as revealed by electron tomography and optical spectroscopy. Both systems behave very similarly with respect to charge generation and transport, but differ significantly in bimolecular recombination. Only the system containing P3HT aggregates of high crystalline quality and purity is found to achieve exceptionally low recombination rates. The high-quality aggregates support charge delocalization, which assists the re-dissociation of interfacial charge-transfer states formed upon the encounter of free carriers. For devices with the optimized morphology, an exceptional long hole diffusion length is found, which allows them to work as Shockley-type solar cells even in thick junctions of 300 nm. In contrast, the encounter rate and the size of the phase-separated domains appears to be less important., Comment: final version, journal reference and DOI added

Solar cells with a heterojunction between colloidal CuInS$_2$ and ZnO nanocrystals are an innovative concept in solution-processed photovoltaics, but the conversion efficiency cannot compete yet with devices employing lead chalcogenide quantum dots. Here, we present a detailed study on the charge collection in CuInS$_2$/ZnO solar cells. An inverted device architecture was utilized, in which the ZnO played an additional role as optical spacer layer. Variations of the ZnO thickness were exploited to create different charge generation profiles within the light-harvesting CuInS$_2$ layer, which strongly affected both the external and internal quantum efficiency. By the reconstruction of these experimental findings with the help of a purely optical model, we were able to draw conclusions on the spatial dependency of the charge collection probability. We provide evidence that only carriers generated within a narrow zone of circa 40 nm near the CuInS$_2$/ZnO interface contribute to the external photocurrent. The remaining part of the absorber can be considered as "dead zone" for charge collection, which reasonably explains the limited device performance and indicates a direction for future research. From the methodical point of view, the optical modeling approach developed in the present work has the advantage that no electrical input parameters are required and is believed to be easily transferable to other material systems., Comment: 13 pages, 9 figures; Supplemental Material: 13 pages, 8 figures

With the usage of two transparent electrodes, organic solar cells are semitransparent and may be combined to parallel-connected multi-junction devices or used for innovative applications like power-generating windows. A challenging issue is the optimization of the electrodes, in order to combine high transparency with adequate electric properties. In the present work, we study the potential of sputter-deposited aluminum-doped zinc oxide (AZO) as an alternative to the widely used but relatively expensive indium tin oxide (ITO) as cathode material in semitransparent polymer-fullerene solar cells. Concerning the anode, we utilized an insulator/metal/insulator structure based on ultra-thin Au films embedded between two evaporated MoO$_3$ layers, with the outer MoO$_3$ film (capping layer) serving as a light coupling layer. The performance of the ITO-free semitransparent solar cells is systematically studied as dependent on the thickness of the capping layer and the active layer, as well as the illumination direction. These variations are found to have strong impact on the obtained photocurrent. We performed optical simulations of the electric field distribution within the devices to analyze the origin of the current variations and provide deep insight in the device physics. With the conventional absorber materials studied herein, optimized ITO-free and semitransparent devices reached 2.0% power conversion efficiency and a maximum optical transmission of 60%, with the device concept being potentially transferable to other absorber materials., Comment: 15 pages, 10 figures; Supplemental Material: 13 pages, 7 figures

Colloidal zinc oxide (ZnO) nanoparticles are frequently used in the field of organic photovoltaics for the realization of solution-producible, electron-selective interfacial layers. Despite of the widespread use, there is a lack of detailed investigations regarding the impact of structural properties of the particles on the device performance. In this work, ZnO nanoparticles with varying surface-area-to-volume ratio were synthesized and implemented into polymer-fullerene bulk heterojunction solar cells with a gas-permeable top electrode. By comparing the electrical characteristics before and after encapsulation, it was found that the internal surface area of the ZnO layer plays a crucial role under conditions where oxygen can penetrate the solar cells. The adsorption of oxygen species at the nanoparticle surface causes band bending and electron depletion next to the surface. Both effects result in the formation of a barrier for electron injection and extraction at the ZnO/bulk heterojunction interface and were more pronounced in case of small ZnO nanocrystals (high surface-area-to-volume ratio). Different transport-related phenomena in the presence of oxygen are discussed in detail, i.e., Ohmic losses, expressed in terms of series resistance, as well as the occurrence of space-charge-limited currents, related to charge accumulation in the polymer-fullerene blend. Since absorption of UV light can cause desorption of adsorbed oxygen species, the electrical properties depend also on the illumination conditions. With the help of systematic investigations of the current versus voltage characteristics of solar cells under different air exposure and illumination conditions as well as studies of the photoconductivity of pure ZnO nanoparticle layers, we gain detailed insight into the role of the ZnO nanoparticle surface for the functionality of the organic solar cells., Comment: 12 pages, 9 figures; Supplemental Material: 10 pages, 7 figures

We present measurements of the near-field heat transfer between the tip of a thermal profiler and planar material surfaces under ultrahigh vacuum conditions. For tip-sample distances below 10-8 m our results differ markedly from the prediction of fluctuating electrodynamics. We argue that these differences are due to the existence of a material-dependent small length scale below which the macroscopic description of the dielectric properties fails, and discuss a corresponding model which yields fair agreement with the available data. These results are of importance for the quantitative interpretation of signals obtained by scanning thermal microscopes capable of detecting local temperature variations on surfaces.