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We present a pathway for thermal bistability detectable in four physical properties: magnetic, light absorption, second\u2010harmonic generation (SHG), and dielectric. We report a novel heterometallic (TBA){[Fe<jats:sup>II<\/jats:sup>(phIN)<jats:sub>4<\/jats:sub>][Re<jats:sup>V<\/jats:sup>(CN)<jats:sub>8<\/jats:sub>]}\u2009\u22c5\u2009(phIN) (<jats:bold>1<\/jats:bold>) (TBA=tetrabutylammonium cation, phIN=phenyl isonicotinate) cyanido\u2010bridged chain material. Owing to an appropriate {N<jats:sub>6<\/jats:sub>} coordination sphere of Fe(II) centers, <jats:bold>1<\/jats:bold> reveals a thermal spin crossover (SCO) effect which is complete and cooperative providing a distinct thermal hysteresis loop in magnetic measurements. Moreover, it exhibits simultaneous thermal bistability in (a) visible\u2010light absorption due to the presence of efficient d\u2010d electronic transitions in the low\u2010spin (LS) state, (b) SHG activity as it crystallizes in a polar <jats:italic>C<\/jats:italic>c space group due to the bulky substituent on phIN ligands, and (c) dielectric parameters, including dielectric constant, which can be correlated with subtle changes in polarity between LS and HS (high spin) phases. Thus, we present a remarkable thermally controlled hysteretic behavior in four physical functionalities realized by properly functionalizing an SCO\u2010active coordination compound.<\/jats:p>","DOI":"10.1002\/anie.202419242","type":"journal-article","created":{"date-parts":[[2024,11,26]],"date-time":"2024-11-26T04:44:17Z","timestamp":1732596257000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Thermal Bistability of Magnetic Susceptibility, Light Absorption, Second Harmonic Generation, and Dielectric Properties in a Polar Spin\u2010Crossover Iron\u2013Rhenium Chain Material"],"prefix":"10.1002","volume":"64","author":[{"given":"Tomasz","family":"Charytanowicz","sequence":"first","affiliation":[{"name":"Faculty of Chemistry Jagiellonian University  Gronostajowa 2 30-387 Krak\u00f3w Poland"},{"name":"Doctoral School of Exact and Natural Sciences Jagiellonian University in Krak\u00f3w  \u0141ojasiewicza 11 30-348 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