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.

http://absimage.aps.org/image/MAR06/MWS_MAR06-2005-007233.pdf

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

The projection of the eigenfunctions obtained in standard plane-wave first-principle electronic-structure calculations into atomic-orbital basis sets is proposed as a formal and practical link between the methods based on plane waves and the ones based on atomic orbitals. Given a candidate atomic basis, ({\it i}) its quality is evaluated by its projection into the plane-wave eigenfunctions, ({\it ii}) it is optimized by maximizing that projection, ({\it iii}) the associated tight-binding Hamiltonian and energy bands are obtained, and ({\it iv}) population analysis is performed in a natural way. The proposed method replaces the traditional trial-and-error procedures of finding appropriate atomic bases and the fitting of bands to obtain tight-binding Hamiltonians. Test calculations of some zincblende semiconductors are presented.

https://arxiv.org/pdf/cond-mat/9505075.pdf

Projection of plane-wave calculations into atomic orbitals

Arsenic, selenium, boron, lead, cadmium, copper, and zinc in naturally contaminated rocks: A review of their sources, modes of enrichment, mechanisms of release, and mitigation strategies.

Review on manganese dioxide for catalytic oxidation of airborne formaldehyde

The efficient conversion of solar energy by means of photocatalysis shows huge potential to relieve the ongoing energy crisis and increasing environmental pollution. However, unsatisfactory conversion efficiency still hinders its practical application. The introduction of external fields can remarkably enhance the photocatalytic performance of semiconductors from the inside out. This review focuses on recent advances in the application of diverse external fields, including microwaves, mechanical stress, temperature gradient, electric field, magnetic field, and coupled fields, to boost photocatalytic reactions, for applications in, for example, contaminant degradation, water splitting, CO2 reduction, and bacterial inactivation. The relevant reinforcement mechanisms of photoabsorption, the transport and separation of photoinduced charges, and adsorption of reagents by the external fields are highlighted. Finally, the challenges and outlook for the development of external-field-enhanced photocatalysis are presented.

Photocatalysis Enhanced by External Fields.

DFT study of interactions between calcium hydroxyl ions and pyrite, marcasite, pyrrhotite surfaces

DFT study on the electronic structure and optical properties of N, Al, and N-Al doped graphene

DFT study on the galvanic interaction between pyrite (100) and galena (100) surfaces

A density functional based tight binding (DFTB+) study on the sulfidization-amine flotation mechanism of smithsonite

Pyrite is the most common sulfide in nature, and it is well-known for its roles in acid mine drainage, flotation separation of useful metal (Cu, Pb, Zn, and Mo) sulfide minerals, optoelectronic and photovoltaic application, pneumoconiosis, and even in the origin of life. However, the detailed oxidation behaviors of pyrite are still unclear and not well-understood. New oxidation pathways by O2 on the pyrite (100) surface have been found in this work for the first time using density functional theory simulation; that is, besides Fe sites, S sites are also possible oxidation sites in the initial oxidation state of pyrite, where easier and stronger oxidation may occur. This is the first time to confirm the other researchers' conjecture on the direct oxidation of S sites, which explains the isotopic composition experiments that a minor amount of O2 is permanently incorporated into SO42- during pyrite oxidation (O in SO42- is mainly derived from water). We constructed various H2O-O2 coadsorption models on the pyrite surface by considering the adsorption sequence of H2O and O2. It is found that the H2O molecule undergoes step-wise dissociation in the presence of the O2 molecule. Hydroxyl radical •OH is the reactive oxygen species during H2O dissociation. Cyclic voltammetric measurements confirm the presence of •OH. In addition, H2O2 may also be formed on the surface in terms of H2O-then-O2 sequence adsorption.

Cuihua Zhao

Papers

DFT study of interactions between calcium hydroxyl ions and pyrite, marcasite, pyrrhotite surfaces

DFT study on the electronic structure and optical properties of N, Al, and N-Al doped graphene

DFT study on the galvanic interaction between pyrite (100) and galena (100) surfaces

A density functional based tight binding (DFTB+) study on the sulfidization-amine flotation mechanism of smithsonite

Interactions of Oxygen and Water Molecules with Pyrite Surface: A New Insight