Computational chemistry’s rocky revolution

Density functional theory (DFT), which provides a simplified quantum mechanical approach to studying electronic structure for atoms, molecules and materials, is the cornerstone of modern computational chemistry. Yet despite its ubiquity in chemistry today, DFT faced a rocky road to acceptance.

Modern DFT was first formulated in the 1960s and was quickly adopted by condensed matter physicists. But early limitations to computational accuracy dissuaded many chemists from considering its potential.

Nordholm et al. provide a look back at how DFT came to be widely accepted in chemistry through a summary of the 2024 Royal Swedish Academy of Sciences symposium on the topic. The paper, which combines personal perspectives of symposium attendees, provides first-hand accounts of how scientists became introduced to DFT over the years.

“I hope that the paper can show how the DFT revolution of computational chemistry came about, from original ideas … to ingenious practical implementations that now dominate calculations, particularly for larger molecules,” said author Sture Nordholm. “I think we have revealed both the scientific breakthroughs and the scientists behind this hugely important development of computational chemistry and physics.”

In addition to discussing the history of DFT, the paper honors late chemist Axel Becke, who played a key role in showing DFT could be both accurate and efficient. Though the advances of DFT are generally credited to Walter Kohn and John Pople, who were awarded the 1998 Nobel Prize in chemistry for their contributions to the theory, the paper acknowledges others like Becke and John Perdew as equally important contributors.

Source: “The rocky path of DFT into chemistry – Discussions at a symposium and reflections on a circular journey in honor of Axel Becke 1953 – 2025,” by Sture Nordholm, Evert Jan Baerends, Kieron Burke, Peter Gill, Paola Gori-Giorgi, Stefan Grimme, Martin Head-Gordon, Trygve Helgaker, Erin Johnson, Robert O. Jones, John Perdew, Dennis Salahub, Andreas Savin, Gustavo Scuseria, David J. Tozer, Weitao Yang, Russell J. Boyd, and Henry F. Schaefer III, Journal of Chemical Physics (2026). The article can be accessed at https://doi.org/10.1063/5.0337560 .

This paper is part of the Electron Densities: From Algorithms and Functionals to Molecular Modelling and Chemical Insights Collection, learn more here .