Subsystem density‐functional theory (update)

Abstract

The past years since the publication of our review on subsystem density‐functional theory (sDFT) (WIREs Comput Mol Sci. 2014, 4:325–362) have witnessed a rapid development and diversification of quantum mechanical fragmentation and embedding approaches related to sDFT and frozen‐density embedding (FDE). In this follow‐up article, we provide an update addressing formal and algorithmic work on sDFT/FDE, novel approximations developed for treating the non‐additive kinetic energy in these DFT/DFT hybrid methods, new areas of application and extensions to properties previously not accessible, projection‐based techniques as an alternative to solely density‐based embedding, progress in wavefunction‐in‐DFT embedding, new fragmentation strategies in the context of DFT which are technically or conceptually similar to sDFT, and the blurring boundary between advanced DFT/MM and approximate DFT/DFT embedding methods.This article is categorized under: Electronic Structure Theory > Density Functional Theory

Toward Modeling the Complexity of the Chemical Mechanism in SERS

“…The requirement for accurate description of the coupled mechanisms and the detailed local environments poses significant challenges to computational models. To overcome these challenges, the development of faster quantum mechanical methods, , quantum embedding methods − and machine learning models − are likely to be important future directions. We expect that the next generation computational toolbox will enable a more complete description of the enhancement mechanisms necessary to elucidate the full physical contents of SERS.…”

Unraveling the Hydration Shell Structure and Dynamics of Group 10 Aqua Ions

“…For more information on sDFT, we refer the reader to several reviews. 34,35,46,47 Particularly important in this work is the use of adaptive sDFT dynamics. That is, the AIMDs are run with a fluctuating number of subsystems.…”

“…The nonadditive term, E nad [{ρ I , v ext I }], is approximated by computationally advantageous expressions based on orbital-free DFT. For more information on sDFT, we refer the reader to several reviews. ,,, …”

Nonadiabatic molecular dynamics with subsystem density functional theory: application to crystalline pentacene

“…In this work, we explore yet another possibility of using the reduced-scaling electronic structure methods, namely the subsystem DFT (sDFT) [128], for modeling NA-MD in extended periodic systems. We rely on the sDFT implementation [129][130][131][132] within the embedded Quantum Espresso (eQE) package [128]. Recently, sDFT has been successfully employed for studying a range of phenomena and time/length scales, such as the structure of molecular liquids [133,134], solvation [135,136], spin systems [137], large biosystems [138][139][140] and an array of phenomena involving excited electronic states [141,142].…”

“…Recently, sDFT has been successfully employed for studying a range of phenomena and time/length scales, such as the structure of molecular liquids [133,134], solvation [135,136], spin systems [137], large biosystems [138][139][140] and an array of phenomena involving excited electronic states [141,142]. For a more extensive overview of the prospects of using sDFT in various kinds of applications, we refer the reader to the excellent reviews on the topic by Jacob and Neugebauer [129,132]. Despite the wide use of sDFT in more traditional electronic structure calculations, including in excited states calculations [140,143,144], sDFT is yet to unleash its full potential in the NA-MD simulations.…”