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A single-component molecular crystal [Pd(dddt)2] has been shown to exhibit almost temperature-independent resistivity under high pressure, leading theoretical studies to propose it as a three-dimensional (3D) Dirac electron system. To obtain more experimental information about the high-pressure electronic states, detailed resistivity measurements were performed, which show temperature-independent behavior at 13 GPa and then an upturn in the low temperature region at higher pressures. High-pressure single-crystal structure analysis was also performed for the first time, revealing the presence of pressure-induced structural disorder, which is possibly related to the changes in resistivity in the higher-pressure region. Calculations based on the disordered structure reveal that the Dirac cone state and semiconducting state coexist, indicating that the electronic state at high pressure is not a simple Dirac electron system as previously believed. Finally, the first measurements of magnetoresistance on [Pd(dddt)2] under high pressure are reported, revealing unusual behavior that seems to originate from the Dirac electron state.

crystals

High-Pressure Crystal Structure and Unusual Magnetoresistance of a Single-Component Molecular Conductor [Pd(dddt)2] (dddt = 5,6-dihydro-1,4-dithiin-2,3-dithiolate)