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While alloying and intercalation have been shown to modulate ground states, the role of d\u2010shell filling in governing these transitions remains insufficiently understood. Here, we investigate electron doping effects in MPS\n                    <jats:sub>3<\/jats:sub>\n                    using angle\u2010resolved photoemission spectroscopy (ARPES), X\u2010ray photoelectron spectroscopy (XPS), and density functional theory (DFT+U). Lithium and cesium deposition are employed to induce doping across different MPS\n                    <jats:sub>3<\/jats:sub>\n                    compounds. We identify two distinct doping mechanisms: in MnPS\n                    <jats:sub>3<\/jats:sub>\n                    , electrons are primarily donated to the P\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>6<\/jats:sub>\n                    ligand clusters, with negligible Mn 2p core\u2010level shifts and no major changes in the valence band. In contrast, FePS\n                    <jats:sub>3<\/jats:sub>\n                    , CoPS\n                    <jats:sub>3<\/jats:sub>\n                    , and NiPS\n                    <jats:sub>3<\/jats:sub>\n                    exhibit clear reductions in transition\u2010metal oxidation states, with a \u223c1.0\u00a0eV reduction in spin\u2010orbit splitting for Co upon doping. ARPES on CoPS\n                    <jats:sub>3<\/jats:sub>\n                    reveals a \u223c400 meV shift of Co\u2010derived bands toward higher binding energies and new dispersive states up to 1\u00a0eV above the valence band maximum, indicating metallic behavior. These results establish a direct correlation between d\u2010shell filling and doping response, highlighting alkali metal doping as a tunable route to tailor the electronic and magnetic properties of 2D AFM semiconductors for spintronic applications.\n                  <\/jats:p>","DOI":"10.1002\/advs.202510675","type":"journal-article","created":{"date-parts":[[2026,3,24]],"date-time":"2026-03-24T12:43:01Z","timestamp":1774356181000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Electronic Structure Reorganization in MPS\n                    <sub>3<\/sub>\n                    via d\u2010Shell\u2010Selective Alkali Metal Doping"],"prefix":"10.1002","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-7171-608X","authenticated-orcid":false,"given":"Jonah Elias","family":"Nitschke","sequence":"first","affiliation":[{"name":"TU Dortmund University  Dortmund 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