DFT Exchange: Sharing Perspectives on the Workhorse of Quantum Chemistry and Materials Science

Teale, Andrew M.; Helgaker, Trygve; Savin, Andreas; Adamo, Carlo; Aradi, Bálint; Arbuznikov, Alexei V.; Ayers, Paul L.; Baerends, Evert Jan; Barone, Vincenzo; Calaminici, Patrizia; Cancès, Éric; Carter, Emily A.; Chattaraj, Pratim Kumar; Chermette, Henry; Ciofini, Ilaria; Crawford, Daniel A.; Proft, Frank De; Dobson, John F.; Draxl, Caludia; Frauenheim, Thomas; Fromager, Emmanuel; Fuentealba, Patricio; Gagliardi, Laura; Galli, Giulia; Gao, Jiali; Geerlings, Pau̧l; Gidopoulous, Nikitas; Gill, Peter M. W.; Gori‐Giorgi, Paola; Görling, Andreas; Gould, Tim; Gritsenko, O. V.; Jensen, Henrik H.; Johnson, Erin R.; Jones, Robert; Kaupp, Martin; Köster, Andreas M.; Kronik, Leeor; Krylov, Anna I.; Kvaal, Simen; Laestadius, Andre; Levy, Mel; Lewin, Mathieu; Liu, Shubin; Loos, Pierre‐François; Maitra, Neepa T.; Neese, Frank; Perdew, John P.; Pernal, Katarzyna; Pernot, Pascal; Piecuch, Piotr; Rebolini, Elisa; Reining, Lucia; Ruzsinszky, Adrienn; Salahub, Dennis R.; Scheffler, Matthias; Schwerdtfeger, Peter; Staroverov, Viktor N.; Sun, Jianwei; Tellgren, Erik I.; Tozer, David J.; Trickey, Sam; Ullrich, Carsten A.; Vela, Alberto García; Vignale, Giovanni; Wesołowski, Tomasz Adam; Xu, Xin; Yang, Weitao

doi:10.26434/chemrxiv-2022-13j2v-v2

Cited by 7 publications

(9 citation statements)

References 140 publications

(149 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…What we have delineated here is, in a way, self-serving, in that we are certain we would be helped by having some answers to the questions posed. Leads to other questions of rigorous nature about DFT and TDDFT may be found in a recent "round-table" paper [57].…”

Section: Discussionmentioning

confidence: 99%

Some Problems in Density Functional Theory

Wrighton¹,

Albavera-Mata²,

Rodriguez³

et al. 2022

Preprint

View full text Add to dashboard Cite

Though calculations based on density functional theory (DFT) are used remarkably widely in chemistry, physics, materials science, and biomolecular research and though the modern form of DFT has been studied for almost 60 years, some mathematical problems remain. For context, we provide an outline of the basic structure of DFT, then pose several questions regarding both its time-independent and time-dependent forms. Progress on any of these would aid in development of better approximate functionals and in interpretation.

show abstract

Section: Discussionmentioning

confidence: 99%

Some Problems in Density Functional Theory

Wrighton¹,

Albavera-Mata²,

Rodriguez³

et al. 2022

Preprint

View full text Add to dashboard Cite

show abstract

“…With an aim of providing large datasets with energy targets from wide variety of methods to help build both these novel molecular ML tasks and ML for reaction networks, we provide multi-level energies of the QM9 molecules and reactions derived from there. Molecular Quantum chemistry community utilizes a wide variety of exchange correlation functional 19 and thus any new ML method need to be tested for predictions across many different XC to prove generalization and universality. Therefore, by providing data for QM9 molecules with a number of DFT functionals and basis set will provide new challenges to ML community to build robust ML methods that can be applied to a variety of methods.…”

Section: Background and Summarymentioning

confidence: 99%

Large dataset of molecular and reaction energies from multi-level quantum chemical methods

Nandi

Vegge

Bhowmik

2022

Preprint

View full text Add to dashboard Cite

Well curated extensive datasets have have helped spur intense molecular machine learning(ML) method development activities over last few years encouraging non-chemists to be part of the effort as well. QM9 dataset is the one of the benchmark database for small molecules with molecular energies based on B3LYP functional. G4MP2 based energies of these molecules were published later. To enable a widely variety of ML tasks with QM9 molecules, in this article, we introduce a new dataset with QM9 molecule energies estimated with 76 different DFT functionals and three different basis sets (228 energy numbers for each molecule). We additionally enumerated all possible A <-> B molecular conversions within the QM9 dataset and provide the reaction energies based on these 76 functionals, and basis sets. Lastly, we also provide the bond changes for all the 162 million reactions with the dataset to enable structure and bond based reaction energy prediction tools based on ML.

show abstract

“…For the off-diagonal terms, we have shown that under special situations such as spin coupling interactions, the transition density functional can be consistently determined using the high-spin energy as a constraint; , the latter can in principle be determined exactly using KS-DFT. It took nearly 30 years before KS-DFT gained a widespread appreciation, and it was another 30 years before a broad understanding of the fundamental theory was achieved, becoming the method of choice today for large molecular systems. Useful approximations to will come for excited states in time.…”

mentioning

confidence: 99%

Multistate Density Functional Theory of Excited States

Gao

2022

J. Phys. Chem. Lett.

Self Cite

111

View full text Add to dashboard Cite

We report a rigorous formulation of density functional theory for excited states, providing a theoretical foundation for a multistate density functional theory. We prove the existence of a Hamiltonian matrix functional of the multistate matrix density D(r) in the subspace spanned by the lowest N eigenstates. Here, D(r) is an N-dimensional matrix of state densities and transition densities. Then, a variational principle of the multistate subspace energy is established, whose minimization yields both the energies and densities of the individual N eigenstates. Furthermore, we prove that the N-dimensional matrix density D(r) can be sufficiently represented by N 2 nonorthogonal Slater determinants, based on which an interacting active space is introduced for practical calculations. This work establishes that the ground and excited states can be treated on an equal footing in density functional theory.

show abstract

DFT Exchange: Sharing Perspectives on the Workhorse of Quantum Chemistry and Materials Science

Cited by 7 publications

References 140 publications

Some Problems in Density Functional Theory

Some Problems in Density Functional Theory

Large dataset of molecular and reaction energies from multi-level quantum chemical methods

Multistate Density Functional Theory of Excited States

Contact Info

Product

Resources

About