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Compared with oxide-based systems, molecular materials offer greater structural tunability for realizing coupled ferroic behavior. Here we report a low-symmetry crown ether design for constructing a layered molecular crystal of [(o-fluoroanilinium+)(benzo[18]crown-6)][MnIICrIII(oxalate)3]\u2212, in which supramolecular ferroelectricity coexists with two-dimensional ferromagnetic layers. This compound undergoes a reversible, single-crystal-to-single-crystal phase transition driven by the reorientation and conformational change of the polar benzo[18]crown-6 molecule, involving a 180\u00b0 in-plane rotation and transformation of a polar V-shaped conformation into a planar configuration. Single-crystal X-ray diffraction, dielectric measurements, pyroelectric current, P\u2013E hysteresis loops, and magnetic susceptibility measurements support the coexistence of ferroelectricity and ferromagnetism. Density functional theory (DFT) calculations and structural analysis identify the noncollinear supramolecular geometry of benzo[18]crown-6 units, their tilted assemblies, and the bistable motion as the origin of spontaneous polarization. This work demonstrates the effectiveness of the low-symmetry crown ether in designing molecular multiferroics.<\/jats:p>","DOI":"10.1021\/jacs.6c10197","type":"journal-article","created":{"date-parts":[[2026,8,18]],"date-time":"2026-08-18T20:02:29Z","timestamp":1787083349000},"page":"44218-44227","source":"Crossref","is-referenced-by-count":1,"title":["Low-Symmetry\nCrown Ether Design for Coexisting Ferroelectricity\nand Ferromagnetism in a Two-Dimensional Molecular Crystal"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3374-3348","authenticated-orcid":true,"given":"Jia-bing","family":"Wu","sequence":"first","affiliation":[{"name":"Hokkaido University , , ,","place":["Sapporo, Japan, 001-0020"]},{"name":"University of Glasgow , , ,","place":["Glasgow, U.K., G12 8QQ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kiyonori","family":"Takahashi","sequence":"additional","affiliation":[{"name":"Hokkaido University , , ,","place":["Sapporo, Japan, 001-0020"]},{"name":"Kumamoto University , , ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Masaru","family":"Fujibayashi","sequence":"additional","affiliation":[{"name":"National Institute of Technology, Ube College , , ,","place":["Yamaguchi, Japan, 755-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8852-6992","authenticated-orcid":true,"given":"Ryo","family":"Tsunashima","sequence":"additional","affiliation":[{"name":"Yamaguchi University , , ,","place":["Yamaguchi, Japan, 753-8512"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7275-7123","authenticated-orcid":true,"given":"Yasutaka","family":"Suzuki","sequence":"additional","affiliation":[{"name":"Yamaguchi University , , ,","place":["Yamaguchi, Japan, 753-8512"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8252-186X","authenticated-orcid":true,"given":"Jun","family":"Kawamata","sequence":"additional","affiliation":[{"name":"Yamaguchi University , , ,","place":["Yamaguchi, Japan, 753-8512"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Masato","family":"Haneda","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Hiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4030-786X","authenticated-orcid":true,"given":"Sadafumi","family":"Nishihara","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Hiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4757-4741","authenticated-orcid":true,"given":"Shin-ichiro","family":"Noro","sequence":"additional","affiliation":[{"name":"Hokkaido University , , ,","place":["Sapporo, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Chen","sequence":"additional","affiliation":[{"name":"Nanjing Xiaozhuang University , , ,","place":["Nanjing, China, 211171"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8170-5605","authenticated-orcid":true,"given":"Ichiro","family":"Hisaki","sequence":"additional","affiliation":[{"name":"The University of Osaka , , ,","place":["Osaka, Japan, 560-8531"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3040-1078","authenticated-orcid":true,"given":"Tomoyuki","family":"Akutagawa","sequence":"additional","affiliation":[{"name":"Tohoku University , , ,","place":["Sendai, Japan, 980-8577"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6122-2075","authenticated-orcid":true,"given":"Rui-Kang","family":"Huang","sequence":"additional","affiliation":[{"name":"Hokkaido University , , ,","place":["Sapporo, Japan, 001-0020"]},{"name":"Shantou University , , ,","place":["Shantou, China, 515063"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takayoshi","family":"Nakamura","sequence":"additional","affiliation":[{"name":"Hokkaido University , , ,","place":["Sapporo, Japan, 001-0020"]},{"name":"Hiroshima University , , ,","place":["Hiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,18]]},"reference":[{"issue":"11","key":"2026102111064110700_cit1","doi-asserted-by":"publisher","first-page":"L329","DOI":"10.1088\/0022-3719\/10\/11\/011","article-title":"Ferroelectrically\nInduced Ferromagnetism","volume":"10","author":"Fox","year":"1977","journal-title":"J. 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