Quantum Chemical Topology of the Electron Localization Function in the Field of Attosecond Electron Dynamics

Parise, Angela; Alvarez-Ibarra, Aurélio; Wu, Xiaojing; Zhao, Xiaodong; Pilmé, Julien; Lande, Aurélien de la

doi:10.1021/acs.jpclett.7b03379

Cited by 23 publications

(28 citation statements)

References 38 publications

(56 reference statements)

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“…The study of systems at excited states is, however, possible with the recent development of Real-Time Time-Dependent DFT. Recent applications of this method include the topological analysis of charge migration after irradiation 74 and the calculation of stopping power of lithium cluster, 75 or biomolecules. 76 By employing this method, it would then be interesting to model and study the irradiation of the different water structures either in bulk or at the interface.…”

Section: Discussionmentioning

confidence: 99%

Probing the structural properties of the water solvation shell around gold nanoparticles: A computational study

Tandiana

Brun

Sicard-Roselli

et al. 2021

The Journal of Chemical Physics

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While subjected to radiation, gold nanoparticles (GNP) have been shown to enhance the production of radicals when added to aqueous solutions. It has been proposed that the arrangement of water solvation layers near the water-gold interface plays a significant role. As such, the structural and electronic properties of the first water solvation layer surrounding GNP of varying sizes were compared to bulk water using classical molecular dynamics, quantum and semiempirical methods. Classical molecular dynamics was used to understand the change in macroscopic properties of bulk water in the presence of different sizes of GNP, as well as by including salt ions. The analysis of these macroscopic properties has led to the conclusion that larger GNPs induce the rearrangement of water molecules to form a 2D hydrogen-bond network at the interface. Quantum methods were employed to understand the electronic nature of the interaction between water molecules and GNP along with the change in the water orientation and the vibrational density of states. The stretching region of vibrational density of states was found to extend into the higher wavenumber region, as the size of the GNP increases. This extension represents the dangling water molecules at the interface, as a result of reorientation of the water molecules in the first solvation shell. This multi-level study suggests that in the presence of GNP of increasing sizes, the first water solvation shell undergoes a rearrangement to maximize the water-water interactions as well as the water-GNP interactions.

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Section: Discussionmentioning

confidence: 99%

Probing the structural properties of the water solvation shell around gold nanoparticles: A computational study

Tandiana

Brun

Sicard-Roselli

et al. 2021

The Journal of Chemical Physics

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“…We use the aug-cc-pVTZ basis set [114] on sulfur and hydrogen atoms and a very diffuse basis set from Reference [115] for carbons. To remove emitted electrons from the system a complex absorbing potential is placed 10 Å away from the QM region [25,116]. We first conducted purely RT-TD-ADFT to simulate energy deposition and ionization.…”

Section: Applicationsmentioning

confidence: 99%

Molecular Simulations with in-deMon2k QM/MM, a Tutorial-Review

et al. 2019

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deMon2k is a readily available program specialized in Density Functional Theory (DFT) simulations within the framework of Auxiliary DFT. This article is intended as a tutorial-review of the capabilities of the program for molecular simulations involving ground and excited electronic states. The program implements an additive QM/MM (quantum mechanics/molecular mechanics) module relying either on non-polarizable or polarizable force fields. QM/MM methodologies available in deMon2k include ground-state geometry optimizations, ground-state Born–Oppenheimer molecular dynamics simulations, Ehrenfest non-adiabatic molecular dynamics simulations, and attosecond electron dynamics. In addition several electric and magnetic properties can be computed with QM/MM. We review the framework implemented in the program, including the most recently implemented options (link atoms, implicit continuum for remote environments, metadynamics, etc.), together with six applicative examples. The applications involve (i) a reactivity study of a cyclic organic molecule in water; (ii) the establishment of free-energy profiles for nucleophilic-substitution reactions by the umbrella sampling method; (iii) the construction of two-dimensional free energy maps by metadynamics simulations; (iv) the simulation of UV-visible absorption spectra of a solvated chromophore molecule; (v) the simulation of a free energy profile for an electron transfer reaction within Marcus theory; and (vi) the simulation of fragmentation of a peptide after collision with a high-energy proton.

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“…Real-time timedependent electronic-structure approaches can be conceptually separated in two classes: (1) real-time time-dependent wave function (RT-TDWF) based methods [18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34][35] and (2) real-time timedependent density functional theory (RT-TDDFT). [36][37][38][39][40][41][42][43][44][45][46] In RT-TDWF, the many-electron dynamics is described by a correlated time-dependent wave function, while in RT-TDDFT, the key quantity is the time-dependent density.…”

Section: Introductionmentioning

confidence: 99%

Role of exchange and correlation in high-harmonic generation spectra of H2, N2, and CO2: Real-time time-dependent electronic-structure approaches

Pauletti

Coccia²,

Luppi

2021

The Journal of Chemical Physics

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This study arises from the attempt to answer the following question: how different descriptions of electronic exchange and correlation affect the high-harmonic generation (HHG) spectroscopy of H 2 , N 2 , and CO 2 molecules? We compare HHG spectra for H 2 , N 2 , and CO 2 with different ab initio electronic structure methods: real-time time-dependent configuration interaction and real-time time-dependent density functional theory (RT-TDDFT) using truncated basis sets composed of correlated wave functions expanded on Gaussian basis sets. In the framework of RT-TDDFT, we employ Perdew-Burke-Ernzerhof (PBE) and long-range corrected Perdew-Burke-Ernzerhof (LC-ωPBE) functionals. We study HHG spectroscopy by disentangling the effect of electronic exchange and correlation. We first analyze the electronic exchange alone, and in the case of RT-TDDFT with LC-ωPBE, we use ω = 0.3 and ω = 0.4 to tune the percentage of long-range Hartree-Fock exchange and short-range exchange PBE. Then, we added the correlation as described by the PBE functional. All the methods give very similar HHG spectra, and they seem not to be particularly sensitive to the different description of exchange and correlation or to the correct asymptotic behavior of the Coulomb potential. Despite this general trend, some differences are found in the region connecting the cutoff and the background. Here, the harmonics can be resolved with different accuracy depending on the theoretical schemes used. We believe that the investigation of the molecular continuum and its coupling with strong fields merits further theoretical investigations in the near future.

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Quantum Chemical Topology of the Electron Localization Function in the Field of Attosecond Electron Dynamics

Cited by 23 publications

References 38 publications

Probing the structural properties of the water solvation shell around gold nanoparticles: A computational study

Probing the structural properties of the water solvation shell around gold nanoparticles: A computational study

Molecular Simulations with in-deMon2k QM/MM, a Tutorial-Review

Role of exchange and correlation in high-harmonic generation spectra of H2, N2, and CO2: Real-time time-dependent electronic-structure approaches

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