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The rovibrational spectrum of the molecular ion HCCCH was investigated in a 4~K cryogenic ion trap instrument employing the leak-out spectroscopy method. Transitions within the fundamental (C-H stretch) and the combination band + (C-C stretches) were detected, the search aided by high level quantum chemical calculations. The analysis of the rovibrational measurements enabled us to predict the rotational structure of the ground state. Using a rotational-vibrational double-resonance scheme, 14 pure rotational transitions were measured. This, in turn, led to the radio astronomical detection of HCCCH in the interstellar medium, as recently reported (Silva et al., Astron. Astrophys. 676, L1, 2023).

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