Auxiliary Density Functional Theory: From Molecules to Nanostructures

Calaminici, Patrizia; Alvarez-Ibarra, Aurélio; Cruz-Olvera, Domingo; Domı́nguez-Soria, Victor-Daniel; Flores‐Moreno, Roberto; Gamboa, Gabriel U.; Geudtner, Gerald; Goursot, Annick; Mejı́a-Rodrı́guez, Daniel; Salahub, Dennis R.; Zúñiga-Gutiérrez, Bernardo; Köster, AndreasM.

doi:10.1007/978-94-007-6169-8_16-2

Cited by 11 publications

(11 citation statements)

References 234 publications

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“…[26,27] Calaminici et al [28] performed full geometry optimizations of single-shell fullerenes, that is, C 180 , C 240 , C 320 , and C 540 , using closed-shell configuration and double-ζ plus valence polarization in the local density approximation (LDA). Similar calculations in terms of basis sets are reported in other works, [29,30] although the latter were carried out in the frame of the auxiliary DFT.…”

Section: Computational Detailsmentioning

confidence: 63%

DFT study on electronic properties of single‐ and double‐shell icosahedral fullerenes

Luca

Valverde

Morrone

et al. 2019

Int J of Quantum Chemistry

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Multi‐shell fullerenes are widely studied for their interesting properties although comparative studies on single‐ and multi‐shell structures remain scarce. In this work, important electronic features of single‐ and double‐shell icosahedral fullerenes as a function of their sizes were calculated in the framework of the density functional theory. Fully optimized structures were used to get the gap between the highest occupied molecular and the lowest unoccupied molecular orbital (H‐L gap), electronegativity, softness and density of the electronic states. This work shows that the H‐L gap of the single‐shell fullerenes decreases nonlinearly as the nanoparticles size increases, whereas for the double‐shell fullerenes an opposite trend is obtained. A decrease of the H‐L gap is found going from single‐ to double‐shell fullerenes with similar external sizes, up to a diameter of 3.13 nm. The electron density of states revealed that isolated peaks give way to more dense electronic states for nanoparticles with diameters above 2 nm.

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Section: Computational Detailsmentioning

confidence: 63%

DFT study on electronic properties of single‐ and double‐shell icosahedral fullerenes

Luca

Valverde

Morrone

et al. 2019

Int J of Quantum Chemistry

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“…This dramatic reduction of the spacial dimensionality of the problem permits firstprinciple DFT calculations on large systems with hundreds or even thousands of atoms. 27,39 At the same time, the accuracy of KohnSham DFT calculations match well with correlated wave function approaches in many instances. This has made Kohn-Sham DFT the method of choice for a large variety of electronic structure calculations on atoms, molecules, and solids.…”

Section: Theorymentioning

confidence: 74%

“…26,27 One of the main reasons for using ADFT is the dramatic reduction in computational demands without sacrificing the accuracy of the underlying Kohn-Sham formalism. The improved computational efficiency is due to the variational fitting of the Coulomb potential [28][29][30] and the use of the resulting approximated density for the calculation of the exchange-correlation energy and potential.…”

Section: Introductionmentioning

confidence: 99%

Photoabsorption spectra from time-dependent auxiliary density functional theory

Carmona-EspíndolaJavier

KösterAndreas

2013

Can. J. Chem.

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Time-dependent auxiliary density perturbation theory (TDADPT) is extended to the calculation of excited states. The resulting time-dependent auxiliary density functional theory (TDADFT) is structurally identical to the original formulation of Casida. However, significant simplifications occur for the Coulomb and exchange-correlation response due to the underlying auxiliary density functional theory. Here, we present the working equations for TDADFT and a new implementation. Because this new parallel TDADFT implementation is particularly well suited for the calculation of large numbers of excitations, we validate it by the calculation of photoabsorption spectra. Direct comparison with experiment underlines the accuracy and reliability of TDADFT. For selected peaks of the studied polycyclic aromatic hydrocarbon spectra, the assignments of the underlying excitations are also presented. Résumé :On étend la théorie de la perturbation de la fonctionnelle de la densité auxiliaire dépendantes du temps (TDADPT) au calcul des états excités. La théorie de la fonctionnelle de la densité auxiliaire dépendante du temps (TDADFT) résultante est structurellement identique à la formulation originale de Casida. Cependant, la théorie de la fonctionnelle de la densité auxiliaire sous-jacente donne lieu à des simplifications importantes de la réponse coulombienne et d'échange-corrélation. On présente ici les équations de travail pour la TDADFT ainsi qu'une nouvelle mise en oeuvre. Comme cette nouvelle mise en oeuvre parallèle de la TDADFT convient particulièrement bien pour le calcul de grands nombres d'excitations, on la valide par le calcul des spectres de photoabsorption. Une comparaison directe avec l'expérience met en relief l'exactitude et la fiabilité de la TDADFT. On présente aussi l'attribution des excitations sous-jacentes pour certains pics des spectres des hydrocarbures aromatiques polycycliques étudiés. [Traduit par la Rédaction] Mots-clés : spectres de photoabsorption, hydrocarbures aromatiques polycycliques, théorie de la fonctionnelle de la densité auxiliaire dépendante du temps, théorie des perturbations.

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“…The QM engine relies on Auxiliary DFT that complies to the Kohn-Sham framework but makes use of variationally fitted electron densities (i.e. auxiliary electron densities) to evaluate classical electron repulsion terms and exchange-correlation (XC) matrix elements [29].…”

Section: Methodsmentioning

confidence: 99%

Femtosecond responses of hydrated DNA irradiated by ionizing rays focus on the sugar-phosphate part

Lande

2021

Theor Chem Acc

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In this article we investigate the mechanisms of DNA ionization upon irradiation by 0.5 MeV alpha particles. We focus on the sugar-phosphate group and its hydration shell. In radiation chemistry, the term quasi-direct effect refers the physical and chemical responses taking place after irradiation of solvent molecules pertaining to the solvation shells of solutes. The molecular mechanisms accounting for the quasi-direct effect are actually largely elusive, especially for those prevailing in the early time scales (<10 -12 s). We report Real-Time-Time-Dependent Auxiliary Density Functional Theory simulations carried out within the framework of hybrid QM/MM scheme (Quantum Mechanics/Molecular Mechanics) with polarizable and non-polarizable embedding. Ten water molecules from the solvation shell of DNA backbone are independently irradiated. We find that during the first femtoseconds after irradiation, the holes formed on the irradiated water remains at their sites of formation. Electrostatic induction within the environment doesn't significantly impact charge migrations. We address the hypothesis that charge migration driven by electron correlation is responsible for an ultrafast H2O + -to-DNA charge transfers, which would account for a quasi-direct effect. We find that pure charge migration at fixed nuclear positions is not responsible for the quasi-direct effect when considering sugar-phosphate solvation shells.

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Auxiliary Density Functional Theory: From Molecules to Nanostructures

Cited by 11 publications

References 234 publications

DFT study on electronic properties of single‐ and double‐shell icosahedral fullerenes

DFT study on electronic properties of single‐ and double‐shell icosahedral fullerenes

Photoabsorption spectra from time-dependent auxiliary density functional theory

Femtosecond responses of hydrated DNA irradiated by ionizing rays focus on the sugar-phosphate part

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