Carbyne is an infinitely long linear chain of carbon atoms with sp
1 hybridization and the truly one-dimensional allotrope of carbon. While obtaining freestanding carbyne is still an open challenge, the study of confined carbyne, linear chains of carbon encapsulated in carbon nanotubes, provides a pathway to explore carbyne and its remarkable properties in a well-defined environment. In this review, we discuss the basics and recent advances in studying single confined carbyne chains by Raman spectroscopy, which is their primary spectroscopic characterization method. We highlight where single carbyne chain studies are needed to advance our understanding of confined carbyne as a material system and provide an overview of the open questions that need to be addressed and of those aspects currently under debate.
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