Semi-supervised Machine Learning Enables the Robust Detection of Multireference Character at Low Cost

The Journal of Physical Chemistry Letters
Chenru DuanHeather Kulik

Abstract

Multireference (MR) diagnostics are common tools for identifying strongly correlated electronic structure that makes single-reference (SR) methods (e.g., density functional theory or DFT) insufficient for accurate property prediction. However, MR diagnostics typically require computationally demanding correlated wave function theory (WFT) calculations, and diagnostics often disagree or fail to predict MR effects on properties. To overcome these challenges, we introduce a semi-supervised machine learning (ML) approach with virtual adversarial training (VAT) of an MR classifier using 15 WFT and DFT MR diagnostics as inputs. In semi-supervised learning, only the most extreme SR or MR points are labeled, and the remaining point labels are learned. The resulting VAT model outperforms the alternatives, as quantified by the distinct property distributions of SR- and MR-classified molecules. To reduce the cost of generating inputs to the VAT model, we leverage the VAT model's robustness to noisy inputs by replacing WFT MR diagnostics with regression predictions in an MR decision engine workflow that preserves excellent performance. We demonstrate the transferability of our approach to larger molecules and those with distinct chemical c...Continue Reading

References

Dec 8, 2005·The Journal of Physical Chemistry. a·Nathan E SchultzDonald G Truhlar
Mar 5, 2008·The Journal of Chemical Physics·Jeng-Da Chai, Martin Head-Gordon
Mar 15, 2008·The Journal of Physical Chemistry. a·John S Sears, C David Sherrill
Jul 3, 2008·The Journal of Physical Chemistry. a·John S Sears, C David Sherrill
Oct 11, 2011·Journal of Cheminformatics·Noel M O'BoyleGeoffrey R Hutchison
Jan 25, 2012·Nature Chemistry·Christopher E WilmerRandall Q Snurr
Mar 10, 2012·Physical Review Letters·Matthias RuppO Anatole von Lilienfeld
Mar 22, 2012·ACS Combinatorial Science·Sangil HanJ Carson Meredith
Dec 6, 2012·Angewandte Chemie·Jens K Nørskov, Thomas Bligaard
Feb 21, 2013·Nature Materials·Stefano CurtaroloOhad Levy
Apr 4, 2013·Journal of the American Chemical Society·Aaron M VirshupDavid N Beratan
Oct 1, 2013·Scientific Reports·Ghanshyam PilaniaRamamurthy Ramprasad
Mar 18, 2015·The Journal of Chemical Physics·Yinan Shu, Benjamin G Levine
Apr 18, 2015·Angewandte Chemie·Stefan Grimme, Andreas Hansen
Jan 1, 2014·Scientific Data·Raghunathan RamakrishnanO Anatole von Lilienfeld
May 16, 2013·The Journal of Physical Chemistry Letters·Ilana Y KanalGeoffrey R Hutchison
Feb 14, 2012·Journal of Chemical Theory and Computation·Wanyi JiangAngela K Wilson
Aug 1, 2008·Journal of Chemical Theory and Computation·Oksana TishchenkoDonald G Truhlar
Mar 10, 2016·Journal of Chemical Theory and Computation·Christopher Johannes Stein, Markus Reiher
Apr 23, 2016·Physical Chemistry Chemical Physics : PCCP·Sandip DeMichele Ceriotti
May 2, 2016·The Journal of Chemical Physics·Jeffrey B Schriber, Francesco A Evangelista
Jun 10, 2016·The Journal of Chemical Physics·Lee-Ping Wang, Chenchen Song
Jul 2, 2016·Journal of Computational Chemistry·Efthymios I IoannidisHeather J Kulik
Aug 16, 2016·Physical Chemistry Chemical Physics : PCCP·Eloy Ramos-CordobaEduard Matito
May 11, 2017·Journal of Chemical Theory and Computation·Robert M ParrishC David Sherrill
May 19, 2017·Journal of Chemical Theory and Computation·Eloy Ramos-Cordoba, Eduard Matito
Nov 3, 2017·The Journal of Physical Chemistry. a·Jon Paul Janet, Heather J Kulik
Dec 20, 2017·Journal of Chemical Information and Modeling·Suzanne McAnanama-Brereton, Mark P Waller
Feb 21, 2018·Journal of Chemical Information and Modeling·Patrick BleizifferSereina Riniker
Jul 2, 2018·The Journal of Chemical Physics·Christopher R CollinsDavid J Yaron
Jul 25, 2018·IEEE Transactions on Pattern Analysis and Machine Intelligence·Takeru MiyatoShin Ishii
Jul 25, 2018·Journal of Chemical Theory and Computation·Matthew WelbornThomas F Miller
Oct 13, 2018·Chemical Science·Benjamin MeyerClémence Corminboeuf
Oct 22, 2018·The Journal of Chemical Physics·Manoj K KesharwaniJan M L Martin
Oct 31, 2018·Chemical Reviews·Konstantinos D VogiatzisEvgeny A Pidko
Mar 10, 2019·Proceedings of the National Academy of Sciences of the United States of America·Carey E PriebeEric Bridgeford
Mar 13, 2019·Journal of Chemical Theory and Computation·Chenru DuanHeather J Kulik
Apr 22, 2019·The Journal of Chemical Physics·Michele Ceriotti
Jul 6, 2019·The Journal of Physical Chemistry Letters·Mireia Via-NadalEduard Matito
Mar 3, 2020·Journal of Chemical Theory and Computation·WooSeok JeongLaura Gagliardi
Mar 23, 2020·The Journal of Chemical Physics·Daniel SüßAndreas Mauracher
Jun 17, 2020·Journal of Chemical Theory and Computation·Chenru DuanHeather J Kulik

❮ Previous
Next ❯

Citations

Mar 10, 2021·The Journal of Chemical Physics·Sumanta K GhoshDebashree Ghosh
Nov 20, 2020·Chemical Reviews·Julia Westermayr, Philipp Marquetand
Apr 17, 2021·Journal of Chemical Theory and Computation·Daniel S King, Laura Gagliardi
Jul 10, 2021·The Journal of Chemical Physics·Julia WestermayrReinhard J Maurer
Aug 11, 2021·The Journal of Physical Chemistry Letters·Daniel S KingLaura Gagliardi
Nov 10, 2020·Journal of Chemical Information and Modeling·David Balcells, Bastian Bjerkem Skjelstad
Sep 1, 2020·The Journal of Physical Chemistry Letters·Fang LiuHeather J Kulik
Jan 7, 2021·The Journal of Physical Chemistry. B·Qiang CuiLuke Xie

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.