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Spin Crossover in Fe(II) Complexes with N4S2Coordination

Journal article
Authors Alejandra Arroyave
Anders Lennartsson
Alina Dragulescu-Andrasi
Kasper S. Pedersen
Stergios Piligkos
Sebastian A. Stoian
Samuel M. Greer
Chongin Pak
Oleksandr Hietsoi
Hoa Phan
Stephen Hill
Christine J. McKenzie
Michael Shatruk
Published in Inorganic Chemistry
Volume 55
Pages 5904-5913
ISSN 00201669
Publication year 2016
Published at
Pages 5904-5913
Language en
Subject categories Chemical Sciences

Abstract

© 2016 American Chemical Society. Reactions of Fe(II) precursors with the tetradentate ligand S,S′-bis(2-pyridylmethyl)-1,2-thioethane (bpte) and monodentate NCE - coligands afforded mononuclear complexes [Fe(bpte)(NCE) 2 ] (1, E = S; 2, E = Se; 3, E = BH 3 ) that exhibit temperature-induced spin crossover (SCO). As the ligand field strength increases from NCS - to NCSe - to NCBH 3 - , the SCO shifts to higher temperatures. Complex 1 exhibits only a partial (15%) conversion from the high-spin (HS) to the low-spin (LS) state, with an onset around 100 K. Complex 3 exhibits a complete SCO with T 1/2 = 243 K. While the 2 polymorph also shows the complete SCO with T 1/2 = 192 K, the α-2 polymorph exhibits a two-step SCO with the first step leading to a 50% HS LS conversion with T 1/2 = 120 K and the second step proceeding incompletely in the 80-50 K range. The amount of residual HS fraction of α-2 that remains below 60 K depends on the cooling rate. Fast flash-cooling allows trapping of as much as 45% of the HS fraction, while slow cooling leads to a 14% residual HS fraction. The slowly cooled sample of α-2 was subjected to irradiation in the magnetometer cavity resulting in a light-induced excited spin state trapping (LIESST) effect. As demonstrated by Mössbauer spectroscopy, an HS fraction of up to 85% could be achieved by irradiation at 4.2 K.

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