Phonon renormalization effects accompanying the 6 K anomaly in the Quantum Spin Liquid Candidate kappa-(BEDT-TTF)₂Cu₂(CN)₃

The low-temperature state of the quantum spin liquid candidate $\kappa$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$ emerges via an anomaly at $T^{*}\sim6$ K. Although signatures of this anomaly have been revealed in various quantities, its origin has remained unclear. Here we report inelastic neutron scattering measurements on single crystals of $\kappa$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$, aiming at studying phonon renormalization effects at $T^{*}$. A drastic change was observed in the phonon damping across $T^{*}$ for a breathing mode of BEDT-TTF dimers at $E=4.7$ meV. The abrupt change in the phonon damping is attributed to a phase transition into a valence bond solid state based on an effective model describing the spin-charge coupling in this dimer-Mott system.