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Here we present a series of cyanide-bridged {W6Co9} clusters, [Co@{W(CN)8}6{Co(L)}6{Co(H2O)x(MeOH)3\u2013x}2]\u00b7sol {L = 2,2,2-tris(1H-pyrazolyl)ethanol, x = 3, sol = MeOH (1) and EtOH (3); L = 1,1\u2032,1\u2033-(2-(allyloxy)ethane-1,1,1-triyl)tris(1H-pyrazole), x = 2, sol = 4H2O (2)}, that exhibit unprecedented coexistence of reversible SCO, MMET, and photoinduced slow magnetic relaxation. By strategically modulating ligand fields and supramolecular packing, we achieve distinct switching behaviors: one-step incomplete transitions in elastically frustrated triangular-packed systems (1 and 3) and a two-step complete transition in a nonfrustrated grid-like system (2). Remarkably, the frustrated systems exhibit \u201cspin-state-ice-like\u201d behavior, with each triangular unit adopting either a two high-spin\/one low-spin (2HS\/1LS) or 1HS\/2LS configuration, representing the first experimental observation of such behavior in molecular clusters. These findings establish a new paradigm for designing multistable magnetic materials with coupled electronic and spin transitions, offering insights into the interplay between elastic frustration and cooperative spin-state switching.<\/jats:p>","DOI":"10.1021\/jacs.6c02220","type":"journal-article","created":{"date-parts":[[2026,6,4]],"date-time":"2026-06-04T05:27:52Z","timestamp":1780550872000},"page":"23818-23828","source":"Crossref","is-referenced-by-count":0,"title":["A Molecular\nPlayground for Spin-State Ice and Coupled\nElectron\u2013Spin Dynamics"],"prefix":"10.1021","volume":"148","author":[{"given":"Shihao","family":"Liu","sequence":"first","affiliation":[{"name":"Southern University of Science and Technology (SUSTech) , , ,","place":["Shenzhen, China, 518055"]},{"name":"National University of Singapore , , ,","place":["Singapore, Singapore, 117543"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zi-Yi","family":"Chen","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology (SUSTech) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifan","family":"Deng","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi-Fei","family":"Deng","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology (SUSTech) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qi","family":"Li","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology (SUSTech) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiong","family":"Yang","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology (SUSTech) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8092-5959","authenticated-orcid":true,"given":"Bing-Wu","family":"Wang","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kim R.","family":"Dunbar","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77840"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1676-2427","authenticated-orcid":true,"given":"Yuan-Zhu","family":"Zhang","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology (SUSTech) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,6,4]]},"reference":[{"issue":"7","key":"2026073023081731400_cit1","doi-asserted-by":"publisher","first-page":"644","DOI":"10.1038\/nchem.2547","article-title":"Dynamic molecular\ncrystals with switchable physical properties","volume":"8","author":"Sato","year":"2016","journal-title":"Nat. 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