Mott transition and suppression of orbital fluctuations in orthorhombic 3d1 perovskites.

INFM and Dipartimento di Fisica A. Volta, Università di Pavia, Via Bassi 6, I-27100 Pavia, Italy.
Physical Review Letters (Impact Factor: 7.73). 05/2004; 92(17):176403. DOI: 10.1103/PhysRevLett.92.176403
Source: PubMed

ABSTRACT Using t(2g) Wannier functions, a low-energy Hamiltonian is derived for orthorhombic 3d(1) transition-metal oxides. Electronic correlations are treated with a new implementation of dynamical mean-field theory for noncubic systems. Good agreement with photoemission data is obtained. The interplay of correlation effects and cation covalency (GdFeO3-type distortions) is found to suppress orbital fluctuations in LaTiO3 and even more in YTiO3, and to favor the transition to the insulating state.

  • [Show abstract] [Hide abstract]
    ABSTRACT: In the Mott-Hubbard insulators YTiO3 and SmTiO3 we study optical excitations from the lower to the upper Hubbard band, d^1d^1 -> d^0d^2. The multi-peak structure observed in the optical conductivity reflects the multiplet structure of the upper Hubbard band in a multi-orbital system. Absorption bands at 2.55 and 4.15 eV in the ferromagnet YTiO3 correspond to final states with a triplet d^2 configuration, whereas a peak at 3.7 eV in the antiferromagnet SmTiO3 is attributed to a singlet d^2 final state. A strongly temperature-dependent peak at 1.95 eV in YTiO3 and 1.8 eV in SmTiO3 is interpreted in terms of a Hubbard exciton, i.e., a charge-neutral (quasi-)bound state of a hole in the lower Hubbard band and a double occupancy in the upper one. The binding to such a Hubbard exciton may arise both due to Coulomb attraction between nearest-neighbor sites and due to a lowering of the kinetic energy in a system with magnetic and/or orbital correlations. Furthermore, we observe anomalies of the spectral weight in the vicinity of the magnetic ordering transitions, both in YTiO3 and SmTiO3. In the G-type antiferromagnet SmTiO3, the sign of the change of the spectral weight at T_N depends on the polarization. This demonstrates that the temperature dependence of the spectral weight is not dominated by the spin-spin correlations, but rather reflects small changes of the orbital occupation.
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: We introduce a novel computational approach for the investigation of complex correlated electron materials which makes it possible to evaluate interatomic forces and, thereby, determine atomic displacements and structural transformations induced by electronic correlations. It combines ab initio band structure and dynamical mean-field theory and is implemented with the linear-response formalism regarding atomic displacements. We apply this new technique to explore structural transitions of prototypical correlated systems such as elemental hydrogen, SrVO3, and KCuF3.
    Physical Review Letters 04/2014; 112(14):146401. · 7.73 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: Materials with strong electronic Coulomb correlations play an increasing role in modern materials applications. “Thermochromic” systems, which exhibit thermally induced changes in their optical response, provide a particularly interesting case. The optical switching associated with the metal–insulator transition of vanadium dioxide (VO2), for example, has been proposed for use in numerous applications, ranging from anti-laser shields to “intelligent” windows, which selectively filter radiative heat in hot weather conditions. Are present-day electronic structure techniques able to describe, or – eventually even predict – such a kind of behavior? How far are we from materials design using correlated oxides? These are the central questions we try to address in this article. We review recent attempts of calculating optical properties of correlated materials within dynamical mean field theory, and summarize results for VO2 obtained within a novel scheme aiming at particularly simple and efficient calculations of optical transition matrix elements within localized basis sets. Finally, by optimizing the geometry of “intelligent windows,” we argue that this kind of technique can, in principle, be used to provide guidance for experiments, thus giving a rather optimistic answer to the above questions.
    physica status solidi (b) 09/2009; 246(9). · 1.49 Impact Factor

Full-text (2 Sources)

Available from
May 23, 2014