Effect of External Pressure on the Metal–Insulator Transition of the Organic Quasi-Two-Dimensional Metal K-(BEDT-TTF)2Hg(SCN)2Br

The metal–insulator transition in the organic quasi-two-dimensional metal κ-(BEDT-TTF)2Hg(SCN)2Br at TMI ≈ 90 K has been investigated. The crystal structure changes during this transition from monoclinic above TMI to triclinic below TMI. A theoretical study suggested that this phase transition should be of the metal-to-metal type and brings about a substantial change of the Fermi surface. Apparently, the electronic system in the triclinic phase is unstable toward a Mott insulating state, leading to the growth of the resistance when the temperature drops below TMI ≈ 90 K. The application of external pressure suppresses the Mott transition and restores the metallic electronic structure of the triclinic phase. The observed quantum oscillations of the magnetoresistance are in good agreement with the calculated Fermi surface for the triclinic phase, providing a plausible explanation for the puzzling behavior of κ-(BEDT-TTF)2Hg(SCN)2Br as a function of temperature and pressure around 100 K. The present study points out interesting differences in the structural and physical behaviors of the two room temperature isostructural salts of κ-(BEDT-TTF)2Hg(SCN)2X with X = Br, Cl.The work at the Federal Research Center of Problems of Chemical Physics and Medicinal Chemistry was carried out within the project of state assignment number AAAA-A19-119092390079-8. V.N.Z. acknowledges the support of the Russian Foundation for Basic Research No. 21-52-12027. The work in Spain was supported by the MICIU (Grant PGC2018-096955-B-C44) and Generalitat de Catalunya (2017SGR1506). E.C. acknowledges the support of the Spanish MICIU through the Severo Ochoa FUNFUTURE (CEX2019-000917-S) Excellence Center distinction.With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).Peer reviewe