• Accepted Paper

Investigation of the role of π-d interactions in λ-type salts using pressure-temperature phase diagram

Rikumaru Saito, Takuya Kobayashi, Hiromi Taniguchi, Noriaki Matsunaga, Shuhei Fukuoka, and Atsushi Kawamoto

Phys. Rev. B - Accepted 26 August, 2026

DOI: https://doi.org/10.1103/9pq4-g9wb

Abstract

We performed electrical resistivity and ^{13}C nuclear magnetic resonance (NMR) measurements on λ-(BEDSe-TTF)_2FeCl_4 under various pressures to obtain insights into the effect of π-d interactions on the antiferromagnetic (AF) phase. The resistivity shows that the insulating state is maintained up to 2.0 GPa. ^{13}C NMR measurements reveal that the AF transition occurs at 28, 31, and 23 K under 0.5, 1.0, and 2.0 GPa, respectively, indicating that a single AF phase in λ-(BEDSe- TTF)_2FeCl_4 is observed under various pressures, whereas two AF phases were observed in λ- (BEDSe-TTF)_2GaCl_4. The difference in phase diagrams between the magnetic anion salt, λ- (BEDSe-TTF)_2FeCl_4, and the non-magnetic anion salt, λ-(BEDSe-TTF)_2GaCl_4, is attributed to π-d interactions. These results provide insight into a possible microscopic role of π-d interactions in the Fe salt. The magnetic properties of -(BEDSe-TTF)2FeCl4 are described by the isolated cluster comprising two dimers and two anions with positive and negative π-d interactions, suggesting antiferromagnetic coupling between two dimers in the cluster. We also discuss the possible AF structures of λ-(BEDSe-TTF)_2FeCl_4.

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