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The recent discovery of helical van der Waals multiferroics down to the ultrathin limit raises prospects of large chiral magnetoelectric correlations in two dimensions\n                    <jats:sup>5,6<\/jats:sup>\n                    . However, the exact nature and magnitude of these couplings have remained unknown so far. Here we perform a precision measurement of the dynamical magnetoelectric coupling for an enantiopure domain in an exfoliated van der Waals multiferroic. We evaluate this interaction in resonance with a collective electromagnon mode, capturing the impact of its oscillations on the dipolar and magnetic orders of the material with a suite of ultrafast optical probes. Our data show a giant natural optical activity at terahertz frequencies, characterized by quadrature modulations between the electric polarization and magnetization components. First-principles calculations further show that these chiral couplings originate from the synergy between the non-collinear spin texture and relativistic spin\u2013orbit interactions, resulting in substantial enhancements over lattice-mediated effects. Our findings highlight the potential for intertwined orders to enable unique functionalities in the two-dimensional limit and pave the way for the development of van der Waals magnetoelectric devices operating at terahertz speeds.\n                  <\/jats:p>","DOI":"10.1038\/s41586-024-07678-5","type":"journal-article","created":{"date-parts":[[2024,7,17]],"date-time":"2024-07-17T12:02:19Z","timestamp":1721217739000},"page":"273-279","update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":69,"title":["Giant chiral magnetoelectric oscillations in a van der Waals multiferroic"],"prefix":"10.1038","volume":"632","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8982-4601","authenticated-orcid":false,"given":"Frank Y.","family":"Gao","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyue","family":"Peng","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinle","family":"Cheng","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3318-4454","authenticated-orcid":false,"given":"Emil","family":"Vi\u00f1as Bostr\u00f6m","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4551-7727","authenticated-orcid":false,"given":"Dong Seob","family":"Kim","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5069-5176","authenticated-orcid":false,"given":"Ravish K.","family":"Jain","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Deepak","family":"Vishnu","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kalaivanan","family":"Raju","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Raman","family":"Sankar","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5899-7200","authenticated-orcid":false,"given":"Shang-Fan","family":"Lee","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Michael A.","family":"Sentef","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2157-3727","authenticated-orcid":false,"given":"Takashi","family":"Kurumaji","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2279-3078","authenticated-orcid":false,"given":"Xiaoqin","family":"Li","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6345-5809","authenticated-orcid":false,"given":"Peizhe","family":"Tang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2060-3151","authenticated-orcid":false,"given":"Angel","family":"Rubio","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8131-9974","authenticated-orcid":false,"given":"Edoardo","family":"Baldini","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2024,7,17]]},"reference":[{"key":"7678_CR1","doi-asserted-by":"publisher","first-page":"20","DOI":"10.1103\/Physics.2.20","volume":"2","author":"D Khomskii","year":"2009","unstructured":"Khomskii, D. 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