Theoretical study on collision dynamics of H+ + CH4 at low energies

Gao, Cong-Zhang; Wang, Jing; Wang, Feng; Zhang, Feng-Shou

doi:10.1063/1.4863635

Cited by 26 publications

(22 citation statements)

References 79 publications

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“…Higherlevel self-interaction-free approaches like LDA + ADSIC and EXX overestimate the rainbow angle too, but are relatively closer to the experimental results. The AD-SIC results agree with Gao et al [41] and the EXX compare favorably with the HF-based method of Jaquemin et al [40]. Both LDA and PBE show the same features in Octopus and Qbox as shown in Fig.…”

Section: Resultssupporting

confidence: 86%

“…This orientation is identical to the Face II orientations of Jacquemin et al [40] and Gao et al [41] in which the incoming proton moves towards the methane from the negative-to-positive z-axis. The impact parameter b was increased in the positive x-axis.…”

Section: Computational Detailssupporting

confidence: 78%

“…This suggests that a repulsive interaction is taking place at long ranges due to electronic self-interaction effects [88,89]. [41]) for Face II orientation. Horizontal line is the experimentally determined rainbow angle over random orientations [12].…”

Section: Resultsmentioning

confidence: 97%

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Self-interaction effects on charge-transfer collisions

et al. 2017

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In this article, we investigate the role of the self-interaction error in the simulation of collisions using time-dependent density functional theory (TDDFT) and Ehrenfest dynamics. We compare many different approximations of the exchange and correlation potential, using as a test system the collision of H + + CH4 at 30 eV. We find that semi-local approximations, like PBE, and even hybrid functionals, like B3LYP, produce qualitatively incorrect predictions for the scattering of the proton. This discrepancy appears because the self-interaction error allows the electrons to jump too easily to the proton, leading to radically different forces with respect to the non-self-interacting case. From our results, we conclude that using a functional that is self-interaction free is essential to properly describe charge-transfer collisions between ions and molecules in TDDFT.

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Section: Resultssupporting

confidence: 86%

Section: Computational Detailssupporting

confidence: 78%

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Self-interaction effects on charge-transfer collisions

et al. 2017

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“…Our results are based on 1D models so cannot capture effects from channels where the electron scatters around the target in real systems. Also, whether the errors from the approximate methods are so large for realistic systems with more electrons and vibronic effects, is unclear; still, the results here suggest the tendency of adiabatic TDDFT to underestimate scattering in realistic systems [6,7,8,9,10,11,12].…”

Section: Discussionmentioning

confidence: 86%

Electron scattering in time-dependent density functional theory

et al. 2018

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It was recently shown [Y. Suzuki, L. Lacombe, K. Watanabe, and N. T. Maitra, Phys. Rev. Lett. 119, 263401 (2017)] that peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory are crucial for accurately capturing time-resolved dynamics of electron scattering in a model one-dimensional system. Approximate functionals used today miss these structures and consequently underestimate the scattering probability. The dynamics can vary significantly depending on the choice of the initial Kohn-Sham state, and, with a judicious choice, a recently-proposed non-adiabatic approximation provides extremely accurate dynamics on approach to the target but this ultimately also fails to capture reflection accurately. Here we provide more details, using a model of electron-He + as illustration, in both the inelastic and elastic regimes. In the elastic case, the time-resolved picture is contrasted with the time-independent picture of scattering, where the linear response theory of TDDFT can be used to extract transmission and reflection coefficients. Although the exact functional yields identical scattering probabilities when used in this way as it does in the time-resolved picture, we show that the currently-available approximate functionals do not, even when they have the correct asymptotic behavior.

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“…The lack of memory dependence is believed to be responsible for errors in its predictions, e.g., Refs. [11][12][13][14][15][16][17][18][19][20][21][22], including sometimes qualitative failures. Still, the approximations are often accurate enough to be useful, and some characterization of when to expect the adiabatic approximation to work well has also been done [23].…”

Section: Introductionmentioning

confidence: 99%

Exact time-dependent density-functional theory for nonperturbative dynamics of the helium atom

et al. 2021

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By inverting the time-dependent Kohn-Sham equation for a numerically exact dynamics of the helium atom, we show that the dynamical step and peak features of the exact correlation potential found previously in onedimensional models persist for real three-dimensional systems. We demonstrate that the Kohn-Sham and true current densities differ by a rotational component. The results have direct implications for approximate timedependent density functional theory calculations of atoms and molecules in strong fields, emphasizing the need to go beyond the adiabatic approximation, and highlighting caution in the quantitative use of the Kohn-Sham current.

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Theoretical study on collision dynamics of H+ + CH4 at low energies

Cited by 26 publications

References 79 publications

Self-interaction effects on charge-transfer collisions

Self-interaction effects on charge-transfer collisions

Electron scattering in time-dependent density functional theory

Exact time-dependent density-functional theory for nonperturbative dynamics of the helium atom

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