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The closed-shell nature of the reference state in an X2C-IP-EOMCC calculation allows for accurate predictions of spin\u2013orbit splittings in open-shell molecules without breaking degeneracies, as would occur in an excitation-energy EOMCC calculation carried out directly on an unrestricted open-shell reference. We apply X2C-IP-EOMCC to the ground and first excited states of the HCCX+ (X = Cl, Br, I) cations, where it is demonstrated that a large basis set (i.e., quadruple-zeta quality) and 3h2p correlation effects are necessary for accurate absolute energetics. The maximum error in calculated adiabatic IPs is on the order of 0.1\u00a0eV, whereas spin\u2013orbit splittings themselves are accurate to \u22480.01 eV, as compared to experimentally obtained values.<\/jats:p>","DOI":"10.1063\/5.0248535","type":"journal-article","created":{"date-parts":[[2025,2,26]],"date-time":"2025-02-26T08:37:12Z","timestamp":1740559032000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":14,"title":["Two-component relativistic equation-of-motion coupled cluster for electron ionization"],"prefix":"10.1063","volume":"162","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6604-3543","authenticated-orcid":false,"given":"Stephen H.","family":"Yuwono","sequence":"first","affiliation":[{"name":"Department of Chemistry and Biochemistry, Florida State University 1 , Tallahassee, Florida 32306-4390,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3349-3169","authenticated-orcid":false,"given":"Run R.","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry, Florida State University 1 , Tallahassee, Florida 32306-4390,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9655-7927","authenticated-orcid":false,"given":"Tianyuan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Department of Chemistry, University of Washington 2 , Seattle, Washington 98195,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7341-6240","authenticated-orcid":false,"given":"Xiaosong","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemistry, University of Washington 2 , Seattle, Washington 98195,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1061-2521","authenticated-orcid":false,"suffix":"III","given":"A. 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