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The spectrum is recorded up to a binding energy of 23\u00a0eV, and the vibrationally resolved bands of the cationic ground state (X\u0303+2\u03a0) and the lowest excited cationic states (A\u0303+2A\u2033, B\u0303+2A\u2032, and 32A\u2033) are reported. The spectrum exhibits a complex and rich vibronic structure, which was analyzed using advanced first-principles methodologies. The equilibrium geometries and the potential energy surfaces of the neutral and cationic ground state as well as of the lowest cationic excited states were computed using post-Hartree\u2013Fock configuration interaction methods. For the photoionization populating the linear X\u0303+2\u03a0 state of HNCS+, an adiabatic ionization energy of 9.918 \u00b1 0.008\u00a0eV is determined, which agrees well with our calculated value of 9.921\u00a0eV. For an accurate calculation of ionization energies of sulfur-containing molecules, previous explicitly correlated computational schemes were revised as tight d functions need to be included. The lowest photoelectron band is subject to Renner\u2013Teller splitting and spin\u2013orbit splitting and was analyzed using a perturbative approach. The bands corresponding to transitions populating the A\u0303+2A\u2033 and B\u0303+2A\u2032 cationic states show vibrationally resolved progressions that were also assigned, leading to adiabatic ionization energies of 13.361 \u00b1 0.012 and 13.555 \u00b1 0.012\u00a0eV. This work highlights the complex vibronic structure of the HNCS cation, and the data may help identify HNCS+ in astrophysical media.<\/jats:p>","DOI":"10.1063\/5.0261472","type":"journal-article","created":{"date-parts":[[2025,4,24]],"date-time":"2025-04-24T14:11:39Z","timestamp":1745503899000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":4,"title":["Photoelectron spectrum of isothiocyanic acid, HNCS: Theory and experiment"],"prefix":"10.1063","volume":"162","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-6572-9214","authenticated-orcid":false,"given":"Dorothee","family":"Schaffner","sequence":"first","affiliation":[{"name":"Institute of Physical and Theoretical Chemistry, University of W\u00fcrzburg 1 , D-97074 W\u00fcrzburg,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Ayad","family":"Bellili","sequence":"additional","affiliation":[{"name":"U. 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