Total Cluster Energy Calculation of Lithium Ion Conductors by the DV-Xα Method

Recently several programs for the total cluster energy calculation have been developing in the DV-Xα method. In this study, we have tried to calculate and compare total cluster energies of several diatomic molecules and model clusters of ionic conductors. The total cluster energies of diatomic molecules have minimum near the equilibrium atomic distance of each molecules though the absolute value of the total cluster energy were slightly different each other. In the case of the model cluster of the Li3N crystal, which is one of the typical Li ion conductors, we have obtained the energy change as a function of the site during the movement of a Li ion. The energy change with the movement of the Li ion along the conduction path was considerably smaller than along other paths, consistent with the results by the band calculation and experiments. The total cluster energy calculation method was enough useful for the discussion of the cluster energy

Formation of superconducting yttrium barium copper oxide using sulphur-containing templates

The formation of yttrium barium copper oxide (YBCO) via biotemplated routes is often plagued by unwanted stable intermediates, some of which arise from the template itself. Here we describe a method which allows sulphur-containing templates, such as proteins, to form superconducting YBCO which would have hitherto resulted in non-superconducting sulphated phases

Dimensionality dependence of optical nonlinearity and relaxation dynamics in cuprates

Femtosecond pump-probe measurements find pronounced dimensionality dependence of the optical nonlinearity in cuprates. Although the coherent two-photon absorption (TPA) and linear absorption bands nearly overlap in both quasi-one and two-dimensional (1D and 2D) cuprates, the TPA coefficient is one order of magnitude smaller in 2D than in 1D. Furthermore, picosecond recovery of optical transparency is observed in 1D cuprates, while the recovery in 2D involves relaxation channels with a time scales of tens of picoseconds. The experimental results are interpreted within the two-band extended Hubbard model.Comment: 10 pages, 4 figure

Nonlinear Optical Response in two-dimensional Mott Insulators

We study the third-order nonlinear optical susceptibility $\chi^{(3)}$ and photoexcited states of two-dimensional (2D) Mott insulators by using an effective model in the strong-coupling limit of a half-filled Hubbard model. In the numerically exact diagonalization calculations on finite-size clusters, we find that the coupling of charge and spin degrees of freedom plays a crucial role in the distribution of the dipole-allowed states with odd parity and the dipole-forbidden states with even parity in the photoexcited states. This is in contrast with the photoexcited states in one dimension, where the charge and spin degrees of freedom are decoupled. In the third-harmonic generation (THG) spectrum, main contribution is found to come from the process of three-photon resonance associated with the odd-parity states. As a result, the two-photon resonance process is less pronounced in the THG spectrum. The calculated THG spectrum is compared with recent experimental data. We also find that $\chi^{(3)}$ with cross-polarized configuration of pump and probe photons shows spectral distributions similar to $\chi^{(3)}$ with co-polarized configuration, although the weight is small. These findings will help the analyses of the experimental data of $\chi^{(3)}$ in the 2D Mott insulators.Comment: 9 pages,5 figures,RevTeX

Ultrafast photoinduced reflectivity transients in (Nd0.5Sr0.5)MnO3(Nd_{0.5}Sr_{0.5})MnO_3

The temperature dependence of ultrafast photoinduced reflectivity transients is reported in Nd$_{0.5}$Sr$_{0.5}$MnO$_{3}$ thin film. The photoinduced reflectivity shows a complex response with very different temperature dependences on different timescales. The response on the sub-ps timescale appears to be only weakly sensitive to the 270K-metal-insulator phase transition. Below $\sim 160$ K the sub-ps response displays a two component behavior indicating inhomogeneity of the film resulting from the substrate induced strain. On the other hand, the slower response on the 10-100 ps timescale is sensitive only to the metal-insulator phase transition and is in agreement with some previously published results. The difference in the temperature dependences of the responses on nanosecond and $\mu$s timescales indicates that thermal equilibrium between the different degrees of fredom is established relatively slowly - on a nanosecond timescale

Ultrafast optical nonlinearity in quasi-one-dimensional Mott-insulator Sr2CuO3{\rm Sr_2CuO_3}

We report strong instantaneous photoinduced absorption (PA) in the quasi-one-dimensional Mott insulator ${\rm Sr_2CuO_3}$ in the IR spectral region. The observed PA is to an even-parity two-photon state that occurs immediately above the absorption edge. Theoretical calculations based on a two-band extended Hubbard model explains the experimental features and indicates that the strong two-photon absorption is due to a very large dipole-coupling between nearly degenerate one- and two-photon states. Room temperature picosecond recovery of the optical transparency suggests the strong potential of ${\rm Sr_2CuO_3}$ for all-optical switching.Comment: 10 pages, 4 figure

Nuclei beyond the drip line

In a Thomas-Fermi model, calculations are presented for nuclei beyond the nuclear drip line at zero temperature. These nuclei are in equilibrium by the presence of an external gas, as may be envisaged in the astrophysical scenario. We find that there is a limiting asymmetry beyond which these nuclei can no longer be made stable.Comment: Physical Review C (in press), 1 ReVteX file for text, 4 PS-files for figure

Exchange Interaction in Binuclear Complexes with Rare Earth and Copper Ions: A Many-Body Model Study

We have used a many-body model Hamiltonian to study the nature of the magnetic ground state of hetero-binuclear complexes involving rare-earth and copper ions. We have taken into account all diagonal repulsions involving the rare-earth 4f and 5d orbitals and the copper 3d orbital. Besides, we have included direct exchange interaction, crystal field splitting of the rare-earth atomic levels and spin-orbit interaction in the 4f orbitals. We have identified the inter-orbital $4f$ repulsion, U$_{ff}$ and crystal field parameter, $\Delta_f$ as the key parameters involved in controlling the type of exchange interaction between the rare earth $4f$ and copper 3d spins. We have explored the nature of the ground state in the parameter space of U$_{ff}$, $\Delta_f$, spin-orbit interaction strength $\lambda$ and the $4f$ filling n$_f$. We find that these systems show low-spin or high-spin ground state depending on the filling of the $4f$ levels of the rare-earth ion and ground state spin is critically dependent on U$_{ff}$ and $\Delta_f$. In case of half-filling (Gd(III)) we find a reentrant low-spin state as U$_{ff}$ is increased, for small values of $\Delta_f$, which explains the recently reported apparent anomalous anti-ferromagnetic behaviour of Gd(III)-radical complexes. By varying U$_{ff}$ we also observe a switch over in the ground state spin for other fillings . We have introduced a spin-orbit coupling scheme which goes beyond L-S or j-j coupling scheme and we find that spin-orbit coupling does not significantly alter the basic picture.Comment: 22 pages, 11 ps figure

Nonlinear Optical Response Functions of Mott Insulators Based on Dynamical Mean Field Approximation

We investigate the nonlinear optical susceptibilities of Mott insulators with the dynamical mean field approximation. The two-photon absorption (TPA) and the third-harmonic generation (THG) spectra are calculated, and the classification by the types of coupling to external fields shows different behavior from conventional semiconductors. The direct transition terms are predominant both in the TPA and THG spectra, and the importance of taking all types of interaction with the external field into account is illustrated in connection with the THG spectrum and dcKerr effect. The dependence of the TPA and THG spectra on the Coulomb interaction indicate a scaling relation. We apply this relation to the quantitative evaluation and obtain results comparable to those of experiments.Comment: 14 pages, 12 figure