Publication date: 21st July 2025
Polyynes, chains consisting of alternating triple and single carbon-carbon bonds, are a model system for investigating low-dimensional allotropes of carbon.1 While such allotropes, e.g., 1D carbynes, are yet to be synthesized, they have been suggested to have a range of outstanding thermal, electrical and mechanical properties, and hence are of intense interest.2 Recently, relatively long (up to 48 alkyne units) linear and cyclic polyynes have been synthesized.3,4 These molecules allow for the investigation of 1D carbon, close to its infinite limit and explore fundamental links between topology and electronic structure in molecular systems.
Here, using a combination of temperature, polarization and time resolved optical spectroscopy we explore the electronic structure/dynamics of a linear and cyclic, C-[48] polyyne. We find on moving from a linear to ring geometry there are drastic changes in polyyene electronic properties, including reduced singlet-triplet intersystem crossing times, bond-length alternation strengths and dipole reorientation mechanisms. Comparing our results with literature calculations, allows to validate theoretical predications of polyynes, and comment, from an experimental viewpoint, on potential electronic properties/structures of a hypothetical carbyne.
S.B. acknowledges receipt of a Royal Society Newton International Fellowship.
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