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The compound forms two-dimensional charge-transfer layers with large interlayer separation induced by bulky ligands, enabling a dimensional crossover of magnetization from two-dimensional to three-dimensional behavior at low temperatures. Applying moderate pressure up to 0.27\u202fGPa selectively compresses the layers, eliminating the dimensional crossover and enhancing ferromagnetic interactions, increasing both the Curie temperature and coercive field. Upon further compression, the interlayer distance reaches a limit, triggering a pressure-induced charge-transfer phase transition from the high-spin CoII\u2013WV to the low-spin CoIII\u2013WIV state, which weakens ferromagnetism and eventually leads to complete paramagnetic behavior at higher pressures. The difference in the compressibility between the soft interlayer regions and the rigid charge-transfer intralayer enables two-step magnetic control solely by pressure, a rare feature in molecule-based magnets. High-pressure X-ray diffraction and microscopic imaging confirm the structural sensitivity of the interlayer regions and correlate the pressure-induced phase transitions with the sequential pressure-induced color changes. These findings demonstrate that the interlayer distance and its rigid layer are key parameters for designing pressure-responsive magnetic materials, offering a new strategy for controllable molecular magnetism via external stimuli.<\/jats:p>","DOI":"10.1021\/jacs.6c10267","type":"journal-article","created":{"date-parts":[[2026,8,7]],"date-time":"2026-08-07T04:01:42Z","timestamp":1786075302000},"page":"34780-34790","source":"Crossref","is-referenced-by-count":0,"title":["Pressure-Selective Magnetic Switching via Spatially\nSeparated Soft Interlayer and Rigid Charge-Transfer Intralayer"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-1401-9373","authenticated-orcid":true,"given":"Wakano","family":"Ota","sequence":"first","affiliation":[{"name":"The University of Tokyo , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 113-0033"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-3807-3567","authenticated-orcid":true,"given":"Kazuki","family":"Nakamura","sequence":"additional","affiliation":[{"name":"Univ Rennes, CNRS, IPR (Institut de Physique)\u2500UMR 6251 , ,","place":["Rennes, France, 35000"]},{"name":"DYNACOM IRL 2015 University of Tokyo\u2500CNRS\u2500Universite de Rennes , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 113-0033"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4086-751X","authenticated-orcid":true,"given":"Gae\u0308l","family":"Privault","sequence":"additional","affiliation":[{"name":"DYNACOM IRL 2015 University of Tokyo\u2500CNRS\u2500Universite de Rennes , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 113-0033"]},{"name":"University of Tsukuba , , 1-1-1 Tennodai , ,","place":["Tsukuba, Japan, 305-8573"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haruki","family":"Taira","sequence":"additional","affiliation":[{"name":"University of Tsukuba , , 1-1-1 Tennodai , ,","place":["Tsukuba, Japan, 305-8573"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Riyo","family":"Nagao","sequence":"additional","affiliation":[{"name":"University of Tsukuba , , 1-1-1 Tennodai , ,","place":["Tsukuba, Japan, 305-8573"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5946-944X","authenticated-orcid":true,"given":"Koji","family":"Nakabayashi","sequence":"additional","affiliation":[{"name":"The University of Tokyo , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 113-0033"]},{"name":"DYNACOM IRL 2015 University of Tokyo\u2500CNRS\u2500Universite de Rennes , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 113-0033"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0810-7411","authenticated-orcid":true,"given":"Eric","family":"Collet","sequence":"additional","affiliation":[{"name":"Univ Rennes, CNRS, IPR (Institut de Physique)\u2500UMR 6251 , ,","place":["Rennes, France, 35000"]},{"name":"DYNACOM IRL 2015 University of Tokyo\u2500CNRS\u2500Universite de Rennes , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 113-0033"]},{"name":"Institut Universitaire de France (IUF) , ,","place":["Paris, France, 75005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hirokazu","family":"Kadobayashi","sequence":"additional","affiliation":[{"name":"Japan Synchrotron Radiation Research Institute (JASRI) , SPring-8 , , ,","place":["Sayo-gun, Hyogo, Japan, 679-5198"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0320-0302","authenticated-orcid":true,"given":"Naohisa","family":"Hirao","sequence":"additional","affiliation":[{"name":"Japan Synchrotron Radiation Research Institute (JASRI) , SPring-8 , , ,","place":["Sayo-gun, Hyogo, Japan, 679-5198"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0509-8444","authenticated-orcid":true,"given":"Laurent","family":"Gue\u0301rin","sequence":"additional","affiliation":[{"name":"Univ Rennes, CNRS, IPR (Institut de Physique)\u2500UMR 6251 , ,","place":["Rennes, France, 35000"]},{"name":"DYNACOM IRL 2015 University of Tokyo\u2500CNRS\u2500Universite de Rennes , , 7-3-1 Hongo , Bunkyo-ku, ,","place":["Tokyo, Japan, 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