Abstract

Coulomb repulsion among conduction electrons in solids hinders their motion and leads to a rise in resistivity. A regime of electronic phase separation is expected at the first-order phase transition between a correlated metal and a paramagnetic Mott insulator, but remains unexplored experimentally as well as theoretically nearby T = 0. We approach this issue by assessing the complex permittivity via dielectric spectroscopy, which provides vivid mapping of the Mott transition and deep insight into its microscopic nature. Our experiments utilizing both physical pressure and chemical substitution consistently reveal a strong enhancement of the quasi-static dielectric constant ε1 when correlations are tuned through the critical value. All experimental trends are captured by dynamical mean-field theory of the single-band Hubbard model supplemented by percolation theory. Our findings suggest a similar ’dielectric catastrophe’ in many other correlated materials and explain previous observations that were assigned to multiferroicity or ferroelectricity.

Highlights

  • Insulator-metal transitions (IMTs) remain one of the unresolved science problems of condensed-matter physics, which are rather general and of fundamental importance

  • The substitutional series κ-[(BEDT-TTF)1−x(BEDT-STF)x]2Cu2(CN)[3] (0 ≤ x ≤ 1, abbreviated κSTFx) spans the interval ranging from a Mott insulator to a Fermiliquid metal

  • We focus on the out-of-plane dielectric response measured from f = 7.5 kHz to 5 MHz down to T = 5 K. Both physical pressure and BEDT-STF substitution allow us to monitor the permittivity while shifting the system across the first-order IMT

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Summary

Introduction

Insulator-metal transitions (IMTs) remain one of the unresolved science problems of condensed-matter physics, which are rather general and of fundamental importance Intriguing are those IMTs not associated with static symmetry changes, where paradigms for conventional phase transitions provide little guidance. IMTs with no symmetry breaking were identified around the Mott transition[2,3,4,5], which bears close connection to exotic states of strongly correlated electron matter, such as unconventional superconductivity and quantum spin liquids (QSLs). While commonly concealed by antiferromagnetism, recent development in the field of organic QSLs enabled investigation of the lowtemperature Mott IMT in absence of magnetic order[11,12,13,14], revealing finite-frequency precursors of the metal already on the insulating side[15]

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