Stability of correlated insulating states in molecular conductors from first-principles calculation

Abstract

Electronic properties of molecular conductors exhibiting antiferromagnetic (AFM) spin order and charge order (CO) owing to electron correlation are studied using first-principles density functional theory calculations. We investigate two systems, a quasi-two-dimensional Mott insulator ${\beta }^{\prime }$-(BEDT-TTF)${}_2$ICl${}_2$ with an AFM ground state, and several members of quasi-one-dimensional (TMTTF)${}_2$$X$ showing CO. The stabilities of the AFM and CO states are compared between the use of a standard exchange-correlation functional based on the generalized gradient approximation and that of a range-separated hybrid functional; we find that the latter describes these states better. For ${\beta }^{\prime }$-(BEDT-TTF)${}_2$ICl${}_2$, the AFM order is much stabilized with a wider band gap. For (TMTTF)${}_2$$X$, only by using the hybrid functional, the AFM insulating state is realized and the CO states coexisting with AFM order are stable under structural optimization, whose stability among different \textit{X} shows the tendency consistent with experiments.

References in corpus (22)

• Spin current generation in organic antiferromagnets
• Charge Ordering in Organic ET Compounds
• Quantum frustration in organic Mott insulators: from spin liquids to unconventional superconductors
• Charge ordering in the TMTTF family of molecular conductors
• The ferroelectric Mott-Hubbard phase of organic (TMTTF)2X conductors
• Antiferromagnetic Phases of One-Dimensional Quarter-Filled Organic Conductors
• Ab initio Derivation of Low-Energy Model for $\kappa$-ET Type Organic Conductors
• Theoretical Aspects of Charge Ordering in Molecular Conductors
• Anomalous Hall effect in $\kappa$-type organic antiferromagnets
• Competition and coexistence of bond and charge orders in (TMTTF)2AsF6
• Electron-lattice coupling and the broken symmetries of the molecular salt (TMTTF)${}_2$SbF${}_6$
• Coexistence of Charge Order and Spin-Peierls Lattice Distortion in One-Dimensional Organic Conductors
• From charge- and spin-ordering to superconductivity in the organic charge-transfer solids
• Tuning the magnetic dimensionality by charge ordering in the molecular TMTTF salts
• Electronic properties of Fabre charge-transfer salts under various temperature and pressure conditions
• Finite-Temperature Phase Diagram of Quasi-One-Dimensional Molecular Conductors: Quantum Monte Carlo Study
• Origin of the Superconductivity in β'-(BEDT-TTF)_2ICl_2 under High Pressure and β-(BEDT-TTF)_2X at Ambient Pressure
• Temperature-driven transition from the Wigner Crystal to the Bond-Charge-Density Wave in the Quasi-One-Dimensional Quarter-Filled band
• Emergence of charge degrees of freedom under high pressure in an organic dimer-Mott insulator ${\beta }^{\prime }$-(BEDT-TTF)${}_2$ICl${}_2$
• Phase Diagram of ${\beta }^{\prime }$-(BEDT-TTF)${}_2$ICl${}_2$ under High Pressure Based on the First-Principles Electronic Structure
• Comprehensive $ab$ $initio$ investigation of the phase diagram of quasi-one-dimensional molecular solids
• First-principles study of the charge ordered phase in $\kappa$-D${}_3$(Cat-EDT-TTF/ST)${}_2$: Stability of $\pi$-electron deuterium coupled ordering in hydrogen-bonded molecular conductors