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Impact of Pressure on Magnetic Order in Jarosite.
Klein, Ryan A; Walsh, James P S; Clarke, Samantha M; Guo, Yinsheng; Bi, Wenli; Fabbris, Gilberto; Meng, Yue; Haskel, Daniel; Alp, E Ercan; Van Duyne, Richard P; Jacobsen, Steven D; Freedman, Danna E.
Afiliación
  • Klein RA; Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States.
  • Walsh JPS; Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States.
  • Clarke SM; Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States.
  • Guo Y; Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States.
  • Bi W; Advanced Photon Source , Argonne National Laboratory , 9700 South Cass Avenue , Lemont , Illinois 60439 , United States.
  • Fabbris G; Department of Geology , University of Illinois at Urbana-Champaign , Urbana , Illinois 61801 , United States.
  • Meng Y; Advanced Photon Source , Argonne National Laboratory , 9700 South Cass Avenue , Lemont , Illinois 60439 , United States.
  • Haskel D; Advanced Photon Source , Argonne National Laboratory , 9700 South Cass Avenue , Lemont , Illinois 60439 , United States.
  • Alp EE; HPCAT, Geophysical Laboratory , Carnegie Institute of Washington , Argonne , Illinois 60439 , United States.
  • Van Duyne RP; Advanced Photon Source , Argonne National Laboratory , 9700 South Cass Avenue , Lemont , Illinois 60439 , United States.
  • Jacobsen SD; Advanced Photon Source , Argonne National Laboratory , 9700 South Cass Avenue , Lemont , Illinois 60439 , United States.
  • Freedman DE; Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States.
J Am Chem Soc ; 140(38): 12001-12009, 2018 09 26.
Article en En | MEDLINE | ID: mdl-30063832
Jarosite, a mineral with a kagomé lattice, displays magnetic frustration yet orders magnetically below 65 K. As magnetic frustration can engender exotic physical properties, understanding the complex magnetism of jarosite comprises a multidecade interdisciplinary challenge. Unraveling the nature of the disparate magnetic coupling interactions that lead to magnetic order in jarosite remains an open question. Specifically, there is no observed trend in the interlayer spacing with magnetic order. Similarly, the relationship between metal-ligand bond distance and magnetic order remains uninvestigated. Here, we use applied pressure to smoothly vary jarosite's structure without manipulating the chemical composition, enabling a chemically invariant structure-function study. Using single-crystal and powder X-ray diffraction, we show that high applied pressures alter both the interlayer spacing and the metal-ligand bond distances. By harnessing a suite of magnetic techniques under pressure, including SQUID-based magnetometry, time-resolved synchrotron Mössbauer spectroscopy, and X-ray magnetic circular dichroism, we construct the magnetic phase diagram for jarosite up to 40 GPa. Notably, we demonstrate that the magnetic ordering temperature increases dramatically to 240 K at the highest pressures. Additionally, we conduct X-ray emission spectroscopy, Mössbauer spectroscopy, and UV-visible absorption spectroscopy experiments to comprehensively map the magnetic and electronic structures of jarosite at high pressure. We use these maps to construct chemically pure magnetostructural correlations which fully explain the nature and role of the disparate magnetic coupling interactions in jarosite.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2018 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2018 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos