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Yet, the microscopic mechanism governing Cu\n                    <jats:sup>+<\/jats:sup>\n                    ordering has remained elusive. Here, we combine single\u2010crystal X\u2010ray and neutron diffraction with pair distribution function analysis to uncover a temperature\u2010driven evolution of Cu\n                    <jats:sup>+<\/jats:sup>\n                    ordering, giving rise to an incommensurate quasi\u2010antipolar phase between the paraelectric and antiferroelectric states. The modulation originates from correlated Cu\n                    <jats:sup>+<\/jats:sup>\n                    occupancy redistribution coupled to\n                    <jats:italic>breathing<\/jats:italic>\n                    distortion of surrounding S\n                    <jats:sub>3<\/jats:sub>\n                    triangles, establishing a symmetry\u2010adapted lattice distortion mode. Diffuse scattering persisting over 35\u00a0K above the transition confirms that the structural instability follows an order\u2010disorder mechanism. The spontaneous off\u2010centering of Cu\n                    <jats:sup>+<\/jats:sup>\n                    positions CuCrP\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>6<\/jats:sub>\n                    as a model platform for correlated order\u2010disorder phenomena in 2D layered ferroics, and provides design principles for next\u2010generation memory and logic\u00a0devices.\n                  <\/jats:p>","DOI":"10.1002\/advs.202524227","type":"journal-article","created":{"date-parts":[[2026,2,4]],"date-time":"2026-02-04T19:09:58Z","timestamp":1770232198000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["On the Ordering Mechanism of Cu\n                    <sup>+<\/sup>\n                    in 2D van der Waals Multiferroic CuCrP\n                    <sub>2<\/sub>\n                    S\n                    <sub>6<\/sub>"],"prefix":"10.1002","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-7708-1476","authenticated-orcid":false,"given":"Jiasen","family":"Guo","sequence":"first","affiliation":[{"name":"Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3263-4812","authenticated-orcid":false,"given":"Yongqiang","family":"Cheng","sequence":"additional","affiliation":[{"name":"Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1211-8749","authenticated-orcid":false,"given":"Michael A.","family":"Susner","sequence":"additional","affiliation":[{"name":"Materials and Manufacturing Directorate, Air Force Research Laboratory Wright\u2010Patterson Air Force Base Ohio 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