Wolansky, JakobJakobWolanskyHoffmann, CedricCedricHoffmannPanhans, MichelMichelPanhansWinkler, Louis ConradLouis ConradWinklerTalnack, FelixFelixTalnackHutsch, SebastianSebastianHutschZhang, HuotianHuotianZhangKirch, AntonAntonKirchYallum, Kaila M.Kaila M.YallumFriedrich, HannesHannesFriedrichKublitski, JonasJonasKublitskiGao, FengFengGaoSpoltore, DonatoDonatoSpoltoreMannsfeld, Stefan C BStefan C BMannsfeld0000-0003-0268-519XOrtmann, FrankFrankOrtmannBanerji, NatalieNatalieBanerji0000-0001-9181-2642Leo, KarlKarlLeoBenduhn, JohannesJohannesBenduhn2024-12-182024-12-182024-11-06https://boris-portal.unibe.ch/handle/20.500.12422/189688Typically, organic solar cells (OSCs) and photodetectors (OPDs) comprise an electron donating and accepting material to facilitate efficient charge carrier generation. This approach has proven successful in achieving high-performance devices but has several drawbacks for upscaling and stability. This study presents a fully vacuum-deposited single-component OPD, employing the neat oligothiophene derivative DCV2-5T in the photoactive layer. Free charge carriers are generated with an internal quantum efficiency of 20 % at zero bias. By optimizing the device structure, a very low dark current of 3.4 · 10-11 A cm-2 at -0.1 V is achieved, comparable to the dark current of state-of-the-art bulk heterojunction OPDs. This optimization results in specific detectivities of 1· 1013 Jones (based on noise measurements), accompanied by a fast photoresponse (f-3dB = 200 kHz) and a broad linear dynamic range (> 150 dB). Ultrafast transient absorption spectroscopy unveils that charge carriers are already formed at very short time scales (< 1 ps). The surprisingly efficient bulk charge generation mechanism is attributed to a strong electronic coupling of the molecular exciton and charge transfer states. This work demonstrates the very high performance of single-component OPDs and proves that this novel device design is a successful strategy for highly efficient, morphological stable and easily manufacturable devices.enorganic photodetectorssingle‐componentsmall moleculeultrafast spectroscopy500 - Science::540 - Chemistryarticle10.48620/785823950200710.1002/adma.202402834