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Raman studies of ion-irradiated MoS\n                    <jats:sub>2<\/jats:sub>\n                    are often complicated by high ion energies, incomplete defect quantification, and uncontrolled adsorbates at defect sites. Here, we irradiate large-area monolayer MoS\n                    <jats:sub>2<\/jats:sub>\n                    with low-energy (600\u2009eV) Ar\n                    <jats:sup>+<\/jats:sup>\n                    ions in a ultrahigh vacuum chamber and perform\n                    <jats:italic>in situ<\/jats:italic>\n                    Raman spectroscopy over a range of fluences. Atomic-resolution scanning transmission electron microscopy reveals predominantly randomly distributed sulfur vacancies as the dominant defect type. With increasing fluence, Raman spectra show a downshift and broadening of the E\n                    <jats:inline-formula>\n                      <jats:tex-math>\n                        \n                      <\/jats:tex-math>\n                      <mml:math xmlns:mml=\"http:\/\/www.w3.org\/1998\/Math\/MathML\" overflow=\"scroll\">\n                        <mml:mrow>\n                          <mml:msubsup>\n                            <mml:mi\/>\n                            <mml:mrow>\n                              <mml:mn>2<\/mml:mn>\n                              <mml:mtext>g<\/mml:mtext>\n                            <\/mml:mrow>\n                            <mml:mn>1<\/mml:mn>\n                          <\/mml:msubsup>\n                        <\/mml:mrow>\n                      <\/mml:math>\n                    <\/jats:inline-formula>\n                    mode, a slight upshift and broadening of the A\n                    <jats:inline-formula>\n                      <jats:tex-math>\n                        \n                      <\/jats:tex-math>\n                      <mml:math xmlns:mml=\"http:\/\/www.w3.org\/1998\/Math\/MathML\" overflow=\"scroll\">\n                        <mml:mrow>\n                          <mml:msub>\n                            <mml:mi\/>\n                            <mml:mrow>\n                              <mml:mn>1<\/mml:mn>\n                              <mml:mtext>g<\/mml:mtext>\n                            <\/mml:mrow>\n                          <\/mml:msub>\n                        <\/mml:mrow>\n                      <\/mml:math>\n                    <\/jats:inline-formula>\n                    mode, and the emergence of defect-activated features, including a prominent LA(\n                    <jats:italic>M<\/jats:italic>\n                    ) mode. A controlled ambient exposure followed by remeasurement separates intrinsic defect signatures from extrinsic doping: an additional A\n                    <jats:inline-formula>\n                      <jats:tex-math>\n                        \n                      <\/jats:tex-math>\n                      <mml:math xmlns:mml=\"http:\/\/www.w3.org\/1998\/Math\/MathML\" overflow=\"scroll\">\n                        <mml:mrow>\n                          <mml:msub>\n                            <mml:mi\/>\n                            <mml:mrow>\n                              <mml:mn>1<\/mml:mn>\n                              <mml:mtext>g<\/mml:mtext>\n                            <\/mml:mrow>\n                          <\/mml:msub>\n                        <\/mml:mrow>\n                      <\/mml:math>\n                    <\/jats:inline-formula>\n                    upshift and linewidth narrowing indicate a modest, largely reversible p-doping contribution from weak physisorption at vacancy sites, corresponding to an apparent charge transfer of \u223c0.02\n                    <jats:italic>e<\/jats:italic>\n                    per STEM-counted vacancy. Within the sensitivity of our\n                    <jats:italic>in situ<\/jats:italic>\n                    Raman measurements, oxidation-related signatures remain negligible, and adsorbate effects largely vanish upon returning to vacuum and under laser illumination. These results establish Raman fingerprints of sulfur-vacancy ensembles in monolayer MoS\n                    <jats:sub>2<\/jats:sub>\n                    and provide quantitative guidance for defect engineering and metrology under controlled vacuum conditions.\n                  <\/jats:p>","DOI":"10.1088\/2053-1583\/ae6b2b","type":"journal-article","created":{"date-parts":[[2026,5,10]],"date-time":"2026-05-10T16:47:50Z","timestamp":1778431670000},"page":"025033","update-policy":"https:\/\/doi.org\/10.1088\/crossmark-policy","source":"Crossref","is-referenced-by-count":2,"title":["<i>In situ<\/i>\n                    Raman study on sulfur vacancies in monolayer MoS\n                    <sub>2<\/sub>"],"prefix":"10.1088","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-6382-3679","authenticated-orcid":true,"given":"Leon","family":"Daniel","sequence":"first","affiliation":[{"name":"University of Duisburg-Essen"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7943-2089","authenticated-orcid":true,"given":"Yossarian","family":"Liebsch","sequence":"additional","affiliation":[{"name":"University of Duisburg-Essen"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-9738-9706","authenticated-orcid":true,"given":"Charleen","family":"Lintz","sequence":"additional","affiliation":[{"name":"University of Duisburg-Essen"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-3600-6071","authenticated-orcid":true,"given":"Umair","family":"Javed","sequence":"additional","affiliation":[{"name":"University of Vienna"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8737-6227","authenticated-orcid":true,"given":"Osamah","family":"Kharsah","sequence":"additional","affiliation":[{"name":"University of Duisburg-Essen"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7797-9662","authenticated-orcid":true,"given":"Lars","family":"Breuer","sequence":"additional","affiliation":[{"name":"University of Duisburg-Essen"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1301-5266","authenticated-orcid":true,"given":"Jani","family":"Kotakoski","sequence":"additional","affiliation":[{"name":"University of Vienna"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5785-1186","authenticated-orcid":true,"given":"Marika","family":"Schleberger","sequence":"additional","affiliation":[{"name":"University of Duisburg-Essen"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"266","published-online":{"date-parts":[[2026,5,26]]},"reference":[{"key":"tdmae6b2bbib1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.105.136805","type":"journal-article","volume":"105","author":"Mak","year":"2010","journal-title":"Phys. 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