Colossal Density-Driven Resistance Response in the Negative Charge Transfer Insulator MnS2

A reversible density driven insulator to metal to insulator transition in high-spin MnS2 is experimentally observed, leading with a colossal electrical resistance drop of 108 Ω by 12 GPa. Density functional theory simulations reveal the metallization to be unexpectedly driven by previously unoccupied S22− σ3p* antibonding states crossing the Fermi level. This is a unique variant of the charge transfer insulator to metal transition for negative charge transfer insulators having anions with an unsaturated valence. By 36 GPa the emergence of the low-spin insulating arsenopyrite (P21/c) is confirmed, and the bulk metallicity is broken with the system returning to an insulative electronic state.Received 9 February 2021Revised 8 April 2021Accepted 4 June 2021DOI:https://doi.org/10.1103/PhysRevLett.127.016401© 2021 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasElectrical conductivityElectronic structurePhase diagramsPhysical SystemsMott insulatorsTechniquesCrystallographyDensity functional theoryRaman spectroscopyCondensed Matter, Materials & Applied Physics