Advances and challenges in DFT-based energy materials design

Abstract

The growing worldwide energy needs call for developing novel materials for energy applications. Ab initio density functional theory (DFT) calculations allow the understanding and prediction of material properties at the atomic scale, thus, play an important role on the energy materials design. Due to the fast progress of computer power and development of calculation methodologies, DFT-based calculations have greatly improved its predictive power, and are now leading to a paradigm shift towards theory-driven materials design. The aim of this perspective is to introduce the advances in DFT calculations which accelerate energy materials design. We first present state-of-the-art DFT methods for accurate simulation of various key properties of energy materials. Then we show examples of how these advances lead to the discovery of new energy materials for photovoltaic, photocatalytic, thermoelectric, and battery applications. The challenges and future research directions in computational design of energy materials are highlighted at the end.

Defect modeling and control in structurally and compositionally complex materials

“…In recent years, there has been remarkable progress in improving the accuracy of first-principles calculations. For instance, more accurate exchange-correlation functionals and many-body GW approaches have been developed to allow computation of accurate total energy and electronic structure 63 .…”

Critical Role of Configurational Disorder in Stabilizing Chemically Unfavorable Coordination in Complex Compounds

“…The electronic structure and material properties of a compound are determined by its composition, crystal structure, and atomic arrangement. Typically, the chemical bonding of the constituting elements in a crystal determines the coordination preference. – Some criteria, for example, Pauling’s rule and electronegativity, have been established to rationalize the experimentally observed correlation between elemental chemistry and coordination for numerous compounds. , These two criteria can be used to estimate the bonding environment and provide a general trend. For instance, the IB-IIIA-VIA 2 ternary compounds, such as AgGaSe 2 , adopt a tetrahedrally coordinated structure (TCS) because of their covalent nature. ,, In contrast, IA-VA-VIA 2 compounds, such as NaBiS 2 , favor an octahedrally coordinated structure (OCS) because of their more ionic nature and suitable ionic radii. , Therefore, for IB-VA-VIA 2 compounds, such as AgBiS 2 , with intermediate ionicity or covalency, one may expect that they prefer a mix-coordinated structure (MCS) consisting of covalent AgS 4 tetrahedra and ionic BiS 6 octahedra.…”

Profiling Electronic and Phononic Band Structures of Semiconductors at Finite Temperatures: Methods and Applications

“…[1][2][3][4][5][6][7][8][9][10] Understanding the properties of semiconductors and the sophisticated microscopic processes and mechanisms that enable the excellent properties are thus at the core of modern semiconductors research. [2,[11][12][13][14][15][16][17] Among the basic properties of semiconductors, their electronic and phononic band structures are of key interest, since various functional properties such as optical absorption and emission, charge and heat transport coefficients, carrier recombination, and thermodynamic free energies can be derived from the basic band structures.…”