A new Hofmann-type metal-organic framework with bent pillar ligand, [Fe(dpoda){Ag(CN)}] (dpoda = 2,5-di-(pyridyl)-1,3,4-oxadiazole), was synthesized. Four-, two- and one-step spin-crossover (SCO) properties were obtained by using different sizes of aromatic guests. Most importantly, hysteretic four-step SCO behaviour with the sequence of LS ↔ HSLS↔ HSLS↔ HSLS↔ HS is observed for the first time.
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Ising-Like Model Hasn't Yet Said Its Last Word: Exact and Mean-Field Investigations of 2, 3 and 4-Body Interactions in 1D Ising Chain of Binuclear Spin-Crossover Solids.
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We investigate the static properties of a new class of 1D Ising-like Hamiltonian for binuclear spin-crossover materials accounting for two-, three-, and four-body short-range interactions between binuclear units of spins and . The following 2-, 3-, and 4-body , , and terms are considered, in addition to intra-binuclear interactions, such as effective ligand-field energy and exchange-like coupling. An exact treatment is carried out within the frame of the transfer matrix method, leading to a 4×4 matrix from which, we obtained the thermal evolution of the thermodynamic quantities.
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Departamento de Química Inorgánica, Instituto de Ciencia Molecular (ICMol), Universidad de Valencia Valencia Spain
A binary reversible switch between low-temperature multi-step spin crossover (SCO), through the evolution of the population () with high-spin (HS)-low-spin (LS) sequence: HSLS (state 1) ↔ HSLS (state 2) ↔ HSLS (state 3) ↔ HSLS (state 4) ↔ HSLS (state 5), and complete one step hysteretic spin transition featuring 20 K wide thermal hysteresis centred at 290 K occurs in the three-dimensional (3D) Hofmann-type porous coordination polymer {Fe(3,8phen)[Au(CN)]}·PhNO (3,8phen = 3,8-phenanthroline, PhNO = nitrobenzene), made up of two identical interpenetrated pcu-type frameworks. The included PhNO guest ( = 1, ) acts as a molecular wedge between the interpenetrated 3D frameworks PhNO-3,8phen intermolecular recognition and is the source of the strong elastic frustration responsible for the multi-step regime. Detailed X-ray single crystal analysis reflects competition between spatial periodicities of structurally inequivalent HS and LS SCO centres featuring: (i) symmetry breaking (state 3) with ⋯HS-LS⋯ ordering with = 1/2; and (ii) occurrence of spatial modulation of the structure providing evidence for stabilization of local or aperiodic ordered mixed spin states for states 2 and 4 (with ≈ 2/3) and 4 (with ≈ 1/3), respectively.
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Chem Commun (Camb)
September 2019
Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, P. R. China.
A new Hofmann-type metal-organic framework with bent pillar ligand, [Fe(dpoda){Ag(CN)}] (dpoda = 2,5-di-(pyridyl)-1,3,4-oxadiazole), was synthesized. Four-, two- and one-step spin-crossover (SCO) properties were obtained by using different sizes of aromatic guests. Most importantly, hysteretic four-step SCO behaviour with the sequence of LS ↔ HSLS↔ HSLS↔ HSLS↔ HS is observed for the first time.
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Article Synopsis
- - The study focuses on two new 3D porous compounds featuring iron and silver or gold, which have been structurally characterized and studied for their magnetic properties.
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Materials with hysteretic multi-step spin-crossover (SCO) have potential application in high-order data storage. Here, an unprecedented hysteretic four-step SCO behavior with the sequence of LS↔HS LS ↔HS LS ↔ HS LS ↔HS is found in a three-dimensional (3D) Hofmann-type metal-organic framework (MOF), which is evidenced by magnetic, differential scanning calorimetry, and crystal data. Further experiments involving guest exchange leads to the first reversible modulation of four-, two-, and one-stepped SCO behaviors, which provides a new strategy for developing multi-step SCO materials.
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