Modulating hydrogen diffusion on metal surfaces by nonadiabatic transitions
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TL;DR: In this paper, a nonadiabatic model was proposed based on the classical mapping theory to introduce multistate couplings in addition to the bare surface diffusion, and the simulation results showed that the diffusion constant of H atom could be enhanced by a factor of 2-6 in the temperature range of T = 500-600 K.
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Abstract: Nonadiabatic transitions may be used as a promising tool for dynamical control. However how it could be applied to and affect surface diffusion remains largely unexplored. Here a nonadiabatic model was proposed based on the classical mapping theory to introduce multistate couplings in addition to the bare surface diffusion. By performing nonadiabatic molecular dynamics simulation on a benchmark system of atomic hydrogen diffusion on the Cu (001) surface, it is demonstrated that nonadiabatic transitions could modulate diffusion dynamics in a robust way, i.e. either suppressing or promoting it. Depending on the design for the coupling regime in the nonadiabatic model, simulation results show that aside for the nonadiabatic damping effect, the diffusion constant of H atom could be enhanced by a factor of 2-6 in the temperature range of T = 500-600 K. The effect of nonadiabatic transitions may provide an explanation to the significant discrepancy between experimental measured diffusion constant and previous theoretical predictions. By highlighting the role of nonadiabatic effects, in particular under nonequilibrium conditions, this work sheds light on the development of new molecular control schemes for practical applications.
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Citations
Tunable Product Selectivity in Electrochemical CO2 Reduction on Well-Mixed Ni-Cu Alloys.
TL;DR: In this article, a random solid solution of Cu1-xNix alloy catalysts is presented to enable a systematic modulation of adsorption energies, leading to an increase of hydrogen evolution with the Ni content.
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Atomic diffusion at the Ni–Ti liquid interface using molecular dynamics simulations
Rizal Arifin,Yoyok Winardi,Yoga Arob Wicaksono,Lucky Poriwikawa,Darminto,Ali Selamat,Wawan Trisnadi Putra,Muhammad Malyadi +7 more
TL;DR: In this article , the authors performed molecular dynamics simulations for 1 ns to investigate the diffusion process of Ni-Ti liquid at temperatures of 2000, 2200, 2400, and 2600 K.
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Nonadiabatic Dynamics of Hydrogen Diffusion on Cu(001): Classical Mapping Model with Multistate Projection Window in Real Space
TL;DR: A new nonadiabatic multistate model for surface diffusion based on a real space decomposition scheme by generalizing the classical mapping theory of Meyer and Miller is proposed.
References
Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations
Georgios Kyriakou,Matthew B. Boucher,April D. Jewell,Emily A. Lewis,Timothy J. Lawton,Ashleigh E. Baber,Heather L. Tierney,Maria Flytzani-Stephanopoulos,E. Charles H. Sykes +8 more
TL;DR: Desorption measurements in combination with high-resolution scanning tunneling microscopy show that individual, isolated Pd atoms in a Cu surface substantially lower the energy barrier to both hydrogen uptake on and subsequent desorption from the Cu metal surface.
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Attosecond real-time observation of electron tunnelling in atoms
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TL;DR: The real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling is reported, and the process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds, suggesting a new technique, attose Cond Tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution.
988
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