We report on the dramatic slowing down of the charge carrier dynamics in a quasi-two-dimensional organic conductor, which can be reversibly tuned through the Mott metal-insulator transition (MIT). At the finite-temperature critical endpoint we observ
e a divergent increase of the resistance fluctuations accompanied by a drastic shift of spectral weight to low frequencies, demonstrating the critical slowing down of the order parameter (doublon density) fluctuations. The slow dynamics is accompanied by non-Gaussian fluctuations, indicative of correlated charge carrier dynamics. A possible explanation is a glassy freezing of the electronic system as a precursor of the Mott MIT.
We utilize a glass-like structural transition in order to induce a Mott metal-insulator transition in the quasi-two-dimensional organic charge-transfer salt $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br. In this material, the terminal ethylene groups of the
BEDT-TTF molecules can adopt two different structural orientations within the crystal structure, namely eclipsed (E) and staggered (S) with the relative orientation of the outer C$-$C bonds being parallel and canted, respectively. These two conformations are thermally disordered at room temperature and undergo a glass-like ordering transition at $T_g sim 75,$K. When cooling through $T_g$, a small fraction that depends on the cooling rate remains frozen in the S configuration, which is of slightly higher energy, corresponding to a controllable degree of structural disorder. We demonstrate that, when thermally coupled to a low-temperature heat bath, a pulsed heating current through the sample causes a very fast relaxation with cooling rates at $T_g$ of the order of several 1000$,$K/min. The freezing of the structural degrees of freedom causes a decrease of the electronic bandwidth $W$ with increasing cooling rate, and hence a Mott metal-insulator transition as the system crosses the critical ratio $(W/U)_{c}$ of bandwidth to on-site Coulomb repulsion $U$. Due to the glassy character of the transition, the effect is persistent below $T_g$ and can be reversibly repeated by melting the frozen configuration upon warming above $T_g$. Both by exploiting the characteristics of slowly-changing relaxation times close to this temperature and by controlling the heating power, the materials can be fine-tuned across the Mott transition. A simple model allows for an estimate of the energy difference between the E and S state as well as the accompanying degree of frozen disorder in the population of the two orientations.
