Abstract
AbstractA molecular Mott insulator β′‐EtMe3Sb[Pd(dmit)2]2 with a quasi‐triangular lattice of a dimer unit [Pd(dmit)2] exhibits quantum spin liquid (QSL) behavior. We introduced Me4Sb+ or Et2Me2Sb+ to the cation site of this anion radical salt without altering its crystal symmetry. The mixing ratio and lattice parameters of these mixed crystals can be continuously tuned. We calculated intermolecular transfer integrals between highest occupied molecular orbitals (HOMOs) based on structural data. Increasing the number of ethyl groups at the cation site reduces the anisotropy of the triangular lattice, and the dimer units form an almost regular triangular lattice in pure Et2Me2Sb salt. In this process, the Pd(dmit)2 molecule is slightly curved to exhibit a crescent shape. This distortion plays an important role in tuning the interdimer transfer integrals.
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