Journal
NANO LETTERS
Volume 21, Issue 22, Pages 9746-9753Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c03663
Keywords
Molecular magnet; emerged metallicity; electric-dipole; one-dimensional
Categories
Funding
- U.S. Division of Materials Sciences and Engineering [DE-SC0018631]
- U.S. Army Research Office [W911NF-18-2-0202]
- National Science Foundation, Directorate for Mathematical and Physical Sciences [DMR-2003932]
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This study presents the design and growth of one-dimensional supramolecular wires, addressing the missing ferromagnetism in ET molecule-based charge-transfer salts. Metallicity is induced by electric current and the stabilization of ferromagnetic spin interaction is achieved by tuning the strain effect of molecular contacts. This breakthrough offers a pathway to explore low-dimensional supramolecular materials exhibiting strong electron correlation, metallicity, and ferromagnetism.
Supramolecular engineering bridges molecular assembly with macromolecular charge-transfer salts, promising the design to construct supramolecular architectures that integrate cooperative properties difficult or impossible to find in conventional lattices. Here, we report the crystal engineering design and kinetic growth of one-dimensional supramolecular wires composed of bis(ethylenedithio)-tetrathiafulvalene (ET+) cation and polymeric Cu[N(CN)(2)](2)(-) anion. A bulk ferromagnetic order is discovered for filling up the gap where strong ferromagnetism is missing in such ET molecule-based charge-transfer salts. Metallicity is induced by electric current from the semiconducting wire, which is attributed to strain effect by tuning its close molecular contact. This structural feature is evidenced through the combination of various mechanistic spectroscopic studies. Electric dipole is established from the close molecular contacts and is suggestive to stabilize ferromagnetic spin interaction through anions bridging spin sites. The breakthrough shown here provides a pathway to explore low-dimensional supramolecular materials exhibiting strong electron correlation, metallicity, and ferromagnetism.
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