Steve notes that Schreiner and co claim a “structure with a rather strong CS double bond or a weak triple bond”. With this size of molecule, the proverbial kitchen sink can be thrown at the analysis of the bonding. But one technique that was NOT applied is ELF (see the earlier post using ELF to analyze the bonding in MgPh2). So here is such an analysis, computed for the CCSD/cc-pVTZ wavefunction at the geometry reported in the publication (see also DOI: 10042/to-2980). The (centroids of the) synaptic basins are the small purple spheres.The key (disynaptic) basin is labelled 10, and it integrates to 2.36 electrons, rather far from the 6 electrons which might be expected for a triple bond! Its centroid is also significantly off-centre from the S-C bond. Basin 11 integrates to 2.01 electrons; it resembles a lone pair on the carbon, although the ELF analysis actually labels it a S-C disynaptic basin. It approximately maps to the HOMO orbital. Monosynaptic basin 9 encompases the two formal lone pairs on the sulfur, and it integrates to 3.59e (quite often, what we regard as separate, rabbit-ear, lone pairs on an atom manifest only as a single monosynaptic basin). Completing the analysis are two further monosynaptic basins 6 and 7, which represent lone pairs on the oxygen (2.45e each) and the disynaptic basin 8 (1.1e).
Bonding, much like the Humpty-Dumpty meaning, is very much what you want it to be! But in this case, one has to ask whether the description of the bonding in the C≡S region really is best described as a weak triple bond, or even a strong double bond, or whether the nominal six electrons of the triple bond split into two regions, one clearly bonding, the other more non-bonding.