Dynamics of ethylene groups and hyperfine interactions between donor and anion molecules in $\lambda$-type organic conductors studied by ${}^{69,71}$Ga-NMR spectroscopy

We present the results of ${}^{69,71}$Ga-NMR measurements on an organic antiferromagnet $\lambda$-(BEDSe-TTF)${}_2$GaCl${}_4$ [BEDSe-TTF=bis(ethylenediseleno)tetrathiafulvalene], with comparison to reports on $\lambda$-(BETS)${}_2$GaCl${}_4$ [BETS=bis(ethylenedithio)tetraselenafulvalene] [T. Kobayashi et al., Phys. Rev. B 102, 235131 (2020)]. We found that the dynamics of two crystallographically independent ethylene groups induce two types of quadrupolar relaxation in the high-temperature region. As the ethylene motion freezes, hyperfine (HF) interactions develop between $\pi$ spin and Ga nuclear spin below 100 K, and thereby magnetic fluctuations of the $\pi$-spin system are detected even from the Ga site. The HF interaction in $\lambda$-(BETS)${}_2$GaCl${}_4$ was more than twice as large as in $\lambda$-(BEDSe-TTF)${}_2$GaCl${}_4$, implying that the short contacts between Cl atoms and the chalcogens of fulvalene part are essential for the transferred HF interaction. We propose that NMR using nuclei in anion layers is useful for studying interlayer interactions in organic conductors, which have not been studied experimentally. In addition, because the mechanism of the transferred HF interaction is considered to be the same as $\pi$-$d$ interaction in isostructural Fe-containing $\lambda$-type salts, our findings aid in the understanding of their physical properties.