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Recently, evidence of the first purely 2D multiferroic material was\u00a0reported in monolayer NiI<jats:sub>2<\/jats:sub>. However, probing multiferroicity with scattering\u2010based and optical bulk techniques is challenging on 2D materials, and experiments on the atomic scale are needed to fully characterize the multiferroic order at the monolayer limit. Here, scanning tunneling microscopy (STM) supported by density functional theory (DFT) calculations is used to probe and characterize the multiferroic order in monolayer NiI<jats:sub>2<\/jats:sub>. It is demonstrated that the type\u2010II multiferroic order displayed by NiI<jats:sub>2<\/jats:sub>, arising from the combination of a magnetic spin spiral order and a strong spin\u2010orbit coupling, allows probing the multiferroic order in the STM experiments. Moreover, the magnetoelectric coupling of NiI<jats:sub>2<\/jats:sub> is directly probed by external electric field manipulation of the multiferroic domains. The findings establish a novel point of view to analyze magnetoelectric effects at the microscopic level, paving the way toward engineering new multiferroic orders in van der Waals materials and their\u00a0heterostructures.<\/jats:p>","DOI":"10.1002\/adma.202311342","type":"journal-article","created":{"date-parts":[[2024,1,19]],"date-time":"2024-01-19T13:24:35Z","timestamp":1705670675000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":66,"title":["Atomic\u2010Scale Visualization of Multiferroicity in Monolayer NiI<sub>2<\/sub>"],"prefix":"10.1002","volume":"36","author":[{"given":"Mohammad","family":"Amini","sequence":"first","affiliation":[{"name":"Department of Applied Physics Aalto University  Aalto FI\u201000076 Finland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3385-6409","authenticated-orcid":false,"given":"Adolfo 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