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 both 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. Ni0.69Fe0.31TTFtt 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.

1,2-oxaborines can shift into 11 different ring shapes to make modifying molecular cores easy

Annual event draws 700 UChicago scientists, 200 volunteers to share science demonstrations on campus

Polyfluoroarenes often exist in functional molecules; however, construction of alkyl–polyfluoroaryl bonds remains nontrivial, and the current approaches exhibit various limitations. Here we report the...

Susumu Kitagawa, Richard Robson and Omar Yaghi take top prize for discovery and development of versatile materials with a huge surface area

Conductive coordination polymers (CPs) with sulfur-based ligands offer strong metal-ligand interactions and redox tunability, making them promising candidates for electronic applications. Tetrathiaful...

The winners are being acknowledged for their outstanding achievements in chemistry across various fields in the discipline

A nickel-silylene complex is shown to reversibly activate benzene via C–H bond activation at ambient temperature. The benzene C–H bond formally adds across the Ni–Si core to form a nickel-silyl comple...

When the cationic, octahedral terminal nitrido complex of Mo(VI) supported by a diborate pentadentate ligand is generated in the absence of trapping nucleophiles, it rapidly activates the C(sp2)-H bon...

Despite recent advances in primary sulfonamide synthesis, approaches using primary amines as starting points for direct sulfonamide construction remain elusive. Now a formal SO2 insertion into the C–N...

In drug development, replacement of a skeletal carbon with a sulfur atom can result in analogs of bioactive compounds with improved properties. Currently, the sulfur analogs are almost exclusively pre...