Quantum dynamics of hydrogen atoms on graphene. II. Sticking

Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H.; Burghardt, Irène; Martinazzo, Rocco

doi:10.1063/1.4931117

Cited by 22 publications

(46 citation statements)

References 49 publications

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“…As is shown in Appendix B of Ref. [ ], the function

g_{q} (v)

required in this case is given by

g_{q} (v) = \sqrt{\frac{m_{S}}{π ℏ Ω_{T}}} e^{- \frac{m_{normalS} u^{2}}{ℏ Ω_{T}}}

where the temperature‐dependent effective frequency Ω T accounts for the coupling with the bulk and is conveniently written in the form

Ω_{T} = \frac{\int_{0}^{+ \infty} d ω J (ω) ω^{2} \coth true(\frac{ℏ ω}{2 k_{B} T} true)}{\int_{0}^{+ \infty} d ω J (ω) ω}

…”

Section: Stickingmentioning

confidence: 99%

“…To the best of our knowledge, the only numerically converged, fully quantum study of a strongly coupled scattering problem, explicitly including the lattice degrees of freedom, is our recent work on the activated dynamics of hydrogen sticking on a graphitic/graphenic surface . This has been possible upon exploiting the relation between the independent oscillator models and the Langevin dynamics discussed in Appendix.…”

Section: Applicationsmentioning

confidence: 99%

“…This has been possible upon exploiting the relation between the independent oscillator models and the Langevin dynamics discussed in Appendix. We have devised and applied an elaborate strategy which, starting from the development of a general technique to extract information on the environmental forces acting on the system and the definition of a suitable dynamical model for a H atom bound to graphene, allowed us to investigate the sticking dynamics in a fully quantum setting …”

Section: Applicationsmentioning

confidence: 99%

See 2 more Smart Citations

Classical and quantum dynamics at surfaces: Basic concepts from simple models

Bonfanti

Martinazzo

2016

Int J of Quantum Chemistry

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Elementary processes involving atomic and molecular species at surfaces are reviewed. The emphasis is on simple classical and quantum models that help to single out unifying dynamical themes and to identify the basic physical mechanisms that underlie the rich variety of phenomena of surface chemistry. Starting from an elementary description of the energy transfer between a gas‐phase species and a surface—for both classical and quantum lattices—the key processes establishing the formation of an adsorbed phase (sticking, diffusion and vibrational relaxation) are discussed. This is instrumental for introducing the simplest chemical transformations involving adsorbed species and/or scattering of gas‐phase molecules: Langmuir–Hinshelwood, Hot‐Atom, and Eley–Rideal reactions forming complex molecules from elementary constituents, and dissociative chemisorption of molecules into smaller fragments. Applications are also provided illustrating the ideas developed along the way at work in real‐world gas‐surface problems.

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“…As is shown in Appendix B of Ref. [ ], the function

g_{q} (v)

required in this case is given by

g_{q} (v) = \sqrt{\frac{m_{S}}{π ℏ Ω_{T}}} e^{- \frac{m_{normalS} u^{2}}{ℏ Ω_{T}}}

where the temperature‐dependent effective frequency Ω T accounts for the coupling with the bulk and is conveniently written in the form

Ω_{T} = \frac{\int_{0}^{+ \infty} d ω J (ω) ω^{2} \coth true(\frac{ℏ ω}{2 k_{B} T} true)}{\int_{0}^{+ \infty} d ω J (ω) ω}

…”

Section: Stickingmentioning

confidence: 99%

Section: Applicationsmentioning

confidence: 99%

Section: Applicationsmentioning

confidence: 99%

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Classical and quantum dynamics at surfaces: Basic concepts from simple models

Bonfanti

Martinazzo

2016

Int J of Quantum Chemistry

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“…In the following paper, 57 henceforth denoted Paper II, we extend the approach to the quantum dynamical, dissipative scattering setting needed to investigate sticking of a hydrogen atom to the graphene surface. This paper is organized as follows.…”

Section: Introductionmentioning

confidence: 99%

Quantum dynamics of hydrogen atoms on graphene. I. System-bath modeling

Bonfanti

Jackson

Hughes

et al. 2015

The Journal of Chemical Physics

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Ab initio molecular dynamics of hydrogen dissociation on metal surfaces using neural networks and novelty sampling J. Chem. Phys. 127, 154716 (2007) An accurate system-bath model to investigate the quantum dynamics of hydrogen atoms chemisorbed on graphene is presented. The system comprises a hydrogen atom and the carbon atom from graphene that forms the covalent bond, and it is described by a previously developed 4D potential energy surface based on density functional theory ab initio data. The bath describes the rest of the carbon lattice and is obtained from an empirical force field through inversion of a classical equilibrium correlation function describing the hydrogen motion. By construction, model building easily accommodates improvements coming from the use of higher level electronic structure theory for the system. Further, it is well suited to a determination of the system-environment coupling by means of ab initio molecular dynamics. This paper details the system-bath modeling and shows its application to the quantum dynamics of vibrational relaxation of a chemisorbed hydrogen atom, which is here investigated at T = 0 K with the help of the multi-configuration time-dependent Hartree method. Paper II deals with the sticking dynamics. C 2015 AIP Publishing LLC. [http://dx

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“…for harmonic system potentials [29]; note that a similar in spirit but technically different method for linear GLEs was developed independently [46] and applied to quantum dynamics of hydrogen atoms on graphene [47,48]. In the following, we extend the method to the non-linear GLEs, Eq.…”

Section: Fourier Methodsmentioning

confidence: 99%

Vibrational spectroscopy via the Caldeira-Leggett model with anharmonic system potentials

Gottwald

Ivanov

Kühn

2016

The Journal of Chemical Physics

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Abstract. The Caldeira-Leggett (CL) model, which describes a system bi-linearly coupled to a harmonic bath, has enjoyed popularity in condensed phase spectroscopy owing to its utmost simplicity. However, the applicability of the model to cases with anharmonic system potentials, as it is required for the description of realistic systems in solution, is questionable due to the presence of the invertibility problem [J. Phys. Chem. Lett., 6, 2722Lett., 6, (2015] unless the system itself resembles the CL model form. This might well be the case at surfaces or in the solid regime, which we here confirm for a particular example of an iodine molecule in the atomic argon environment under high pressure. For this purpose we extend the recently proposed Fourier method for parameterizing linear generalized Langevin dynamics [J. Chem. Phys., 142, 244110 (2015)] to the non-linear case based on the CL model and perform an extensive error analysis. In order to judge on the applicability of this model in advance, we give handy empirical criteria and discuss the effect of the potential renormalization term. The obtained results provide evidence that the CL model can be used for describing a potentially broad class of systems.

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Quantum dynamics of hydrogen atoms on graphene. II. Sticking

Cited by 22 publications

References 49 publications

Classical and quantum dynamics at surfaces: Basic concepts from simple models

Classical and quantum dynamics at surfaces: Basic concepts from simple models

Quantum dynamics of hydrogen atoms on graphene. I. System-bath modeling

Vibrational spectroscopy via the Caldeira-Leggett model with anharmonic system potentials

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