Advances in correlated electronic structure methods for solids, surfaces, and nanostructures

Huang, Patrick (Lawrence Livermore National Laboratory); Carter, Emily A.

Source: Annual Review of Physical Chemistry, v 59, 2008, p 261-290

Publisher: Annual Reviews Inc. 

Abstract: Calculations of the electronic structure of solids began decades ago, but only recently have solid-state quantum techniques become sufficiently reliable that their application is nearly as routine as quantum chemistry is for molecules. We aim to introduce chemists to the pros and cons of first-principles methods that can provide atomic-scale insight into the properties and chemistry of bulk materials, interfaces, and nanostructures. The techniques we review include the ubiquitous density functional theory (DFT), which is often sufficient, especially for metals; extensions such as DFT + U and hybrid DFT, which incorporate exact exchange to rid DFT of its spurious self-interactions (critical for some semiconductors and strongly correlated materials); many-body Green's function (GWand BetheSalpeter) methods for excited states; quantum Monte Carlo, in principle an exact theory but for which forces (hence structure optimization and dynamics) are problematic; and embedding theories that locally refine the quantum treatment to improve accuracy. Copyright © 2008 by Annual Reviews. All rights reserved. (166 refs.)

terms: Nanostructures - Density functional theory - Electronic structure - Excited states - Monte Carlo methods - Quantum chemistry