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However, there are no literature precedents for spin admixing between the IS (\n                    <jats:italic>S<\/jats:italic>\n                    = 3\/2) and low\u2010spin (LS;\n                    <jats:italic>S<\/jats:italic>\n                    = 1\/2) states, which are purely governed by axial ligation. It is also true that systems showing spin\u2010admixed behavior do not exhibit thermal equilibrium between the spin states, that is, spin crossover (SCO). In this article, we report a unique and rare square planar ferric ion complex, [Na(DME)\n                    <jats:sub>3<\/jats:sub>\n                    ][Fe(L1\n                    <jats:sup>2\u2212<\/jats:sup>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    ] (\n                    <jats:bold>1<\/jats:bold>\n                    ), which exhibits two different physical phenomena: SCO is observed between the spin\u2010admixed states, a phenomenon unprecedented in this context. Field\u2010 and temperature\u2010dependent M\u00f6ssbauer spectra, variable temperature X\u2010band EPR spectra, multifrequency EPR (MF\u2010EPR), and temperature\u2010dependent magnetic susceptibility measurements reveal that the spin\u2010admixed state has contributions from IS (\n                    <jats:italic>S<\/jats:italic>\n                    = 3\/2) and LS (\n                    <jats:italic>S<\/jats:italic>\n                    = 1\/2), unlike other reports in the literature. The detailed electronic structure of\n                    <jats:bold>1<\/jats:bold>\n                    , along with the rationale for quantum spin admixing and SCO, is well supported by theoretical calculations.\n                  <\/jats:p>","DOI":"10.1002\/chem.70994","type":"journal-article","created":{"date-parts":[[2026,4,18]],"date-time":"2026-04-18T10:50:26Z","timestamp":1776509426000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["An Unprecedented Square Planar Fe(III) Complex Exhibiting Spin Crossover Between the Spin\u2010Admixed States"],"prefix":"10.1002","volume":"32","author":[{"given":"Kamal Uddin","family":"Ansari","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai Maharashtra India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dipanti","family":"Borah","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai Maharashtra India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lena","family":"Spillecke","sequence":"additional","affiliation":[{"name":"Kirchhoff Institute for Physics Heidelberg University  Heidelberg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kavipriya","family":"Thangavel","sequence":"additional","affiliation":[{"name":"National High Magnetic Field Laboratory Florida State University  Tallahassee Florida USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pardeep","family":"Kumar","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai Maharashtra India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Purva","family":"Dua","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai Maharashtra India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sourav","family":"Dey","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai Maharashtra India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"R\u00fcdiger","family":"Klingeler","sequence":"additional","affiliation":[{"name":"Kirchhoff Institute for Physics Heidelberg University  Heidelberg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Martin","family":"Cl\u00e9mancey","sequence":"additional","affiliation":[{"name":"Laboratoire De Chimie et Biologie des M\u00e9taux Univ. 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