Guest-, Light- and Thermally-Modulated Spin Crossover in [FeII2] Supramolecular Helicates

Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier; Teat, Simon J.; Aromi, Guillem

doi:10.1002/chem.201601080

Title: Guest-, Light- and Thermally-Modulated Spin Crossover in [Fe^II₂] Supramolecular Helicates

Journal Article · Tue May 10 00:00:00 EDT 2016 · Chemistry - A European Journal

DOI:https://doi.org/10.1002/chem.201601080· OSTI ID:1459362

Darawsheh, Mohanad ^[1]; Barrios, Leoni A. ^[1]; Roubeau, Olivier ^[2]; Teat, Simon J. ^[3]; Aromi, Guillem ^[1]

Univ. of Barcelona (Spain). Dept of Inorganic Chemistry
Univ. of Zaragoza (Spain). Inst. of Materials Science of Aragon (ICMA) and Spanish National Research Council (CSIC)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Here, a new bis(pyrazolylpyridine) ligand (H₂L) has been prepared to form functional [Fe₂(H₂L)₃]⁴⁺ metallohelicates. Changes to the synthesis yield six derivatives, X@[Fe₂(H₂L)₃]X(PF₆)₂∙xCH₃OH (1, x=5.7 and X=Cl; 2, x=4 and X=Br), X@[Fe₂(H₂L)₃]X(PF₆)₂∙yCH₃OH∙H₂O (1 a, y=3 and X=Cl; 2 a, y=1 and X=Br) and X@[Fe₂(H₂L)₃](I₃)₂∙3 Et₂O (1 b, X=Cl; 2 b, X=Br). Their structure and functional properties are described in detail by single-crystal X-ray diffraction experiments at several temperatures. Helicates 1 a and 2 a are obtained from 1 and 2, respectively, by a single-crystal-to-single-crystal mechanism. The three possible magnetic states, [LS–LS], [LS–HS], and [HS–HS] can be accessed over large temperature ranges as a result of the structural nonequivalence of the Fe^II centers. The nature of the guest (Cl^- vs. Br^-) shifts the spin crossover (SCO) temperature by roughly 40 K. Also, metastable [LS–HS] or [HS–HS] states are generated through irradiation. All helicates (X@[Fe₂(H₂L)₃])³⁺persist in solution.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Government of Catalonia; European Research Council (ERC); Ministry of Science, Innovation and Universities (MICINN) (Spain); European Union (EU). AVEMPACE II Erasmus Mundus Action 2

Grant/Contract Number:: AC02-05CH11231; 258060; CTQ2012‐32247; MAT2014‐53961‐R

OSTI ID:: 1459362

Journal Information:: Chemistry - A European Journal, Vol. 22, Issue 25; Related Information: © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim; ISSN 0947-6539

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 41 works

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CCDC 1455581: Experimental Crystal Structure Determination: INUGIJ06 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn79 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455601: Experimental Crystal Structure Determination: INUJOS09 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnwy The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455317: Experimental Crystal Structure Determination: INUPEO02 : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcqh The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455582: Experimental Crystal Structure Determination: INUGIJ07 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn8b The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455320: Experimental Crystal Structure Determination: INUFII : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvctl The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455319: Experimental Crystal Structure Determination: INUFII02 : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcsk The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455578: Experimental Crystal Structure Determination: INUGIJ03 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn46 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455585: Experimental Crystal Structure Determination: INUGIJ08 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvncf The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455598: Experimental Crystal Structure Determination: INUJOS07 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnsv The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455315: Experimental Crystal Structure Determination: INUPEO : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcnf The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455577: Experimental Crystal Structure Determination: INUGIJ02 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn35 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455580: Experimental Crystal Structure Determination: INUGIJ05 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn68 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455600: Experimental Crystal Structure Determination: INULIO : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnvx The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455316: Experimental Crystal Structure Determination: INUPEO01 : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcpg The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455579: Experimental Crystal Structure Determination: INUGIJ04 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn57 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455599: Experimental Crystal Structure Determination: INUJOS08 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvntw The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455595: Experimental Crystal Structure Determination: INUJOS04 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnpr The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455594: Experimental Crystal Structure Determination: INUJOS03 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnnq The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455324: Experimental Crystal Structure Determination: INUGEF : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) bromide tris(triiodide) diethyl ether solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcyq The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455576: Experimental Crystal Structure Determination: INUGIJ01 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn24 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455584: Experimental Crystal Structure Determination: INUGIJ10 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnbd The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455597: Experimental Crystal Structure Determination: INUJOS06 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnrt The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455575: Experimental Crystal Structure Determination: INUGIJ : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn13 The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455596: Experimental Crystal Structure Determination: INUJOS05 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnqs The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455592: Experimental Crystal Structure Determination: INUJOS01 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnln The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455321: Experimental Crystal Structure Determination: INUFII03 : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcvm The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455591: Experimental Crystal Structure Determination: INUJOS : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnkm The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455583: Experimental Crystal Structure Determination: INUGIJ09 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dichloride bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvn9c The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455593: Experimental Crystal Structure Determination: INUJOS02 : tris(μ-2-(5-(3-(3-(pyridin-2-yl)-1H-pyrazol-5-yl)phenyl)-1H-pyrazol-3-yl)pyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvnmp The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455323: Experimental Crystal Structure Determination: INUGAB : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) chloride tris(triiodide) diethyl ether solvate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcxp The current record is supplemented by this dataset	dataset	February 2016
CCDC 1455322: Experimental Crystal Structure Determination: INUFII01 : tris(μ-2,2'-(1,3-phenylenebis((1H-pyrazole-5,3-diyl)))dipyridine)-di-iron(ii) dibromide bis(hexafluorophosphate) methanol solvate monohydrate Darawsheh, Mohanad; Barrios, Leoni A.; Roubeau, Olivier https://doi.org/10.5517/ccdc.csd.cc1kvcwn The current record is supplemented by this dataset	dataset	February 2016

Title: Guest-, Light- and Thermally-Modulated Spin Crossover in [FeII2] Supramolecular Helicates

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