Photoexcited Ag ejection from a low-temperature He cluster: a simulation study by nonadiabatic Ehrenfest ring-polymer molecular dynamics

Literature Information

Publication Date 2017-05-03
DOI 10.1039/C7CP00888K
Impact Factor 3.676
Authors

Yusuke Seki, Toshiyuki Takayanagi, Motoyuki Shiga


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Abstract

Ring-polymer molecular dynamics (RPMD) simulations have been performed to understand the photoexcitation dynamics of an Ag atom embedded in a low-temperature cluster consisting of 500 helium atoms, after the electronic excitation 5p 2P1/2 ← 5p 2S1/2 and 5p 2P3/2 ← 5p 2S1/2 of the Ag atom. Along the RPMD trajectory the time evolution of electronic wavefunction within the spin–orbit 2P manifold is calculated, whereby the time-dependent Schrödinger equation and the RPMD equation of motion are coupled, using the à la Ehrenfest mean field approach. It is found from the simulations that the Ag atom is ejected from the helium cluster with the average time of 100 ps after photoexcitation with the average ejection velocity being 60–70 m s−1, which is roughly in line with experiment. Meanwhile it is also found that the present simulations do not agree with experiment as to the final state of the ejected Ag atom.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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