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Instruments / Technical Area	Publication Details	Published
I11-High Resolution Powder Diffraction	Magnetic and magnetocaloric properties of the A2LnSbO6 lanthanide oxides on the frustrated fcc lattice Eliseanne C. Koskelo , Nicola D. Kelly , Liam A. V. Nagle-Cocco , Joshua D. Bocarsly , Paromita Mukherjee , Cheng Liu , Qiang Zhang , Sian E. Dutton Inorganic Chemistry DOI: 10.1021/acs.inorgchem.3c01137 Diamond Proposal Number(s): [28349] Open Access Show Abstract ▼ Abstract: Frustrated lanthanide oxides are promising candidates for cryogen-free magnetic refrigeration due to their suppressed ordering temperatures and high magnetic moments. While much attention has been paid to the garnet and pyrochlore lattices, the magnetocaloric effect in frustrated face-centered cubic (fcc) lattices remains relatively unexplored. We previously showed that the frustrated fcc double perovskite Ba2GdSbO6 is a top-performing magnetocaloric material (per mol Gd) because of its small nearest-neighbor interaction between spins. Here we investigate different tuning parameters to maximize the magnetocaloric effect in the family of fcc lanthanide oxides, A2LnSbO6 (A = {Ba2+, Sr2+} and Ln = {Nd3+, Tb3+, Gd3+, Ho3+, Dy3+, Er3+}), including chemical pressure via the A site cation and the magnetic ground state via the lanthanide ion. Bulk magnetic measurements indicate a possible trend between magnetic short-range fluctuations and the field-temperature phase space of the magnetocaloric effect, determined by whether an ion is a Kramers or a non-Kramers ion. We report for the first time on the synthesis and magnetic characterization of the Ca2LnSbO6 series with tunable site disorder that can be used to control the deviations from Curie–Weiss behavior. Taken together, these results suggest fcc lanthanide oxides as tunable systems for magnetocaloric design.	Jun 2023
	Ultrawide temperature range super-invar behavior of R2(Fe,Co)17 materials (R = rare earth) Yili Cao , Kun Lin , Sergii Khmelevskyi , Maxim Avdeev , Keith M. Taddei , Qiang Zhang , Qingzhen Huang , Qiang Li , Kenichi Kato , Chiu Chung Tang , Alexandra Gibbs , Chin-Wei Wang , Jinxia Deng , Jun Chen , Hongjie Zhang , Xianran Xing Physical Review Letters 127 DOI: 10.1103/PhysRevLett.127.055501 Show Abstract ▼ Abstract: Super Invar (SIV), i.e., zero thermal expansion of metallic materials underpinned by magnetic ordering, is of great practical merit for a wide range of high precision engineering. However, the relatively narrow temperature window of SIV in most materials restricts its potential applications in many critical fields. Here, we demonstrate the controlled design of thermal expansion in a family of R 2 ( Fe , Co ) 17 materials ( R = rare Earth). We find that adjusting the Fe-Co content tunes the thermal expansion behavior and its optimization leads to a record-wide SIV with good cyclic stability from 3–461 K, almost twice the range of currently known SIV. In situ neutron diffraction, Mössbauer spectra and first-principles calculations reveal the 3 d bonding state transition of the Fe-sublattice favors extra lattice stress upon magnetic ordering. On the other hand, Co content induces a dramatic enhancement of the internal molecular field, which can be manipulated to achieve “ultrawide” SIV over broad temperature, composition and magnetic field windows. These findings pave the way for exploiting thermal-expansion-control engineering and related functional materials.	Jul 2021
I19-Small Molecule Single Crystal Diffraction	Solution and surface-confined chloride anion templated redox-active ferrocene catenanes Nicholas H. Evans , Habibur Rahman , Alexandre V. Leontiev , Neil D. Greenham , Grzegorz A. Orlowski , Qiang Zeng , Robert M. J. Jacobs , Christopher J. Serpell , Nathan L. Kilah , Jason J. Davis , Paul D. Beer Chemical Science 3 (4), 1080-1089 DOI: 10.1039/c2sc00909a Diamond Proposal Number(s): [1858] Show Abstract ▼ Abstract: The first examples of ferrocene containing catenanes, in solution and assembled on a surface are described. Chloride anion templation is exploited to synthesize redox-active [2]- and [3]-catenanes via Grubbs ring closing metathesis, utilizing a novel ferrocene-appended isophthalamide macrocycle. X-ray crystal structures of both catenanes were determined. The ability of the [2]catenane to selectively bind and characteristically sense its chloride anion template is demonstrated by use of 1H NMR and electrochemical voltammetric techniques. Self-assembled monolayers of analogous surface-confined catenanes have been prepared on gold. In addition to being characterized by cyclic voltammetry and ellipsometry, detailed information regarding the structure of the catenane monolayers has been provided by use of angle integrated high resolution X-ray photoelectron spectroscopy.	Jan 2012

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