Density functional theory: Its origins, rise to prominence, and future

Abstract

In little more than 20 years, the number of applications of the density functional (DF) formalism in chemistry and materials science has grown in an astonishing fashion. The number of publications alone shows that DF calculations make up a huge success story, and many younger colleagues are surprised to learn that the widespread application of density functional methods, particularly in chemistry, began only after 1990. This is indeed unexpected, because the origins are usually traced to the papers of Hohenberg, Kohn, and Sham more than a quarter of a century earlier. The DF formalism, its applications, and prospects were reviewed for this journal in 1989. About the same time, the combination of DF calculations with molecular dynamics promised to provide an efficient way to study structures and reactions in molecules and extended systems. This paper reviews the development of density-related methods back to the early years of quantum mechanics and follows the breakthrough in their application after 1990. The two examples from biochemistry and materials science are among the many current applications that were simply far beyond expectations in 1990. The reasons why-50 years after its modern formulation and after two decades of rapid expansionsome of the most cited practitioners in the field are concerned about its future are discussed.

First-principles calculations of thermal, electrical, and thermoelectric transport properties of semiconductors

“…Such information has been difficult to obtain within traditional methods because experiments normally probe transport properties that are averaged over all the carriers, while the theoretical models are intractable without certain approximations thus lack accuracy and in many cases, predictive power. The development of the first-principles computational techniques in recent decades enables one to study materials' physical properties accurately without adjustable parameters [1]. The merit of the first-principles methods lies in that they are easily justifiable and useful for a wide range of problems.…”

Stratified construction of neural network based interatomic models for multicomponent materials

“…Given ionic positions, these basic quantities can be found at different levels of approximation with only partial or no explicit treatment of the electronic degrees of freedom. Striking a good balance between computational cost and approximation accuracy is one of the central goals in methodology development for materials research [1][2][3][4][5][6][7][8][9][10].…”

Diffraction at GaAs/Fe3Si core/shell nanowires: The formation of nanofacets

“…The three constraints jointly place an upper and lower limit on µ Si . DFT [26][27][28][29][30] in the generalized gradient approximation 31 was applied in order to determine the surface energy of low index surfaces using the Vienna Ab Initio Simulation Package (VASP). 32,33 The calculations were performed in a slab geometry using slabs from 12 to 16 Å thick and a vacuum region of 10 Å.…”