Selective observation of sublattice magnetization in the molecular π−d system λ−(BEDT−STF)2FeCl4 studied by C13 NMR

We have performed $^{13}\mathrm{C}$ NMR measurements on $\ensuremath{\lambda}\ensuremath{-}{(\mathrm{BEDT}\ensuremath{-}\mathrm{STF})}_{2}{\mathrm{FeCl}}_{4}$ to reveal the mechanism of unconventional paramagneticlike behavior observed in $\ensuremath{\lambda}$-type molecular $\ensuremath{\pi}\ensuremath{-}d$ systems. $^{13}\mathrm{C}$ NMR spectra and nuclear spin-lattice relaxation rate $1/{T}_{1}$ revealed that the $\ensuremath{\pi}$ and $3d$ electron systems undergo an antiferromagnetic transition simultaneously at 16 K with the assistance of the $\ensuremath{\pi}\ensuremath{-}d$ interaction. We found that the sublattice magnetizations of the $\ensuremath{\pi}$ and $3d$ spins show different temperature dependence below ${T}_{\mathrm{N}}$, which is derived from the magnetic coupling between the two sublattice systems with different magnetic natures. We discuss the relationship between the two different magnetization processes and the unconventional magnetic behavior in $\ensuremath{\lambda}$-type molecular $\ensuremath{\pi}\ensuremath{-}d$ system.