Yilmaz, MehmetBabur, EsraOzdemir, MehmetGieseking, Rebecca L.Dede, YavuzTamer, UgurSchatz, George C.2025-03-232025-03-2320171476-11221476-4660https://doi.org/10.1038/NMAT4957https://hdl.handle.net/11486/5933pi-Conjugated organic semiconductors have been explored in several optoelectronic devices, yet their use in molecular detection as surface-enhanced Raman spectroscopy (SERS)-active platforms is unknown. Herein, we demonstrate that SERS-active, superhydrophobic and ivy-like nanostructured films of a molecular semiconductor, alpha,omega-diperfluorohexylquaterthiophene (DFH-4T), can be easily fabricated by vapour deposition. DFH-4T films without any additional plasmonic layer exhibit unprecedented Raman signal enhancements up to 3.4 x 10(3) for the probe molecule methylene blue. The combination of quantum mechanical computations, comparative experiments with a fluorocarbon-free alpha,omega-dihexylquaterthiophene (DH-4T), and thin-film microstructural analysis demonstrates the fundamental roles of the pi-conjugated core fluorocarbon substitution and the unique DFH-4T film morphology governing the SERS response. Furthermore, Raman signal enhancements up to similar to 10(10) and sub-zeptomole (< 10(-21) mole) analyte detection were accomplished by coating the DFH-4T films with a thin gold layer. Our results offer important guidance for the molecular design of SERS-active organic semiconductors and easily fabricable SERS platforms for ultrasensitive trace analysis.eninfo:eu-repo/semantics/closedAccessLight-Emitting TransistorsGold Nanorod ArraysPolymeric ElectronicsBuilding-BlocksScatteringSersDesignPolarizabilityNanoparticlesNanocrystalsArticle169918+10.1038/NMAT4957287831572-s2.0-85028464875Q1WOS:000408591300014Q1