Electron–Hole Pair Effects in Polyatomic Dissociative Chemisorption: Water on Ni(111)

Jiang, Bin; Alducin, M.; Guo, Hua

doi:10.1021/acs.jpclett.5b02737

Cited by 76 publications

(95 citation statements)

References 48 publications

(117 reference statements)

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“…using regular NNs, sharing the same surface periodicity and symmetry. 37 However, the anisotropic TDPT-based EFT is subject to a more intertwined symmetry, with which two symmetry equivalent molecular configurations may have different but correlated individual tensor elements. Any symmetry operation corresponds to a transformation matrix that links the correlated EFTs, For a diatomic molecule interacting with a static surface, as displayed in Fig.…”

Section: Symmetry Adaption From Scalar To Tensorial Propertymentioning

confidence: 99%

Symmetry-Adapted High Dimensional Neural Network Representation of Electronic Friction Tensor of Adsorbates on Metals

2019

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Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics.However, the first principles description of electronic excitation remains challenging.In an efficient molecular dynamics with electronic friction (MDEF) method, the nonadiabatic couplings are effectively included in a so-called electronic friction tensor (EFT), which can be computed from first-order time-dependent perturbation theory (TDPT) in terms of density functional theory (DFT) orbitals. This second-rank tensor depends on adsorbate position and features a complicated transformation with regard to the intrinsic symmetry operations of the system. In this work, we develop a new symmetry-adapted neural network representation of EFT, based on our recently proposed embedded atom neural network (EANN) framework. Inspired by the derivation of the nonadiabatic coupling matrix, we represent the tensorial friction by the first and second derivatives of multiple outputs of NNs with respect to atomic Cartesian coordinates. This rigorously preserves the positive semidefiniteness, directional property, and correct symmetry-equivariance of EFT. Unlike previous methods, our new approach can readily include both molecular and surface degrees of freedom, regardless of the type of surface. Tests on the H2+Ag(111) system show that this approach yields an accurate, efficient, and continuous representation of EFT, making it possible to perform large scale TDPT-based MDEF simulations to study both adiabatic and nonadiabatic energy dissipation in a unified framework.

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Section: Symmetry Adaption From Scalar To Tensorial Propertymentioning

confidence: 99%

Symmetry-Adapted High Dimensional Neural Network Representation of Electronic Friction Tensor of Adsorbates on Metals

2019

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“…Although the studied system could be made from different kinds of DoF [9], the most widely studied one is nuclear or atomic or phononic DoF under the influence of thermal baths [10][11][12][13][14][15][16][17][18]. Interesting applications include the study of nuclear quantum effects [17][18][19][20][21][22][23][24][25][26], heat transport between two different thermal baths [12][13][14][15][16][27][28][29][30][31][32][33][34][35][36][37], scattering of single molecule on surfaces [38][39][40][41][42][43][44][45][46][47][48][49][50]…”

Section: Introductionmentioning

confidence: 99%

Semi-classical generalized Langevin equation for equilibrium and nonequilibrium molecular dynamics simulation

Kai-Lun

Hedegård

et al. 2019

Progress in Surface Science

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Molecular dynamics (MD) simulation based on Langevin equation has been widely used in the study of structural, thermal properties of matters in difference phases. Normally, the atomic dynamics are described by classical equations of motion and the effect of the environment is taken into account through the fluctuating and frictional forces. Generally, the nuclear quantum effects and their coupling to other degrees of freedom are difficult to include in an efficient way. This could be a serious limitation on its application to the study of dynamical properties of materials made from light elements, in the presence of external driving electrical or thermal fields. One example of such system is single molecular dynamics on metal surface, an important system that has received intense study in surface science. In this review, we summarize recent effort in extending the Langevin MD to include nuclear quantum effect and their coupling to flowing electrical current. We discuss its applications in the study of adsorbate dynamics on metal surface, current-induced dynamics in molecular junctions, and quantum thermal transport between different reservoirs.

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“…The adiabatic treatment of DC processes is supported by recent studies using friction models. 27,28 The DC dynamics can be modeled using ab initio molecular dynamics (AIMD), in which the electronic structure calculations are performed on-the-fly along the nuclear trajectories. 29,30 It also has the added advantage that the energy transfer between the impinging molecule and surface phonons can be readily included.…”

mentioning

confidence: 99%

Communication: Enhanced dissociative chemisorption of CO2 via vibrational excitation

Jiang

Guo

2016

The Journal of Chemical Physics

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Electron–Hole Pair Effects in Polyatomic Dissociative Chemisorption: Water on Ni(111)

Cited by 76 publications

References 48 publications

Symmetry-Adapted High Dimensional Neural Network Representation of Electronic Friction Tensor of Adsorbates on Metals

Symmetry-Adapted High Dimensional Neural Network Representation of Electronic Friction Tensor of Adsorbates on Metals

Semi-classical generalized Langevin equation for equilibrium and nonequilibrium molecular dynamics simulation

Communication: Enhanced dissociative chemisorption of CO2 via vibrational excitation

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