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60 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3, 4, 5, 6 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I19-Small Molecule Single Crystal Diffraction	In situ single-crystal synchrotron X-ray diffraction studies of biologically active gases in metal-organic frameworks Russell M. Main , Simon M. Vornholt , Cameron M. Rice , Caroline Elliott , Samantha E. Russell , Peter J. Kerr , Mark R. Warren , Russell E. Morris Communications Chemistry 6 DOI: 10.1038/s42004-023-00845-1 Diamond Proposal Number(s): [29217] Open Access Show Abstract ▼ Abstract: Metal-organic frameworks (MOFs) are well known for their ability to adsorb various gases. The use of MOFs for the storage and release of biologically active gases, particularly nitric oxide (NO) and carbon monoxide (CO), has been a subject of interest. To elucidate the binding mechanisms and geometry of these gases, an in situ single crystal X-ray diffraction (scXRD) study using synchrotron radiation at Diamond Light Source has been performed on a set of MOFs that display promising gas adsorption properties. NO and CO, were introduced into activated Ni-CPO-27 and the related Co-4,6-dihydroxyisophthalate (Co-4,6-dhip). Both MOFs show strong binding affinity towards CO and NO, however CO suffers more from competitive co-adsorption of water. Additionally, we show that morphology can play an important role in the ease of dehydration for these two systems.	Mar 2023
I15-Extreme Conditions I19-Small Molecule Single Crystal Diffraction	Comparative structural evolution under pressure of powder and single crystals of the layered antiferromagnet FePS3 David M. Jarvis , Matthew J. Coak , Hayrullo Hamidov , Charles R. S. Haines , Giulio I. Lampronti , Cheng Liu , Shiyu Deng , Dominik Daisenberger , David R. Allan , Mark R. Warren , Andrew R. Wildes , Siddharth S. Saxena Physical Review B 107 DOI: 10.1103/PhysRevB.107.054106 Diamond Proposal Number(s): [15949, 23524] Show Abstract ▼ Abstract: FePS 3 is a layered magnetic van der Waals compound that undergoes a Mott insulator-metal transition under applied pressure. The transition has an associated change in the crystal symmetry and magnetic structure. Understanding the underlying physics of these transitions requires a detailed understanding of the crystal structure as a function of pressure. Two conflicting models have previously been proposed for the evolution of the structure with pressure. To settle the disagreement, we present a study of the pressure-dependent crystal structures using both single-crystal and powder x-ray diffraction measurements. We show unambiguously that the highest-pressure transition involves a collapse of the interplanar spacing, along with an increase in symmetry from a monoclinic to a trigonal space group, to the exclusion of other models. Our collected results are crucial for understanding high-pressure behavior in these materials and demonstrate a clear and complete methodology for exploring complex two-dimensional material structures under pressure.	Feb 2023
I19-Small Molecule Single Crystal Diffraction	Covalent bond shortening and distortion induced by pressurization of thorium, uranium, and neptunium tetrakis aryloxides Jacob J. Shephard , Victoria E. J. Berryman , Tatsumi Ochiai , Olaf Walter , Amy N. Price , Mark R. Warren , Polly L. Arnold , Nikolas Kaltsoyannis , Simon Parsons Nature Communications 13 DOI: 10.1038/s41467-022-33459-7 Diamond Proposal Number(s): [16139] Show Abstract ▼ Abstract: Covalency involving the 5f orbitals is regularly invoked to explain the reactivity, structure and spectroscopic properties of the actinides, but the ionic versus covalent nature of metal-ligand bonding in actinide complexes remains controversial. The tetrakis 2,6-di-tert-butylphenoxide complexes of Th, U and Np form an isostructural series of crystal structures containing approximately tetrahedral MO4 cores. We show that up to 3 GPa the Th and U crystal structures show negative linear compressibility as the OMO angles distort. At 3 GPa the angles snap back to their original values, reverting to a tetrahedral geometry with an abrupt shortening of the M-O distances by up to 0.1 Å. The Np complex shows similar but smaller effects, transforming above 2.4 GPa. Electronic structure calculations associate the M-O bond shortening with a change in covalency resulting from increased contributions to the M-O bonding by the metal 6d and 5f orbitals, the combination promoting MO4 flexibility at little cost in energy.	Oct 2022
I19-Small Molecule Single Crystal Diffraction	Pressure and guest-mediated pore shape modification in a small pore MOF to 1200 bar Charles J. Mcmonagle , Gemma F. Turner , Isabelle Jones , David R. Allan , Mark R. Warren , Konstantin V. Kamenev , Simon Parsons , Paul A. Wright , Stephen A. Moggach Chemical Communications 3 DOI: 10.1039/D2CC04649K Diamond Proposal Number(s): [14164] Show Abstract ▼ Abstract: Guest-mediated pore-shape modification of the metal–organic framework, Sc2BDC3 upon adsorption of n-pentane and isopentane is examined from 50–1200 bar. Rotation of the BDC linker responsible for the change in pore shape occurs at much lower pressures than previously reported, with distinct adsorption behaviour observed between pentane isomers.	Sep 2022
Detectors	Tristan - a 10 million pixel large area time resolved detector for synchrotron use David Omar , Giulio Crevatin , Alan Greer , Ian Horswell , Jonathan Spiers , Richard Plackett , Paul Booker , Gale Lockwood , Dan Beckett , Emily Galvin , John Lipp , Michelangelo Di Palo , Mark Warren , Scott Williams , Nicola Tartoni Ieee Transactions On Nuclear Science DOI: 10.1109/TNS.2022.3204064 Open Access Show Abstract ▼ Abstract: This paper describes the development of the Tristan 10M detector for time resolved synchrotron experiments. Tristan 10M has an unprecedented time resolution (ns time scale) over long duration continuous acquisition (days). The detector is constructed from an array of 160 Timepix3 readout ASIC (about 10 million pixels) flip chip bonded to 10 monolithic silicon sensors which enable it to cover an area large enough to effectively carry out crystallography experiments. The large array of ASICs resulted in a number of severe technical challenges that had to be overcome during the development of the detector. The minimization of the dead area between sensors required the development of a very challenging mechanical and electronic packaging. Such a packaging had to be able to route the large number of data and power lines within the footprint of a sensor, had to effectively sink the heat generated by the ASICs, and had to be able to position the sensors accurately. In addition, the packaging of the detector was designed to be scalable in consideration of possible future larger versions of this detector which added a further challenge. The data driven nature of Timepix3 and the sheer data volume produced by the array of ASICs required us to devise a dedicated hardware, firmware, and software data acquisition architecture. This architecture proved very effective during the commissioning of Tristan10M when time resolved crystallography experiments were carried out.	Sep 2022
I19-Small Molecule Single Crystal Diffraction	Materials discovery and design limits in MDABCO perovskites Samuel D. Gale , Harry J. Lloyd , Louise Male , Mark R. Warren , Lucy K. Saunders , Paul A. Anderson , Hamish H.-M. Yeung Crystengcomm 91 DOI: 10.1039/D2CE00848C Diamond Proposal Number(s): [26118] Open Access Show Abstract ▼ Abstract: We report the structures of three new materials in the MDABCO-based perovskite family. Analysis of the Goldschmidt tolerance factor and octahedral factor enable us to propose compositional limits for pseudo-cubic perovskite phase formation and suggest directions for further materials discovery in this family of new ferroelectrics.	Aug 2022
I19-Small Molecule Single Crystal Diffraction	LED-pump-X-ray-multiprobe crystallography for sub-second timescales Lauren E. Hatcher , Mark R. Warren , Jonathan M. Skelton , Anuradha R. Pallipurath , Lucy K. Saunders , David R. Allan , Paul Hathaway , Giulio Crevatin , David Omar , Ben. H. Williams , Ben A. Coulson , Chick C. Wilson , Paul R. Raithby Communications Chemistry 5 DOI: 10.1038/s42004-022-00716-1 Diamond Proposal Number(s): [17306, 19670] Open Access Show Abstract ▼ Abstract: The visualization of chemical processes that occur in the solid-state is key to the design of new functional materials. One of the challenges in these studies is to monitor the processes across a range of timescales in real-time. Here, we present a pump-multiprobe single-crystal X-ray diffraction (SCXRD) technique for studying photoexcited solid-state species with millisecond-to-minute lifetimes. We excite using pulsed LEDs and synchronise to a gated X-ray detector to collect 3D structures with sub-second time resolution while maximising photo-conversion and minimising beam damage. Our implementation provides complete control of the pump-multiprobe sequencing and can access a range of timescales using the same setup. Using LEDs allows variation of the intensity and pulse width and ensures uniform illumination of the crystal, spreading the energy load in time and space. We demonstrate our method by studying the variable-temperature kinetics of photo-activated linkage isomerism in [Pd(Bu4dien)(NO2)][BPh4] single-crystals. We further show that our method extends to following indicative Bragg reflections with a continuous readout Timepix3 detector chip. Our approach is applicable to a range of physical and biological processes that occur on millisecond and slower timescales, which cannot be studied using existing techniques.	Aug 2022
I19-Small Molecule Single Crystal Diffraction	Single-crystal to single-crystal addition of H2 to [Ir(iPr-PONOP)(propene)][BArF4] and comparison between solid-state and solution reactivity Cameron G. Royle , Lia Sotorrios , Matthew R. Gyton , Claire N. Brodie , Arron L. Burnage , Samantha K. Furfari , Anna Marini , Mark R. Warren , Stuart A. Macgregor , Andrew S. Weller Organometallics DOI: 10.1021/acs.organomet.2c00274 Diamond Proposal Number(s): [25315] Open Access Show Abstract ▼ Abstract: The reactivity of the Ir(I) PONOP pincer complex [Ir(iPr-PONOP)(η2-propene)][BArF4], 6, [iPr-PONOP = 2,6-(iPr2PO)2C6H3N, ArF = 3,5-(CF3)2C6H3] was studied in solution and the solid state, both experimentally, using molecular density functional theory (DFT) and periodic-DFT computational methods, as well as in situ single-crystal to single-crystal (SC-SC) techniques. Complex 6 is synthesized in solution from sequential addition of H2 and propene, and then the application of vacuum, to [Ir(iPr-PONOP)(η2-COD)][BArF4], 1, a reaction manifold that proceeds via the Ir(III) dihydrogen/dihydride complex [Ir(iPr-PONOP)(H2)H2][BArF4], 2, and the Ir(III) dihydride propene complex [Ir(iPr-PONOP)(η2-propene)H2][BArF4], 7, respectively. In solution (CD2Cl2) 6 undergoes rapid reaction with H2 to form dihydride 7 and then a slow (3 d) onward reaction to give dihydrogen/dihydride 2 and propane. DFT calculations on the molecular cation in solution support this slow, but productive, reaction, with a calculated barrier to rate-limiting propene migratory insertion of 24.8 kcal/mol. In the solid state single-crystals of 6 also form complex 7 on addition of H2 in an SC-SC reaction, but unlike in solution the onward reaction (i.e., insertion) does not occur, as confirmed by labeling studies using D2. The solid-state structure of 7 reveals that, on addition of H2 to 6, the PONOP ligand moves by 90° within a cavity of [BArF4]− anions rather than the alkene moving. Periodic DFT calculations support the higher barrier to insertion in the solid state (ΔG‡ = 26.0 kcal/mol), demonstrating that the single-crystal environment gates onward reactivity compared to solution. H2 addition to 6 to form 7 is reversible in both solution and the solid state, but in the latter crystallinity is lost. A rare example of a sigma amine-borane pincer complex, [Ir(iPr-PONOP)H2(η1-H3B·NMe3)][BArF4], 5, is also reported as part of these studies.	Jul 2022
I19-Small Molecule Single Crystal Diffraction	An electric field cell for performing in situ single-crystal synchrotron X-ray diffraction Lucy K. Saunders , Hamish H.-M. Yeung , Mark Warren , Peter Smith , Stuart Gurney , Stephen F. Dodsworth , Inigo Vitorica-Yrezabal , Adrian Wilcox , Paul V. Hathaway , Geoff Preece , Paul Roberts , Sarah A. Barnett , David R. Allan Journal Of Applied Crystallography 54 DOI: 10.1107/S1600576721007469 Diamond Proposal Number(s): [19670, 22964] Open Access Show Abstract ▼ Abstract: With the recent increase in research into ferroelectric, anti-ferroelectric and piezoelectric materials, studying the solid-state properties in situ under applied electric fields is vital in understanding the underlying processes. Where this behaviour is the result of atomic displacements, crystallographic insight has an important role. This work presents a sample environment designed to apply an electric field to single-crystal samples in situ on the small-molecule single-crystal diffraction beamline I19, Diamond Light Source (UK). The configuration and operation of the cell is described as well as its application to studies of a proton-transfer colour-change material.	Oct 2021
I11-High Resolution Powder Diffraction I19-Small Molecule Single Crystal Diffraction	Post‐synthetic modification unlocks a 2D‐to‐3D switch in MOF breathing response: a single‐crystal‐diffraction mapping study Lee Brammer , Elliot J. Carrington , Stephen F. Dodsworth , Sandra Van Meurs , Mark R. Warren Angewandte Chemie International Edition DOI: 10.1002/anie.202105272 Open Access Show Abstract ▼ Abstract: Post-synthetic modification (PSM) of the interpenetrated diamondoid metal-organic framework (Me 2 NH 2 )[In(BDC-NH 2 ) 2 ] (BDC-NH 2 = aminobenzenedicarboxylate) SHF-61 proceeds quantitatively in a single-crystal-to-single-crystal manner to yield the acetamide derivative (Me 2 NH 2 )[In(BDC-NHC(O)Me) 2 ] SHF-62 . Continuous breathing behaviour during activation/desolvation is retained upon PSM, but pore closing now leads to ring-flipping to avert steric clash of amide methyl groups of the modified ligands. This triggers a reduction in the amplitude of the breathing deformation in the two dimensions associated with pore diameter, but a large increase in the third dimension associated with pore length. The MOF is thereby converted from predominantly 2D breathing (in SHF-61 ) to a distinctly 3D breathing motion (in SHF-62 ) indicating a decoupling of the pore-width and pore-length breathing motions. These breathing motions have been mapped by a series of single-crystal diffraction studies.	Jun 2021

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