Spin Glass Behavior and Giant Magnetoresistance via Aliovalent Fe/Ni Alloying in Amorphous Tetrathiafulvalene-Tetrathiolate Coordination Polymers

The discovery of materials with programmable combinations of charge transport and magnetic properties is a major goal in synthetic chemistry. Molecular materials, such as coordination polymers (CPs), are emerging candidates in this field due to their synthetic modularity. While there are many conductive or magnetic CPs, single-component examples with <i>both</i> properties are still emerging. Here we demonstrate how alloying paramagnetic Fe(III) centers into a highly conductive Ni-based CP results in novel amorphous materials with high conductivity and giant magnetoresistance. Aliovalent doping with paramagnetic Fe centers engenders spin-glass transitions, while Ni and the strong π-stacking interactions of tetrathiafulvalene-2,3,6,7-tetrathiolate (TTFtt) ligands support conductivity. <b>Ni</b><sub><b>0.69</b></sub><b>Fe</b><sub><b>0.31</b></sub><b>TTFtt</b> has σ ≈ 200 S/cm and a 1.8 K magnetoresistance of -52% at 5 T, among the largest for any coordination solid. This work demonstrates not only how magnetic properties can be rationally incorporated into conductive CPs, but also an unexpected potential for amorphous materials in spintronic applications.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-10-14
DOI
https://doi.org/10.1021/jacs.5c12985
Citations
1
Primary Topic
Organic and Molecular Conductors Research
Type
article
Field-Weighted Citation Impact
0.43
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article

Spin Glass Behavior and Giant Magnetoresistance via Aliovalent Fe/Ni Alloying in Amorphous Tetrathiafulvalene-Tetrathiolate Coordination Polymers

Shrayesh N. Patel, J. Hofmann, Henry S. La Pierre, Grant R. Wilkinson et al.
1 citations
Journal of the American Chemical Society
Organic and Molecular Conductors Research
0.43
article

Spin Glass Behavior and Giant Magnetoresistance via Aliovalent Fe/Ni Alloying in Amorphous Tetrathiafulvalene-Tetrathiolate Coordination Polymers

Shrayesh N. Patel, J. Hofmann, Henry S. La Pierre, Grant R. Wilkinson, Karena W. Chapman, Maia E. Czaikowski, Barbara Lavina, Andrew Higginbotham, Dmitri V. Talapin, Anna O. Schouten, David A. Mazziotti, Chen‐Yu Lien, John S. Anderson, Alexander S. Filatov, Di Wang, Jiehao Chen
article en
1 citations

Abstract

The discovery of materials with programmable combinations of charge transport and magnetic properties is a major goal in synthetic chemistry. Molecular materials, such as coordination polymers (CPs), are emerging candidates in this field due to their synthetic modularity. While there are many conductive or magnetic CPs, single-component examples with <i>both</i> properties are still emerging. Here we demonstrate how alloying paramagnetic Fe(III) centers into a highly conductive Ni-based CP results in novel amorphous materials with high conductivity and giant magnetoresistance. Aliovalent doping with paramagnetic Fe centers engenders spin-glass transitions, while Ni and the strong π-stacking interactions of tetrathiafulvalene-2,3,6,7-tetrathiolate (TTFtt) ligands support conductivity. <b>Ni</b><sub><b>0.69</b></sub><b>Fe</b><sub><b>0.31</b></sub><b>TTFtt</b> has σ ≈ 200 S/cm and a 1.8 K magnetoresistance of -52% at 5 T, among the largest for any coordination solid. This work demonstrates not only how magnetic properties can be rationally incorporated into conductive CPs, but also an unexpected potential for amorphous materials in spintronic applications.

Journal of the American Chemical SocietyVol. 147(43)
Argonne National Laboratory (US), Georgia Institute of Technology (US), University of Chicago (US), Advanced Photonix (United States) (US), Advanced Photon Source, Center for Nanoscale Materials, Stony Brook University (US)
Openalex Percentile: Top 35%
Organic and Molecular Conductors Research
0.43
DOISourceOpenAlex
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