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Recently, the novel system of linear carbon chains inside of double-walledcarbon nanotubes has extended the length of $sp^1$ hybridized carbon chainsfrom 44 to thousands of atoms [L. Shi et al., Nat. Mater. 15, 634 (2016)]. Theoptoelectronic properties of these ultra-long chains are poorly described bycurrent theoretical models, which are based on short chain experimental dataand assume a constant environment. As such, a physical understanding of thesystem in terms of charge transfer and van der Waals interactions is widelymissing. We provide a reference for the intrinsic Raman frequency of polyynesin vacuo and explicitly describe the interactions between polyynes and carbonnanotubes. We find that van der Waals interactions strongly shift the Ramanfrequency, which has been neither expected nor addressed before. As aconsequence of charge transfer from the tube to the chain, the Raman responseof long chains is qualitatively different from the known phonon dispersion ofpolymers close to the $\Gamma$-point. Based on these findings we show how tocorrectly interpret the Raman data, considering the nanotube's properties. Thisis essential for its use as an analytical tool to optimize the growth processfor future applications.

Polyyne Electronic and Vibrational Properties under Environmental Interactions