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The two-dimensional organic superconductor $\lambda$-(BETS)$_2$GaCl$_4$exhibits pronounced charge fluctuations below $T \approx 150$~K, in contrast tothe sibling compound $\kappa$-(BETS)$_2$GaCl$_4$ that remains metallic down tomilli-Kelvin. Infrared spectroscopy reveals only minor splitting in thevibrational features of the latter compound, common to other strongly dimerized$\kappa$-salts. When the organic molecules are arranged in the$\lambda$-pattern, however, a strong vibrational $\nu_{27}(b_{1u})$ mode ispresent, that forms a narrow doublet. %indicating static charge imbalance ofabout 2\%. Most important, when cooling $\lambda$-(BETS)$_2$GaCl$_4$ below150~K, two weak side modes appear due to charge disproportionation that amountsto $2\delta=0.14e$. In analogy to the $\beta^{\prime\prime}$-type organicconductors, we propose that charge fluctuations play an important role inemerging of unconventional superconductivity in \l\ at $T_c=4.7$~K. We discussthe possibility of a charge-density-wave that coexists with the proposedspin-density-wave state.

Charge imbalance in $\lambda$-(BETS)$_2$GaCl$_4$ and their interplay with superconductivity