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Non-fullerene acceptors based on perylenediimides (PDIs) have garneredsignificant interest as an alternative to fullerene acceptors in organicphotovoltaics (OPVs), but their charge transport phenomena are not wellunderstood, especially in bulk heterojunctions (BHJs). Here, we investigatecharge transport and current fluctuations by performing correlatedlow-frequency noise and impedance spectroscopy measurements on two BHJ OPVsystems, one employing a fullerene acceptor and the other employing a dimericPDI acceptor. In the dark, these measurements reveal that PDI-based OPVs have agreater degree of recombination in comparison to fullerene-based OPVs.Furthermore, for the first time in organic solar cells, 1/f noise data are fitto the Kleinpenning model to reveal underlying current fluctuations indifferent transport regimes. Under illumination, 1/f noise increases byapproximately four orders of magnitude for the fullerene-based OPVs and threeorders of magnitude for the PDI-based OPVs. An inverse correlation is alsoobserved between noise spectral density and power conversion efficiency.Overall, these results show that low-frequency noise spectroscopy is aneffective in-situ diagnostic tool to assess charge transport in emergingphotovoltaic materials, thereby providing quantitative guidance for the designof next-generation solar cell materials and technologies.

Correlated In-Situ Low-Frequency Noise and Impedance Spectroscopy Reveal  Recombination Dynamics in Organic Solar Cells using Fullerene and  Non-Fullerene Acceptors