An experimentally validated neural-network potential energy surface for H-atom on free-standing graphene in full dimensionality

Wille, Sebastian; Jiang, Hongyan; Bünermann, Oliver; Wodtke, Alec M.; Behler, Jörg; Kandratsenka, Alexander

doi:10.1039/d0cp03462b

Cited by 16 publications

(33 citation statements)

References 42 publications

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“…The accuracy of RPMD decreases with the simulation time, but on the short-time scales characteristic for the hydrogen motion at surfaces (∼100 fs), one can expect a small accuracy loss. 145 …”

Section: Theoretical Methodsmentioning

confidence: 99%

“…Recently, we developed a new PES using neural networks, 145 considerably improving the quality of the PES. Figure 10 shows a comparison of molecular dynamics simulation using the new PES in comparison with experiment.…”

Section: Transient Bond Formation In Collisions Of H On Graphenementioning

confidence: 99%

Section: Transient Bond Formation In Collisions Of H On Graphenementioning

confidence: 99%

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Inelastic Scattering of H Atoms from Surfaces

2021

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We have developed an instrument that uses photolysis of hydrogen halides to produce nearly monoenergetic hydrogen atom beams and Rydberg atom tagging to obtain accurate angle-resolved time-of-flight distributions of atoms scattered from surfaces. The surfaces are prepared under strict ultrahigh vacuum conditions. Data from these experiments can provide excellent benchmarks for theory, from which it is possible to obtain an atomic scale understanding of the underlying dynamical processes governing H atom adsorption. In this way, the mechanism of adsorption on metals is revealed, showing a penetration–resurfacing mechanism that relies on electronic excitation of the metal by the H atom to succeed. Contrasting this, when H atoms collide at graphene surfaces, the dynamics of bond formation involving at least four carbon atoms govern adsorption. Future perspectives of H atom scattering from surfaces are also outlined.

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Section: Theoretical Methodsmentioning

confidence: 99%

Section: Transient Bond Formation In Collisions Of H On Graphenementioning

confidence: 99%

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Inelastic Scattering of H Atoms from Surfaces

2021

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“… 1 DIS may exhibit maximum flux near the specular scattering angle similar to reflection of light from a flat-mirrored surface. Such behavior is often described as “single-bounce” scattering 2 , 3 since measured translational inelasticity is typically consistent with simple models where momentum is exchanged between the projectile and a single surface atom. 4 , 5 Furthermore, the measured translational 6 and internal 7 energy distributions of scattered particles are nonthermal.…”

Section: Introductionmentioning

confidence: 99%

Multibounce and Subsurface Scattering of H Atoms Colliding with a van der Waals Solid

et al. 2021

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We report the results of inelastic differential scattering experiments and full-dimensional molecular dynamics trajectory simulations for 2.76 eV H atoms colliding at a surface of solid xenon. The interaction potential is based on an effective medium theory (EMT) fit to density functional theory (DFT) energies. The translational energy-loss distributions derived from experiment and theory are in excellent agreement. By analyzing trajectories, we find that only a minority of the scattering results from simple single-bounce dynamics. The majority comes from multibounce collisions including subsurface scattering where the H atoms penetrate below the first layer of Xe atoms and subsequently re-emerge to the gas phase. This behavior leads to observable energy-losses as large as 0.5 eV, much larger than a prediction of the binary collision model (0.082 eV), which is often used to estimate the highest possible energy-loss in direct inelastic surface scattering. The sticking probability computed with the EMT-PES (0.15) is dramatically reduced (5 × 10 –6 ) if we employ a full-dimensional potential energy surface (PES) based on Lennard-Jones (LJ) pairwise interactions. Although the LJ-PES accurately describes the interactions near the H–Xe and Xe–Xe energy minima, it drastically overestimates the effective size of the Xe atom seen by the colliding H atom at incidence energies above about 0.1 eV.

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“…Importantly, the PES is a function of both H and C atom coordinates and accurately represents the potential for large displacements of the C atoms from their equilibrium positions in graphene. This was achieved by using machine learning algorithms to train the HDNN to energies calculated with DFT, including configurations of the H and C atoms from ab initio molecular dynamics (AIMD) (on the fly DFT) trajectory calculation 329. The comparison between simulations, based on hundreds of thousands of trajectories, and the experimental results is remarkably good.The success of the trajectory simulations allows us to learn more about the process of covalent C-H bond formation and other scattering phenomena seen in experiment.…”

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confidence: 99%

Chemical dynamics from the gas‐phase to surfaces

2021

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The field of gas‐phase chemical dynamics has developed superb experimental methods to probe the detailed outcome of gas‐phase chemical reactions. These experiments inspired and benchmarked first principles dynamics simulations giving access to an atomic scale picture of the motions that underlie these reactions. This fruitful interplay of experiment and theory is the essence of a dynamical approach perfected on gas‐phase reactions, the culmination of which is a standard model of chemical reactivity involving classical trajectories or quantum wave packets moving on a Born–Oppenheimer potential energy surface. Extending the dynamical approach to chemical reactions at surfaces presents challenges of complexity not found in gas‐phase study as reactive processes often involve multiple steps, such as inelastic molecule‐surface scattering and dissipation, leading to adsorption and subsequent thermal desorption and or bond breaking and making. This paper reviews progress toward understanding the elementary processes involved in surface chemistry using the dynamical approach. Key points The fruitful interplay between chemistry and physics leads to an atomic scale view of reactions taking places at catalytically active surfaces. Improved observations of chemical reactions taking place in complex environments drive the development of new approaches to theoretical chemistry. Complex reaction networks from real catalysts are boiled down to their elementary steps and examined from first principles.

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An experimentally validated neural-network potential energy surface for H-atom on free-standing graphene in full dimensionality

Abstract: We present a first principles-quality potential energy surface (PES) describing the inter-atomic forces for hydrogen atoms interacting with free-standing graphene. The PES is a high-dimensional neural network potential that has...

Cited by 16 publications

References 42 publications

Inelastic Scattering of H Atoms from Surfaces

Inelastic Scattering of H Atoms from Surfaces

Multibounce and Subsurface Scattering of H Atoms Colliding with a van der Waals Solid

Chemical dynamics from the gas‐phase to surfaces

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