Multi-gap absorption in CaCu${}_3$Ti${}_4$O${}_{12}$ and the predictivity of ab initio methods

Abstract

We report the electronic properties of the quadruple perovskite CaCu${}_3$Ti${}_4$O${}_{12}$ as obtained via several density-functional based methods, and propose a new interpretation of optical experiments to the effect that four distinct transitions (centered around 0.7, 1.5, 2.5, and 3.5 eV) contribute to the spectrum. The comparison with experiment is satisfactory, especially after we account for the effects of spin disorder, which does not close the fundamental gap but suppresses the transition intensity. We find that some of the methods we employ tend to overestimate considerably the gaps for standard values of the respective adjustable parameters.

arXiv comment10 pages, 13 figures, 1 table

References in corpus (13)

• A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
• Colossal dielectric constants in transition-metal oxides
• A first-principles study of the structure and lattice dielectric response of CaCu{3}Ti{4}O{12}
• A self-interaction corrected pseudopotential scheme for magnetic and strongly-correlated systems
• Atomic self-interaction correction for molecules and solids
• A variational pseudo-self-interaction correction approach: ab-initio description of correlated oxides and molecules
• Exchange interactions and magnetic phases of transition metal oxides: benchmarking advanced ab initio methods
• Broadband dielectric response of CaCu3Ti4O12: From dc to the electronic transition regime
• Ordering and multiple phase transitions in ultra-thin nickelate superlattices
• Short-range magnetic order and temperature-dependent properties of cupric oxide
• Onset of Magnetic Order in Strongly-Correlated Systems from ab initio Electronic Structure Calculations: Application to Transition Metal Oxides
• Chain metallicity and antiferro-paramagnetism competition in underdoped YBa${}_2$Cu${}_3$O${}_{6+x}$: a first principles description
• Magnetism and unusual Cu valency in quadruple perovskites

Cited by in corpus (1)

• Theoretical and experimental investigation of optical absorption anisotropy in $\beta$-Ga2O3