Zhang, DanStojanovic, MarkoRen, YamengCao, YimingEickemeyer, Felix T.Socie, EtienneVlachopoulos, NickMoser, Jacques-E.Zakeeruddin, Shaik M.Hagfeldt, AndersGrätzel, Michael2021-03-232021-03-232021-03-232021-03-1910.1038/s41467-021-21945-3https://infoscience.epfl.ch/handle/20.500.14299/176075To develop photosensitizers with high open-circuit photovoltage (Voc) is a crucial strategy to enhance the power conversion efficiency (PCE) of co-sensitized solar cells. Here, we show a judiciously tailored organic photosensitizer, coded MS5, featuring the bulky donorN-(2’,4’-bis(dodecyloxy)-[1,1’-biphenyl]-4-yl)-2’,4’-bis(dodecyloxy)-N-phenyl-[1,1’-biphenyl]-4-amineand the electron acceptor 4-(benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid. Employing MS5 with a copper (II/I) electrolyte enables a dye-sensitized solar cell (DSC) to achieve a strikingly high Voc of 1.24 V, with the Voc deficit as low as 130 mV and an ideality factor of merely 1.08. The co-sensitization of MS5 with the wider spectral-response dye XY1b produces a highly efficient and stable DSC with the PCE of 13.5% under standard AM1.5 G, 100 mW cm−2 solar radiation. Remarkably, the co-sensitized solar cell (active area of 2.8 cm2) presents a record PCE of 34.5% under ambient light, rendering it very attractive as an ambient light harvesting energy source for low power electronics.Dye-sensitized solar cellsCopper (II/I)-based electrolyteOrganic dyesCo-sensitizationAmbient light energy harvestingHigh efficiency photovoltaicsA molecular photosensitizer achieves a Voc of 1.24 V enabling highly efficient and stable dye-sensitized solar cells with copper(II/I)-based electrolytetext::journal::journal article::research article