Detailed X-band Studies of the π–d Molecular Conductor λ-(BETS)₂FeCl₄: Observation of Anomalous Angular Dependence of the g-value

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¹Department of Condensed Matter Physics, Graduate School of Science, Hokkaido University, Sapporo 060-0810, Japan²Condensed Molecular Materials Laboratory, RIKEN Cluster for Pioneering Research, RIKEN, Wako, Saitama 351-0198, Japan

Received June 11, 2018; Accepted September 6, 2018; Published October 3, 2018

The antiferromagnetic insulating ground state of the π–d molecular conductor λ-(BETS)₂FeCl₄ has been under intense debate for the last decades. One of the difficulties in studying this system comes from the needle-shape of its single crystal where crystallographic a^*- and b^*-axes are difficult to identify. We performed electron spin resonance (ESR) measurements of λ-(BETS)₂FeCl₄ with precise angular dependence of the g-value to study the relation between the principal axes of the g-tensor and the crystallographic axes. In the paramagnetic metal phase, the angular dependence of the g-value shows a characteristic “canine-teeth” structure owing to the strong π–d interaction. This structure develops rapidly below 150 K suggesting the enhancement of the π–d spin correlation. The principal axes of the g-value are related to the crystal axes, and a simple two-step method using ESR measurements, (i) find the g-value maximum in the a^*b^*-plane, and (ii) find the linewidth maximum in the b^*c-plane, was examined to find the easy-axis of the antiferromagnetic state. Using the two-step method, we found that antiferromagnetic resonance of the easy-axis appears below 11 K, which is higher than the metal–insulator transition temperature.

https://doi.org/10.7566/JPSJ.87.114702

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Detailed X-band Studies of the π–d Molecular Conductor λ-(BETS)₂FeCl₄: Observation of Anomalous Angular Dependence of the g-value