While multi‐junction geometries have the potential to boost the efficiency of organic solar cells, the experimental gains yet obtained are still very modest. This work proposes an alternative spectral splitting device concept in which various individual semiconducting junctions with cascading bandgaps are laid side by side, thus the name RAINBOW. Each lateral sub‐cell receives a fraction of the spectrum that closely matches the main absorption band of the given semiconductor. Here, simulations are used to identify the important material and device properties of each RAINBOW sub‐cell. Using the resulting design rules, three systems are selected, with narrow, medium, and wide effective bandgaps, and their potential as sub‐cells in this geometry is experimentally investigated. With the aid of a custom‐built setup that generates spectrally spread sunlight on demand, the simulations are experimentally validated, showing that this geometry can lead to a reduction in thermalization losses and an improvement in light harvesting, which results in a relative improvement in efficiency of 46.6% with respect to the best sub‐cell. Finally, a working proof‐of‐concept monolithic device consisting of two sub‐cells deposited from solution on the same substrate is fabricated, thus demonstrating the feasibility and the potential of the RAINBOW solar cell concept.

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The correct determination of the exciton diffusion length (LD) in novel organic photovoltaics (OPV) materials is an important, albeit challenging, task required to understand these systems. Herein, a high‐throughput approach to probe LD in nonfullerene acceptors (NFAs) is reported, that builds upon the conventional photoluminescence (PL) surface quenching method using NFA layers with a graded thickness variation in combination with spectroscopic PL mapping. The method is explored for two archetypal NFAs, namely, ITIC and IT‐4F, using PEDOT:PSS and the donor polymer PM6 as two distinct and practically relevant quencher materials. Interestingly, conventional analysis of quenching efficiency as a function of acceptor layer thickness results in a threefold difference in LD values depending on the specific quencher. This discrepancy can be reconciled by accounting for the differences in light in‐ and outcoupling efficiency for different multilayer architectures. In particular, it is shown that the analysis of glass/acceptor/PM6 structures results in a major overestimation of LD, whereas glass/acceptor/PEDOT:PSS structures give no significant contribution to outcoupling, yielding LD values of 6−12 and 8−18 nm for ITIC and IT‐4F, respectively. Hence, practical guidelines for quencher choice, sample geometries, and analysis approach for the accurate assessment of LD are provided.

We report a multi-purpose spectrum-on-demand light source (SOLS), conceived primarily but not exclusively, for the multiple and advanced characterization of photovoltaic (PV) materials and devices. The apparatus is a spectral shaper illumination device, providing a tunable and spectrally shaped light beam produced by modulating the intensity and/or wavelength range of a primary light source. SOLS stands out from the state of the art because it produces almost any spectrum on demand and delivers two types of output: a spectrally shaped and spatially homogeneous beam over its cross section for areal illumination; or a spatially and spectrally split beam into its wavelength components, a unique capability suited to characterize lateral-tandem (Rainbow) solar cells. The tuneability from broadband to narrow band illumination enables two characterization devices into one, namely, a solar simulator for the determination of the power conversion efficiency and an external quantum efficiency measuring system. We expect the SOLS setup to accelerate material screening, enabling the discovery and optimization of novel multi-component materials and devices, in particular for emergent PV technologies like organic, metal halide perovskites or multi-junction geometries as well as novel PV applications such as indoors, building integrated or agrivoltaics, among others.