Due to their tailorable optical properties, organic semiconductors show considerable promise for use in indoor photovoltaics (IPVs), which present a sustainable route for powering ubiquitous “Internet‐of‐Things” devices in the coming decades. However, owing to their excitonic and energetically disordered nature, organic semiconductors generally display considerable sub‐gap absorption and relatively large non‐radiative losses in solar cells. To optimize organic semiconductor‐based photovoltaics, it is therefore vital to understand how energetic disorder and non‐radiative recombination limit the performance of these devices under indoor light sources. In this work, we explore how energetic disorder, sub‐optical gap absorption, and non‐radiative open‐circuit voltage losses detrimentally affect the upper performance limits of organic semiconductor‐based IPVs. Based on these considerations, we provide realistic upper estimates for the power conversion efficiency. Energetic disorder, inherently present in molecular semiconductors, is generally found to shift the optimal optical gap from 1.83 to ≈1.9 eV for devices operating under light emitting diode spectra. Finally, we also describe a methodology (accompanied by a computational tool with a graphical user interface) for predicting IPV performance under arbitrary illumination conditions. Using this methodology, we estimate the indoor power conversion efficiencies of several photovoltaic materials, including the state‐of‐the‐art systems PM6:Y6 and PM6:BTP‐eC9.
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