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Spin Crossover in Fe(II) Complexes with N4S2Coordination

Artikel i vetenskaplig tidskrift
Författare 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
Publicerad i Inorganic Chemistry
Volym 55
Sidor 5904-5913
ISSN 00201669
Publiceringsår 2016
Publicerad vid
Sidor 5904-5913
Språk en
Ämneskategorier Kemi

Sammanfattning

© 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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