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Title: Formation of the layered conductive magnet CrCl 2(pyrazine) 2 through redox-active coordination chemistry [A non-innocent coordination chemistry approach to 2D conductive magnets]

Abstract

The unique properties of graphene, transition-metal dichalcogenides and other two-dimensional (2D) materials have boosted interest in layered coordination solids. In particular, 2D materials that behave as both conductors and magnets could find applications in quantum magnetoelectronics and spintronics. Here, we report the synthesis of CrCl 2(pyrazine) 2, an air-stable layered solid, by reaction of CrCl 2 with pyrazine (pyz). This compound displays a ferrimagnetic order below ~55 K, reflecting the presence of strong magnetic interactions. Electrical conductivity measurements demonstrate that CrCl 2(pyz) 2 reaches a conductivity of 32 mS cm -1 at room temperature, which operates through a 2D hopping-based transport mechanism. These properties are induced by the redox-activity of the pyrazine ligand, which leads to a smearing of the Cr 3 d and pyrazine π states. We suggest that the combination of redox-active ligands and reducing paramagnetic metal ions represents a general approach towards tuneable 2D materials that consist of charge-neutral layers and exhibit both long-range magnetic order and high electronic conductivity.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8];  [8];  [2]; ORCiD logo [9];  [10];  [10];  [11]; ORCiD logo [12]; ORCiD logo [2]
  1. CNRS, Pessac (France); Univ. Bordeaux, Pessac (France); Technical Univ. of Denmark, Lyngby (Denmark)
  2. CNRS, Pessac (France); Univ. Bordeaux, Pessac (France)
  3. Univ. of California, Berkeley, CA (United States)
  4. Univ. of Oxford, Oxford (United Kingdom)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Univ.Andres Bello, Santiago (Chile)
  6. Univ. of Copenhagen, Copenhagen (Denmark)
  7. Technical Univ. of Denmark, Lyngby (Denmark)
  8. Aarhus Univ., Aarhus (Denmark)
  9. CNRS, Pessac (France); Univ. Bordeaux, Pessac (France); Sara Pharm Solutions, Bucharest (Romania)
  10. ESRF – The European Synchrotron, Grenoble (France)
  11. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Kavli Energy Nanosciences Inst. at Berkeley, Berkeley, CA (United States)
  12. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1560564
Grant/Contract Number:  
[AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 10]; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Pedersen, Kasper S., Perlepe, Panagiota, Aubrey, Michael L., Woodruff, Daniel N., Reyes-Lillo, Sebastian E., Reinholdt, Anders, Voigt, Laura, Li, Zheshen, Borup, Kasper, Rouzières, Mathieu, Samohvalov, Dumitru, Wilhelm, Fabrice, Rogalev, Andrei, Neaton, Jeffrey B., Long, Jeffrey R., and Clérac, Rodolphe. Formation of the layered conductive magnet CrCl2(pyrazine)2 through redox-active coordination chemistry [A non-innocent coordination chemistry approach to 2D conductive magnets]. United States: N. p., 2018. Web. doi:10.1038/s41557-018-0107-7.
Pedersen, Kasper S., Perlepe, Panagiota, Aubrey, Michael L., Woodruff, Daniel N., Reyes-Lillo, Sebastian E., Reinholdt, Anders, Voigt, Laura, Li, Zheshen, Borup, Kasper, Rouzières, Mathieu, Samohvalov, Dumitru, Wilhelm, Fabrice, Rogalev, Andrei, Neaton, Jeffrey B., Long, Jeffrey R., & Clérac, Rodolphe. Formation of the layered conductive magnet CrCl2(pyrazine)2 through redox-active coordination chemistry [A non-innocent coordination chemistry approach to 2D conductive magnets]. United States. doi:10.1038/s41557-018-0107-7.
Pedersen, Kasper S., Perlepe, Panagiota, Aubrey, Michael L., Woodruff, Daniel N., Reyes-Lillo, Sebastian E., Reinholdt, Anders, Voigt, Laura, Li, Zheshen, Borup, Kasper, Rouzières, Mathieu, Samohvalov, Dumitru, Wilhelm, Fabrice, Rogalev, Andrei, Neaton, Jeffrey B., Long, Jeffrey R., and Clérac, Rodolphe. Mon . "Formation of the layered conductive magnet CrCl2(pyrazine)2 through redox-active coordination chemistry [A non-innocent coordination chemistry approach to 2D conductive magnets]". United States. doi:10.1038/s41557-018-0107-7. https://www.osti.gov/servlets/purl/1560564.
@article{osti_1560564,
title = {Formation of the layered conductive magnet CrCl2(pyrazine)2 through redox-active coordination chemistry [A non-innocent coordination chemistry approach to 2D conductive magnets]},
author = {Pedersen, Kasper S. and Perlepe, Panagiota and Aubrey, Michael L. and Woodruff, Daniel N. and Reyes-Lillo, Sebastian E. and Reinholdt, Anders and Voigt, Laura and Li, Zheshen and Borup, Kasper and Rouzières, Mathieu and Samohvalov, Dumitru and Wilhelm, Fabrice and Rogalev, Andrei and Neaton, Jeffrey B. and Long, Jeffrey R. and Clérac, Rodolphe},
abstractNote = {The unique properties of graphene, transition-metal dichalcogenides and other two-dimensional (2D) materials have boosted interest in layered coordination solids. In particular, 2D materials that behave as both conductors and magnets could find applications in quantum magnetoelectronics and spintronics. Here, we report the synthesis of CrCl2(pyrazine)2, an air-stable layered solid, by reaction of CrCl2 with pyrazine (pyz). This compound displays a ferrimagnetic order below ~55 K, reflecting the presence of strong magnetic interactions. Electrical conductivity measurements demonstrate that CrCl2(pyz)2 reaches a conductivity of 32 mS cm-1 at room temperature, which operates through a 2D hopping-based transport mechanism. These properties are induced by the redox-activity of the pyrazine ligand, which leads to a smearing of the Cr 3d and pyrazine π states. We suggest that the combination of redox-active ligands and reducing paramagnetic metal ions represents a general approach towards tuneable 2D materials that consist of charge-neutral layers and exhibit both long-range magnetic order and high electronic conductivity.},
doi = {10.1038/s41557-018-0107-7},
journal = {Nature Chemistry},
number = [10],
volume = [10],
place = {United States},
year = {2018},
month = {9}
}

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    The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets
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