The generalization of the Local Density Approximation (LDA) method for the systems with strong Coulomb correlations is presented which gives a correct description of the Mott insulators. The LDA+U method is based on the model hamiltonian approach and allows to take into account the non-sphericity of the Coulomb and exchange interactions. parameters. Orbital-dependent LDA+U potential gives correct orbital polarization and corresponding Jahn-Teller distortion. To calculate the spectra of the strongly correlated systems the impurity Anderson model should be solved with a many-electron trial wave function. All parameters of the many-electron hamiltonian are taken from LDA+U calculations. The method was applied to NiO and has shown good agreement with experimental photoemission spectra and with the oxygen Kα X-ray emission spectrum.

https://iopscience.iop.org/article/10.1088/0953-8984/9/4/002/pdf

First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA+ U method

The Interaction of Water with Solid Surfaces: Fundamental Aspects Revisited

The magnetic properties of many magnetic materials can be controlled by external stimuli. The principal focus here is on the thermal, photochemical, electrochemical, and chemical control of phase transitions that involve changes in magnetization. The molecular compounds described herein range from metal complexes, through pure organic compounds to composite materials. Most of the Review is devoted to the properties of valence-tautomeric compounds, molecular magnets, and spin-crossover complexes, which could find future application in memory devices or optical switches.

Control of magnetic properties through external stimuli.

A2B′B″O6 perovskites: A review

Magnetocapacitance and Magnetoresistance Near Room Temperature in a Ferromagnetic Semiconductor: La2NiMnO6

Neutron-diffraction measurements have revealed a new anomalous thermal lattice expansion of LaCoO 3 near 500 K that indicates the existence of a second spin-state transition, in addition to the one previously established near 100 K. The anomalous expansion and the temperature dependence of the Co magnetic moments are successfully interpreted in a wide temperature range based on a simple model assuming low-spin (LS, S =0), intermediate-spin (IS, S =1), and high-spin (HS, S =2) states of Co atoms. The first spin transition, near 100 K, is from LS to IS, and the second, near 500 K, is from IS to a mixed state of IS and HS. The fitted model parameters indicate that the initially-large energy difference between IS and HS states decreases towards zero as the second transition proceeds. The large drop in resistivity associated with the latter transition appears to be correlated with the population of the HS state.

Two Spin-State Transitions in LaCoO 3

${\mathrm{LaCoO}}_{3}$ exhibits two magnetic-electronic transitions, one near 90 K and a second near 500 K. A previous study of the paramagnetic scattering using polarized neutrons demonstrated that the low-temperature transition is associated with the thermal excitation of ${\mathrm{Co}}^{3+}$ ions from the low-spin to the high-spin state. In the present work, we extend the paramagnetic-scattering measurements up to a temperature of 700 K. We find that the magnetic-scattering intensity decreases monotonically for temperatures above 300 K, indicating that the high-temperature transition is not dominantly magnetic in origin. Furthermore, the anomalous thermal expansion associated with the low-temperature transition is measured and shown to be consistent with a simple theoretical model for the spin-state transition. For comparison, paramagnetic-scattering measurements for ${\mathrm{La}}_{0.92}$${\mathrm{Sr}}_{0.08}$${\mathrm{CoO}}_{3}$ are also presented. In this material the ferromagnetic correlations are substantially stronger than in the undoped compound, and no transition to the low-spin state is observed. Instead, the paramagnetic scattering increases steadily with decreasing temperature until saturating below 24 K, the same temperature at which the magnetization of the zero-field-cooled specimen shows a sharp cusp. These results suggest that the magnetic moments in the doped compound freeze into a spin-glass state at low temperature.

Neutron-scattering study of the spin-state transition and magnetic correlations in La1-xSrxCoO3 (x=0 and 0.08)

Polarized and unpolarized neutron measurements have been performed on ${\mathrm{LaCoO}}_{3}$ in a temperature range between 10 and 295 K. A drastic decrease in the magnetic cross section is observed below 150 K. This is the first concrete experimental evidence for the temperature-induced magnetic moment of Co ions in this oxide as proposed in the thermally populated high-spin model. The temperature dependence of the moment is in qualitative agreement with that calculated from the magnetic-susceptibility data.

Temperature-induced magnetism in LaCoO 3

The pressure dependence of the 100 K spin-state transition in LaCoO 3 is investigated through magnetization measurement under pressures of up to 18.2 kbar. The energy gap, Δ, between the low-spin ground state and the excited magnetic state (intermediate spin) increases remarkably with increasing pressure. The linear part of the pressure dependence of Δ, which is dominant below 5 kbar, is interpreted consistently by the volume expansion due to the spin-state transition under ambient pressure. In the higher pressure region, a quadratic pressure dependence is dominant, which suggests a very steep volume dependence of the energy of the excited magnetic state under the highly compressed condition.

Pressure Dependence of the 100 K Spin-State Transition in LaCoO3.

Magnetic properties of REMe 0.5 Mn 0.5 O 3 with Me = Ni and Co are investigated for a series of rare earth (RE) elements. In both systems with Me = Ni and Co, the Curie temperature ( T C ), below which the magnetic moments of Me 2+ and Mn 4+ allign ferromagnetically, decreases remarkably as RE goes from La to heavier elements; from 295 K for RE = La to 50 K for Lu with Me = Ni, and from 250 K for La to 95 K for Ho with Me = Co. The decrease of T C is interpreted as due to the bond angle (θ) dependence of the superexchange interactions between Me 2+ and Mn 4+ through O 2- ; T C is roughly linear to cos 2 θ as predicted by a simple theory [C. Boekema et al. : Int. J. Mag. 3 (1972) 341], but a distinct deviation from the linear relation is observed for the late RE elements. The magnetic moments of RE ions appears only in a low temperature region, typically below 30 K. Qualitative discussion on the exchange interactions involving RE is presented.

Kichizo Asai

Papers

Two Spin-State Transitions in LaCoO 3

Neutron-scattering study of the spin-state transition and magnetic correlations in La1-xSrxCoO3 (x=0 and 0.08)

Temperature-induced magnetism in LaCoO 3

Pressure Dependence of the 100 K Spin-State Transition in LaCoO3.

Magnetic properties of REMe0.5Mn0.5O3 (RE = Rare Earth Element, Me = Ni, Co)