### ?

## Comment on “Pushing the frontiers of density functionals by solving the fractional electron problem”

Science. 2022. Vol. 377. No. 6606. Article eabq3385.

Gerasimov I., Losev T., Evgeny Yu. Epifanov, Rudenko I., Bushmarinov I., Ryabov A., Zhilyaev P., Medvedev M.

Kirkpatrick et al. (Reports, 9 December 2021, p. 1385) trained a neural network–based DFT functional, DM21, on fractional-charge (FC) and fractional-spin (FS) systems, and they claim that it has outstanding accuracy for chemical systems exhibiting strong correlation. Here, we show that the ability of DM21 to generalize the behavior of such systems does not follow from the published results and requires revisiting.

Keywords: DFTТеория функционала плотностиглубокие нейронные сетиartificial neural networkDensity functional theory (DFT)

Publication based on the results of:

Medvedev M., Bushmarinov I., Sun J. et al., Science 2017 Vol. 355 No. 6320 P. 49-52

The theorems at the core of density functional theory (DFT) state that the energy of a many-electron system in its ground state is fully defined by its electron density distribution. This connection is made via the exact functional for the energy, which minimizes at the exact density. For years, DFT development focused on energies, implicitly ...

Added: October 12, 2019

T.V. Pavlova, S.L. Kovalenko, K.N. Eltsov, Journal of Physical Chemistry C 2020 Vol. 124 No. 15 P. 8218-8224

The structures formed by propylene adsorption on Ni(111) at room temperature are determined by a combination of scanning tunneling microscopy and density functional theory. As a result of the interaction with the Ni(111) surface, propylene molecules are dehydrogenated and coupled into linear hydrocarbon chains. The length of the chains varies from 8 to 60 Å, ...

Added: December 7, 2020

Norman G., Saitov I., Письма в Журнал экспериментальной и теоретической физики 2020 Т. 111 № 3 С. 175-180

Semimetal states of crystalline molecular hydrogen have been obtained at a temperature of 100 K in the pressure
range from 410 to 626 GPa. To analyze the nature of conductivity, the band structure is calculated in the
framework of the density functional theory using the Heyd–Scuseria–Ernzerhof hybrid exchange-correlation
functional. One of the semimetal states occurs in a monoclinic ...

Added: October 29, 2022

Saitov I., Журнал экспериментальной и теоретической физики 2020 Т. 157 № 3 С. 504-512

Density-functional theory (DFT) is applied to the calculation of the equation of state, the pair correlation
function (PCF), and the static electrical conductivity of solid hydrogen near the transition point to
the conducting state. It is found that the pressure versus density exhibits hysteresis at temperature of 100 K
under compression followed by expansion. The overlapping of the ...

Added: October 29, 2022

Medvedev M., Marjewski A., Gerasimov I. et al., Mendeleev Communications 2018 Vol. 28 No. 3 P. 225-235

The task of choosing a reliable density functional (DFT) approximation remains one of the most puzzling ones in quantum chemical modeling and materials simulations. Since DFT functionals are in general not systematically improvable, benchmarking them on specifically designed test sets is the usual way for identifying a method best suited for a particular purpose. To ...

Added: October 12, 2019

Garkul A., Stegailov V., Scientific Reports 2022 Vol. 12 No. 1 Article 13325

Unlike conventional first-order phase transitions, the kinetics of amorphous-amorphous transitions has been much less studied. The ultrasonic experiments on the transformations between low-density and high-density amorphous ice induced by pressure or heating provided the pressure and temperature dependencies of elastic moduli. In this article, we make an attempt to build a microscopic picture of these ...

Added: August 8, 2022

Möllmer J., Uhlig H., Lange M. et al., Journal of Alloys and Compounds 2021 Vol. 859 Article 157782

MgPd2 is an intermetallic compound with a reversible hydrogen uptake near ambient conditions. Hydrogenation occurs near room temperature at pressures below 0.1 MPa to form a hydrogen-rich MgPd2H0.88 phase. In this work, hydrogen sorption isotherms were measured at 283 K ≤ T ≤ 328 K as well as at a cryogenic temperature of 77 K and pressure values up ...

Added: November 5, 2020

Smirnov Grigory, Stegailov Vladimir, Lobachevskii Journal of Mathematics 2017 Vol. 38 No. 5 P. 974-977

The density functional theory (DFT) is a research tool of the highest importance for electronic structure calculations. It is often the only affordable method for ab initio calculations of complex materials. The pseudopotential approach allows reducing the total number of electrons in the model that speeds up calculations. However, there is a lack of pseudopotentials ...

Added: January 29, 2018

Kolesnikov A. L., Budkov Y., Barbosa G. D. et al., Fluid Phase Equilibria 2023 No. 564 Article 113567

Theoretical modeling of water adsorption in micro- and mesoporous materials remains a challenging problem for physical chemistry and chemical engineering despite its great importance for industrial applications. Here, we present the theoretical study of bulk and inhomogeneous water within the classical density functional theory. Our model includes all important intermolecular interactions, such as dispersion, association, ...

Added: August 30, 2022

Gurina D., Budkov Y., Kiselev M. G., Journal of Molecular Liquids 2022 Vol. 352 Article 118758

A full-atomic classical molecular dynamics simulation of polylactide nanoparticle impregnation with carbamazepine in supercritical carbon dioxide was performed. The effect of temperature (333 K, 373 K), pressure (20 MPa, 40 MPa) and ethanol addition (1.7 mol.%) on the impregnation process was studied. Based on the solvent accessible surface area values it was concluded that a pressure increase and cosolvent addition ...

Added: February 19, 2022

Olloqui-Sariego J. L., Zakharova G., Poloznikov A. et al., Electrochimica Acta 2020 Vol. 351 P. 136465

A major challenge in the design of electrochemical biodevices is to achieve fast rates of electron exchange between proteins and electrodes. In this work, we show that a significant increase in the direct electron transfer rate between a graphite electrode and Tobacco Peroxidase takes place when a surface exposed leucine, located in the vicinity of ...

Added: July 22, 2020

Budkov Y., М. : ЛЕНАНД, 2020

Within the presented monograph for the first time statistical approaches, based on the self-consistent field theory, were presented for the theoretical description of the thermodynamic properties of the ion-molecular systems (electrolyte solutions, ionic liquids, dielectric polymers and metal-organic frameworks) in the bulk solution and at the interfaces with the account for their molecular structure. In ...

Added: November 18, 2019

М. : Энциклопедия, Инфра-М, 2018

The New Russian Encyclopedia is a fundamental reference publication in 18 volumes that characterizes nature, population, economy, history, science, art, technology and other important aspects. Contains about 60,000 articles, about 30,000 biographies, about 15,000 color illustrations, maps, charts, diagrams, tables. Leaves since 2003. ...

Added: October 26, 2018

Kolesnikov A. L., Budkov Y., Gor G. Y., Journal of Physics: Condensed Matter 2022 Vol. 34 No. 6 Article 063002

Adsorption-induced deformation is a change in geometrical dimensions of an adsorbent
material caused by gas or liquid adsorption on its surface. This phenomenon is universal and
sensitive to adsorbent properties, which makes its prediction a challenging task. However, the
pure academic interest is complemented by its importance in a number of engineering
applications with porous materials characterization among them. ...

Added: October 20, 2021

Norman G., Saitov I., Physical Review E - Statistical, Nonlinear, and Soft Matter Physics 2016 Vol. 94 No. 043202 P. 043202-1-043202-8

We provide theoretical analysis of the reflectance of shock-compressed plasmas and warm dense matter for normal incidence of laser radiation as well as for the dependence of s- and p-polarized reflectivity on the incidence angle. The self-consistent approach for the calculation of the optical and electronic properties of warm dense matter and nonideal plasmas developed ...

Added: March 30, 2017

Budkov Y., Journal of Physics: Condensed Matter 2019 Vol. 31 P. 078002-078003

We reply to the comment on our paper by Budkov (2018 J. Phys.: Condens. Matter 30 344001). ...

Added: January 4, 2019

Kalikin N., Budkov Y., Kolesnikov A. L. et al., Fluid Phase Equilibria 2021 Vol. 544-545 Article 113096

Despite the modern level of development of computational chemistry methods and technological progress, fast and accurate determination of solvation free energy remains a huge problem for physical chemists. In this paper, we describe two computational schemes that can potentially solve this problem. We consider systems of poorly soluble drug compounds in supercritical carbon dioxide. Considering that the biggest contribution ...

Added: June 1, 2021

Андрюшечкин Б. В., Eltsov K., Pavlova T. et al., Journal of Chemical Physics 2018 Vol. 148 No. 24 Article 244702

The adsorption of O-2 on Ag(111) between 300 and 500 K has been studied with temperature-programmed desorption (TPD) and scanning tunneling microscopy (STM). At the first stage of adsorption, the disordered local oxide phase (commonly looking in STM as an array of black spots) is formed on the surface irrespective of the substrate temperature. The maximum concentration of black spots was found to be approximate to 0.11 ML, which corresponds to an oxygen coverage of approximate to 0.66 ML. Taking into account that the nucleation of the Ag(111)-p(4 x 4)-O phase starts after the saturation of the disordered phase, one ...

Added: October 25, 2021

Maslov V., Теоретическая и математическая физика 2019 Т. 201 № 1 С. 65-83

We study the process of a nucleon separating from an atomic nucleus from the mathematical standpoint
using experimental values of the binding energy for the nucleus of the given substance. A nucleon becomes
a boson at the instant of separating from a fermionic nucleus. We study the further transformations of
boson and fermion states of separation in a ...

Added: November 1, 2019

Zavarzin Semen V., Kolesnikov A. L., Budkov Y. et al., The European Physical Journal E - Soft Matter 2022 Vol. 45 Article 24

A model is developed for describing the transport of charged colloidal particles in an evaporating sessile droplet on the electrified metal substrate in the presence of a solvent flow. The model takes into account the electric charge of colloidal particles and small ions produced by electrolytic dissociation of the active groups on the colloidal particles ...

Added: March 15, 2022

Голосов Е. В., Алдошин С. М., Палий А. В. et al., Reviews and Advances in Chemistry 2021 Vol. 11 No. 3-4 P. 145-165

This article is a short overview of the problem of controllable magnetic spin communicationas an important ingredient of spintronics and molecular electronics. We discuss the problem of communicationof the two localized spins mediated by the mobile electron which is shared between twonon-magnetic sites coupled to the mobile spins. The model system which is assumed to ...

Added: October 10, 2022

Gavryushkin P., Belonoshko Anatoly B., Sagatov N. et al., Crystal Growth & Design 2021 Vol. 21 No. 1 P. 65-74

Using molecular dynamics simulation and evolutionary metadynamic calculations, a series of structures were revealed that possessed enthalpies and Gibbs energies lower than those of aragonite but higher than those of calcite. The structures are polytypes of calcite, differing in the stacking sequence of close-packed (cp) Ca layers. The two- and six-layered polytypes have hexagonal symmetry P6322 ...

Added: January 21, 2021

Andronov M., Kuzmin A. V., Shestakov A. et al., Inorganica Chimica Acta 2022 Vol. 533 Article 120789

Series of anionic salts of fullerenes C60 and C70 with different metal tetraphenylporphyrins, MIITPP, where M = Co, Mn and Zn, and N, N, N, N‘, N‘-pentamethyldiaminoethane cations (PMDAE+) has been obtained in a crystalline form. Composition of the complexes is (PMDAE+)⋅(MIITPP)(C60−)⋅XC6H4Cl2 (M = Co, X = 1.25 (1), M = Mn, X = 0.75 (2) and M = Zn, X = 0.75 (3)) and {(PMDAE+)⋅ZnIITPP}2⋅(C70−)2⋅4C6H4Cl2 ...

Added: October 22, 2022

Budkov Y., Kolesnikov A. L., Polymer Science - Series C 2018 Vol. 60 No. Supplement 1 P. 148-159

Theoretical models of the conformational behavior of flexible polymer chains in mixed solvents enunciated in the world literature during the last decade are critically reviewed. Models describing different mechanisms of coil-to-globule transitions in a good solvent induced by cosolvent addition are highlighted. Special attention is given to the analysis of theoretical approaches to describing the ...

Added: November 30, 2018