Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.052
Publication date: 22nd December 2022
Despite an impressive increase over the last decade, experimentally determined power conversion efficiencies of organic photovoltaic (OPV) cells still fall considerably below the theoretical upper bound for near-equilibrium solar cells, set by the Shockley-Queisser limit. Even in otherwise optimized devices, a prominent yet incompletely understood loss channel is the thermalization of photogenerated charge carriers in the density of states that is broadened by energetic disorder. First, we will show by a detailed comparison between numerical modeling and experiments that the slowness of the mentioned thermalization leads to a 0.1-0.2 eV higher open circuit voltage (Voc) in OPV devices than would be expected for instantaneous thermalization.[1] The latter is commonly assumed when analyzing Voc of OPV devices. Second, we demonstrate by extensive numerical modelling how this loss channel can be mitigated in carefully designed morphologies. Specifically, we show how funnel-shaped donor- and acceptor-rich domains in the phase-separated morphology that is characteristic of organic bulk heterojunction solar cells can promote directed transport of positive and negative charge carriers towards the anode and cathode, respectively.[2] We demonstrate that in optimized funnel morphologies this kinetic, non-equilibrium effect, which is boosted by the said slow thermalization of photogenerated charges, allows to surpass the Shockley-Queisser limit for the same material in absence of gradients and under near-equilibrium conditions. Methodologies by which the proposed morphologies can be realized are discussed, along with the relevance to already published results.
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