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Title: Pressure-induced magnetic crossover driven by hydrogen bonding in CuF2(H2O)2(3-chloropyridine)

Here, hydrogen bonding plays a foundational role in the life, earth, and chemical sciences, with its richness and strength depending on the situation. In molecular materials, these interactions determine assembly mechanisms, control superconductivity, and even permit magnetic exchange. In spite of its long-standing importance, exquisite control of hydrogen bonding in molecule-based magnets has only been realized in limited form and remains as one of the major challenges. Here, we report the discovery that pressure can tune the dimensionality of hydrogen bonding networks in CuF2(H2O)2(3-chloropyridine) to induce magnetic switching. Specifically, we reveal how the development of exchange pathways under compression combined with an enhanced ab-plane hydrogen bonding network yields a three dimensional superexchange web between copper centers that triggers a reversible magnetic crossover. Similar pressure- and strain-driven crossover mechanisms involving coordinated motion of hydrogen bond networks may play out in other quantum magnets.
 [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [5] ;  [6] ;  [4] ;  [7] ;  [1]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States); Univ. of Florida, Gainesville, FL (United States)
  3. Carnegie Institution of Washington, Washington, D.C. (United States); Jilin Univ., Changchun (China)
  4. Virginia Commonwealth Univ., Richmond, VA (United States)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); National Science Foundation, Arlington, VA (United States)
  6. Virginia Commonwealth Univ., Richmond, VA (United States); Center for Applied Physics and Technology of Peking Univ., Beijing (China)
  7. Carnegie Institution of Washington, Washington, D.C. (United States)
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 4; Journal ID: ISSN 2045-2322
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY chemical physics; infrared spectroscopy; Raman spectroscopy