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Inelastic neutron scattering measurements on the molecular dimer-Mottinsulator $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl reveal a phonon anomaly ina wide temperature range. Starting from $T_{\rm ins}\sim50$-$60$ K where thecharge gap opens, the low-lying optical phonon modes become overdamped uponcooling towards the antiferromagnetic ordering temperature $T_\mathrm{N} = 27$K, where also a ferroelectric ordering at $T_{\rm FE} \approx T_{\rm N}$occurs. Conversely, the phonon damping becomes small again when spins andcharges are ordered below $T_\mathrm{N}$, while no change of the latticesymmetry is observed across $T_\mathrm{N}$ in neutron diffraction measurements.We assign the phonon anomalies to structural fluctuations coupled to charge andspin degrees of freedom in the BEDT-TTF molecules.

Lattice dynamics coupled to charge and spin degrees of freedom in the molecular dimer-Mott insulator $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl