This dataset contains the underlying experimental (1H NMR, 13C NMR, 31P NMR, high-resolution mass spectrometry (HRMS), UV-vis absorption, photoluminescence (PL), cyclic voltammetry) and computational (molecular geometries, input/output files for Q-Chem, Gaussian, and TheoDORE) research data for the article “[2.2.2.2]Paracyclophanetetraenes (PCTs): cyclic structural analogues of poly(p-phenylene vinylene)s (PPVs)”. Content (names of folders and files are given in bold face): The folder for each molecule (Br-P2, O-3, O-P1, O-PCT, PCT, S-2, S-3, S-P1, S-P2, S-PCT) contains the molecular structure as .mol and .cdxml file, as well as subfolders for the Experimental research data and, if available, the Computational research data. The Experimental research data folder for each molecule contains the measurement files. The file names are composed of the acronym of the measured molecule, the type of measurement, and further details about the measurement (if needed to distinguish the files). Measurements were performed as described in the article. Computations were performed on the molecules O-PCT and S-PCT as described in the text. The Computational research data folder for each molecule contains subfolders for geometry optimisations of the individual electronic states and rotamers: c2_neut: neutral singlet state for C2 rotamer c2_trip: T1 state of C2 rotamer c2_2P: charged state (2+) of C2 rotamer c2_2M: charged state (2-) of C2 rotamer cs_neut: neutral singlet state for Cs rotamer etc. Additional content: TS: Full transition state optimisation TS_constrained: constrained transition state optimisation VIST: Data for VIST plots Each optimisation folder contains the following: qchem.[in,out]: input/output for geometry optimisation final.xyz: optimised geometry SOLV/qchem.[in,out]: input/output for solvated single-point computation tNICS/gaussian.[com,log]: input/output for NMR shielding tensors

Additional funding has been provided by the Austrian Science Fund (project number J 4463, Conjugated macrocycles for battery electrodes).