LDA+DMFT computation of the electronic spectrum of NiO

The electronic spectrum, energy gap and local magnetic moment of paramagnetic NiO are computed by using the local density approximation plus dynamical mean-field theory (LDA+DMFT). To this end the noninteracting Hamiltonian obtained within the local density approximation (LDA) is expressed in Wannier functions basis, with only the five anti-bonding bands with mainly Ni 3d character taken into account. Complementing it by local Coulomb interactions one arrives at a material-specific many-body Hamiltonian which is solved by DMFT together with quantum Monte-Carlo (QMC) simulations. The large insulating gap in NiO is found to be a result of the strong electronic correlations in the paramagnetic state. In the vicinity of the gap region, the shape of the electronic spectrum calculated in this way is in good agreement with the experimental x-ray-photoemission and bremsstrahlung-isochromat-spectroscopy results of Sawatzky and Allen. The value of the local magnetic moment computed in the paramagnetic phase (PM) agrees well with that measured in the antiferromagnetic (AFM) phase. Our results for the electronic spectrum and the local magnetic moment in the PM phase are in accordance with the experimental finding that AFM long-range order has no significant influence on the electronic structure of NiO.Comment: 15 pages, 6 figures, 1 table; published versio

Heterometallic perovskite-type metal-organic framework with an ammonium cation: structure, phonons, and optical response of [NH4]Na0.5CrxAl0.5-x(HCOO)3 (x = 0, 0.025 and 0.5).

We report the synthesis, crystal structure, vibrational and luminescence properties of two heterometallic perovskite-type metal-organic frameworks (MOFs) containing the ammonium cation (NH4+, Am+): [NH4][Na0.5Cr0.5(HCOO)3] (AmNaCr) and [NH4][Na0.5Al0.475Cr0.025(HCOO)3] (AmNaAlCr) in comparison to the previously reported [NH4][Na0.5Al0.5(HCOO)3] (AmNaAl). The room-temperature crystal structure of AmNaCr and AmNaAlCr was determined to be R3[combining macron]. The hydrogen bonding (HB) energy calculated using density functional theory (DFT) agrees well with experimental data, and confirms the existence of almost identical H-bonding in AmNaCr and AmNaAl, with three short hydrogen bonds and a longer trifurcated H-bond. Temperature-dependent Raman measurements supported by differential scanning calorimetry show that AmNaCr does not undergo any structural phase transitions in the 80-400 K temperature range. The high-pressure Raman spectra of AmNaCr show the onset of two structural instabilities near 0.5 and 1.5 GPa. The first instability involves weak distortion of the framework, while the second leads to irreversible amorphization of the sample. High-pressure DFT simulations show that the unit cell of the AmNaCr compound contracts along the c axis, which leads to a shortening of the trifurcated H-bond. The optical properties show that both studied crystals exhibit Cr3+-based emission characteristic of intermediate ligand field strength

Similarities between the Hubbard and Periodic Anderson Models at Finite Temperatures

The single band Hubbard and the two band Periodic Anderson Hamiltonians have traditionally been applied to rather different physical problems - the Mott transition and itinerant magnetism, and Kondo singlet formation and scattering off localized magnetic states, respectively. In this paper, we compare the magnetic and charge correlations, and spectral functions, of the two systems. We show quantitatively that they exhibit remarkably similar behavior, including a nearly identical topology of the finite temperature phase diagrams at half-filling. We address potential implications of this for theories of the rare earth ``volume collapse'' transition.Comment: 4 pages (RevTeX) including 4 figures in 7 eps files; as to appear in Phys. Rev. Let

A self-interaction corrected pseudopotential scheme for magnetic and strongly-correlated systems

Local-spin-density functional calculations may be affected by severe errors when applied to the study of magnetic and strongly-correlated materials. Some of these faults can be traced back to the presence of the spurious self-interaction in the density functional. Since the application of a fully self-consistent self-interaction correction is highly demanding even for moderately large systems, we pursue a strategy of approximating the self-interaction corrected potential with a non-local, pseudopotential-like projector, first generated within the isolated atom and then updated during the self-consistent cycle in the crystal. This scheme, whose implementation is totally uncomplicated and particularly suited for the pseudopotental formalism, dramatically improves the LSDA results for a variety of compounds with a minimal increase of computing cost.Comment: 18 pages, 14 figure

Exact solution of a linear molecular motor model driven by two-step fluctuations and subject to protein friction

We investigate by analytical means the stochastic equations of motion of a linear molecular motor model based on the concept of protein friction. Solving the coupled Langevin equations originally proposed by Mogilner et al. (A. Mogilner et al., Phys. Lett. {\bf 237}, 297 (1998)), and averaging over both the two-step internal conformational fluctuations and the thermal noise, we present explicit, analytical expressions for the average motion and the velocity-force relationship. Our results allow for a direct interpretation of details of this motor model which are not readily accessible from numerical solutions. In particular, we find that the model is able to predict physiologically reasonable values for the load-free motor velocity and the motor mobility.Comment: 12 pages revtex, 6 eps-figure

Pressure Induced Charge Disproportionation in LaMnO3_{3}

We present a total energy study as a function of volume in the cubic phase of LaMnO$_{3}$. A charge disproportionated state into planes of Mn$^{3+}$O$_{2}$/Mn$^{4+}$O$_{2}$ was found. It is argued that the pressure driven localisation/delocalisation transition might go smoothly through a region of Mn$^{3+}$ and Mn$^{4+}$ coexistence.Comment: 3 pages, 1 figure, Conference Proceedings: Nanospintronics: Design and Realization (Kyoto, Japan 24-28 May, 2004

The Cerium volume collapse: Results from the LDA+DMFT approach

The merger of density-functional theory in the local density approximation (LDA) and many-body dynamical mean field theory (DMFT) allows for an ab initio calculation of Ce including the inherent 4f electronic correlations. We solve the DMFT equations by the quantum Monte Carlo (QMC) technique and calculate the Ce energy, spectrum, and double occupancy as a function of volume. At low temperatures, the correlation energy exhibits an anomalous region of negative curvature which drives the system towards a thermodynamic instability, i.e., the $\gamma$-to-$\alpha$ volume collapse, consistent with experiment. The connection of the energetic with the spectral evolution shows that the physical origin of the energy anomaly and, thus, the volume collapse is the appearance of a quasiparticle resonance in the 4f-spectrum which is accompanied by a rapid growth in the double occupancy.Comment: 4 pages, 3 figure