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The dimer Mott insulator λ-(BEDT-STF)2GaCl4 undergoes no magnetic order down to the lowest temperatures, suggesting the formation of a novel quantum disordered state. Our frequency and temperature-dependent investigations of the dielectric response reveal a relaxor-like behavior below T≈100 K for all three axes, similar to other spin liquid candidates. Optical measurement of the charge-sensitive vibrational mode ν27(b1u) identifies a charge disproportionation Δρ≈0.04e on the dimer that exists up to room temperature and originates from inequivalent molecules in the weakly coupled dimers. The linewidth of the charge sensitive mode is broader than that of typical organic conductors, supporting the existence of a disordered electronic state.

Dielectric Anomaly and Charge Fluctuations in the Non-Magnetic Dimer Mott Insulator λ-(BEDT-STF)2GaCl4