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Instruments / Technical Area	Publication Details	Published
I15-Extreme Conditions	Encoding complexity within supramolecular analogues of frustrated magnets Andrew Cairns , Matthew Cliffe , Joseph Paddison , Dominik Daisenberger , Matthew G. Tucker , François-xavier Coudert , Andrew Goodwin Nature Chemistry 8, 442 - 447 DOI: 10.1038/nchem.2462 Show Abstract ▼ Abstract: The solid phases of gold(I) and/or silver(I) cyanides are supramolecular assemblies of inorganic polymer chains in which the key structural degrees of freedom—namely, the relative vertical shifts of neighbouring chains—are mathematically equivalent to the phase angles of rotating planar (‘XY’) spins. Here, we show how the supramolecular interactions between chains can be tuned to mimic different magnetic interactions. In this way, the structures of gold(I) and/or silver(I) cyanides reflect the phase behaviour of triangular XY magnets. Complex magnetic states predicted for this family of magnets—including collective spin-vortices of relevance to data storage applications—are realized in the structural chemistry of these cyanide polymers. Our results demonstrate how chemically simple inorganic materials can behave as structural analogues of otherwise inaccessible ‘toy’ spin models and also how the theoretical understanding of those models allows control over collective (‘emergent’) phenomena in supramolecular systems.	May 2016
I11-High Resolution Powder Diffraction	Compositional dependence of anomalous thermal expansion in perovskite-like ABX Ines E. Collings , Joshua A. Hill , Andrew B. Cairns , Richard I. Cooper , Amber L. Thompson , Julia E. Parker , Chiu C. Tang , Andrew L. Goodwin Dalton Transactions DOI: 10.1039/C5DT03263F PMID: 26477747 Diamond Proposal Number(s): [7907] Show Abstract ▼ Abstract: The compositional dependence of thermal expansion behaviour in 19 different perovskite-like metal–organic frameworks (MOFs) of composition [AI][MII(HCOO)3] (A = alkylammonium cation; M = octahedrally-coordinated divalent metal) is studied using variable-temperature X-ray powder diffraction measurements. While all systems show essentially the same type of thermomechanical response—irrespective of their particular structural details—the magnitude of this response is shown to be a function of AI and MII cation radii, as well as the molecular anisotropy of AI. Flexibility is maximised for large MII and small AI, while the shape of AI has implications for the direction of framework hingeing.	Oct 2015
	Zero-strain reductive intercalation in a molecular framework Joshua Hill , Andrew B. Cairns , Jared J. K. Lim , Simon J. Cassidy , Simon J. Clarke , Andrew L. Goodwin Crystengcomm 17, 2925 - 2928 DOI: 10.1039/C4CE02364A Open Access Show Abstract ▼ Abstract: Reductive intercalation of potassium within the molecular framework Ag3[Fe(CN)6] gives rise to a volume strain that is an order of magnitude smaller than is typical for common ion-storage materials. We suggest that framework flexibility might be exploited as a general strategy for reducing cycling strain in battery and ion-storage materials.	Jan 2015
I11-High Resolution Powder Diffraction	Homologous critical behaviour in the molecular frameworks Zn(CN)2 and Cd(imidazolate)2 Ines Collings , Andrew Cairns , Amber Thompson , Julia Parker , Chiu Tang , Matthew G. Tucker , Jadna Catafesta , Claire Levelut , Julien Haines , Vladimir Dmitriev , Philip Pattison , Andrew Goodwin Journal Of The American Chemical Society 135 (20) DOI: 10.1021/ja401268g Show Abstract ▼ Abstract: Using a combination of single-crystal and powder X-ray diffraction measurements, we study temperature- and pressure-driven structural distortions in zinc(II) cyanide (Zn(CN)2) and cadmium(II) imidazolate (Cd(im)2), two molecular frameworks with the anticuprite topology. Under a hydrostatic pressure of 1.52 GPa, Zn(CN)2 undergoes a first-order displacive phase transition to an orthorhombic phase, with the corresponding atomic displacements characterized by correlated collective tilts of pairs of Zn-centered tetrahedra. This displacement pattern sheds light on the mechanism of negative thermal expansion in ambient-pressure Zn(CN)2. We find that the fundamental mechanical response exhibited by Zn(CN)2 is mirrored in the temperature-dependent behavior of Cd(im)2. Our results suggest that the thermodynamics of molecular frameworks may be governed by considerations of packing efficiency while also depending on dynamic instabilities of the underlying framework topology.	Apr 2013

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