Over the past two decades, the identification and characterisation of interstellar molecules has often benefitted from a fruitful interplay between theoretical chemistry, laboratory spectroscopy and (radio) astronomy. The article reports on various examples of this sort, concentrating on carbon chains which represent the most prominent structural motif among currently known interstellar molecules. Results of large-scale coupled cluster calculations are reported for cyanopolyynes (HC2n+1N) up to n = 5, the corresponding radicals C2n+1N, linear silicon carbides (SiCn), carbon–sulfur and pure carbon chains. Throughout, detailed comparison with experimental data is made wherever possible.
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