Electron tunneling of photochemical reactions on metal surfaces: Nonequilibrium Green's function-density functional theory approach to photon energy dependence of reaction probability

Nakamura, Hisao; Yamashita, Koichi

doi:10.1063/1.1902946

Title: Electron tunneling of photochemical reactions on metal surfaces: Nonequilibrium Green's function-density functional theory approach to photon energy dependence of reaction probability

Full Record
Other Related Research

Abstract

We have developed a theoretical model of photoinduced reactions on metal surfaces initiated by the substrate/indirect excitation mechanism using the nonequilibrium Green's function approach. We focus on electron transfer, which consists of (1) electron-hole pair creation, (2) transport of created hot electrons, and (3) tunneling of hot electrons to form an anion resonance. We assume that steps (1), (2), and (3) are separable. By this assumption, the electron dynamics might be restated as a tunneling problem of an open system. Combining the Keldysh time-independent formalism with the simple transport theory introduced by Berglund and Spicer, we present a practical scheme for first-principle calculation of the reaction probability as a function of incident photon energy. The method is illustrated by application to the photoinduced desorption/dissociation of O{sub 2} on a Ag(110) surface by adopting density functional theory.

Authors:

Nakamura, Hisao; Yamashita, Koichi ^[1]

Department of Chemical System Engineering, Graduate School of Engineering, University of Tokyo, Tokyo 113-8656 (Japan)

Publication Date:: Sun May 15 00:00:00 EDT 2005

OSTI Identifier:: 20722927

Resource Type:: Journal Article

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 122; Journal Issue: 19; Other Information: DOI: 10.1063/1.1902946; (c) 2005 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606

Country of Publication:: United States

Language:: English

Subject:: 74 ATOMIC AND MOLECULAR PHYSICS; CHARGE EXCHANGE; DENSITY FUNCTIONAL METHOD; DISSOCIATION; ELECTRON TRANSFER; ELECTRONS; ENERGY DEPENDENCE; EXCITATION; GREEN FUNCTION; HOLES; PAIR PRODUCTION; PHOTOCHEMICAL REACTIONS; PHOTOCHEMISTRY; PHOTONS; REACTION KINETICS; SILVER; SURFACES; TRANSPORT THEORY; TUNNEL EFFECT

Citation Formats


                    Nakamura, Hisao, and Yamashita, Koichi. Electron tunneling of photochemical reactions on metal surfaces: Nonequilibrium Green's function-density functional theory approach to photon energy dependence of reaction probability.  United States: N. p., 2005. 
        Web.  doi:10.1063/1.1902946.

Copy to clipboard


                    Nakamura, Hisao, & Yamashita, Koichi. Electron tunneling of photochemical reactions on metal surfaces: Nonequilibrium Green's function-density functional theory approach to photon energy dependence of reaction probability.  United States.  https://doi.org/10.1063/1.1902946

Copy to clipboard


                    Nakamura, Hisao, and Yamashita, Koichi. 2005.  
        "Electron tunneling of photochemical reactions on metal surfaces: Nonequilibrium Green's function-density functional theory approach to photon energy dependence of reaction probability".  United States.  https://doi.org/10.1063/1.1902946.

Copy to clipboard


                    
@article{osti_20722927,

  title        = {Electron tunneling of photochemical reactions on metal surfaces: Nonequilibrium Green's function-density functional theory approach to photon energy dependence of reaction probability},

  author       = {Nakamura, Hisao and Yamashita, Koichi},

  abstractNote = {We have developed a theoretical model of photoinduced reactions on metal surfaces initiated by the substrate/indirect excitation mechanism using the nonequilibrium Green's function approach. We focus on electron transfer, which consists of (1) electron-hole pair creation, (2) transport of created hot electrons, and (3) tunneling of hot electrons to form an anion resonance. We assume that steps (1), (2), and (3) are separable. By this assumption, the electron dynamics might be restated as a tunneling problem of an open system. Combining the Keldysh time-independent formalism with the simple transport theory introduced by Berglund and Spicer, we present a practical scheme for first-principle calculation of the reaction probability as a function of incident photon energy. The method is illustrated by application to the photoinduced desorption/dissociation of O{sub 2} on a Ag(110) surface by adopting density functional theory.},

  doi          = {10.1063/1.1902946},

  url          = {https://www.osti.gov/biblio/20722927},
  journal      = {Journal of Chemical Physics},

  issn         = {0021-9606},

  number       = 19,

  volume       = 122,

  place        = {United States},

  year         = {Sun May 15 00:00:00 EDT 2005},

  month        = {Sun May 15 00:00:00 EDT 2005}

}

Copy to clipboard

Journal Article:

https://doi.org/10.1063/1.1902946

Other availability

Find in Google Scholar

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Similar records in OSTI.GOV collections:

Nonequilibrium functional bosonization of quantum wire networks

Journal Article Bagrets, Dmitry; Mirlin, Alexander - Annals of Physics (New York)

We develop a general approach to nonequilibrium nanostructures formed by one-dimensional channels coupled by tunnel junctions and/or by impurity scattering. The formalism is based on nonequilibrium version of functional bosonization. A central role in this approach is played by the Keldysh action that has a form reminiscent of the theory of full counting statistics. To proceed with evaluation of physical observables, we assume the weak-tunneling regime and develop a real-time instanton method. A detailed exposition of the formalism is supplemented by two important applications: (i) tunneling into a biased Luttinger liquid with an impurity, and (ii) quantum Hall Fabry-Perot interferometry.more »« less
https://doi.org/10.1016/J.AOP.2012.06.004
Finite bias spin dependent tunneling: A nonequilibrium Green{close_quote}s function approach

Journal Article Wang, X - Journal of Applied Physics

The nonequilibrium Green{close_quote}s function theory is applied to a model spin dependent tunneling system at finite bias. In the limit of zero bias, the present result agrees with that of Landauer{close_quote}s formula. For finite bias, it is found that as the bias increases, the magnetoresistance ratio decreases. {copyright} {ital 1998 American Institute of Physics.}
https://doi.org/10.1063/1.367648
Nonequilibrium spin transport through a diluted magnetic semiconductor quantum dot system with noncollinear magnetization

Journal Article Ma, Minjie; Tan, Seng - Annals of Physics (New York)

The spin-dependent transport through a diluted magnetic semiconductor quantum dot (QD) which is coupled via magnetic tunnel junctions to two ferromagnetic leads is studied theoretically. A noncollinear system is considered, where the QD is magnetized at an arbitrary angle with respect to the leads' magnetization. The tunneling current is calculated in the coherent regime via the Keldysh nonequilibrium Green's function (NEGF) formalism, incorporating the electron-electron interaction in the QD. We provide the first analytical solution for the Green's function of the noncollinear DMS quantum dot system, solved via the equation of motion method under Hartree-Fock approximation. The transport characteristics (chargemore »« less
https://doi.org/10.1016/J.AOP.2012.11.016
Hubbard Nonequilibrium Green’s Function Analysis of Photocurrent in Nitroazobenzene Molecular Junction

Journal Article Miwa, Kuniyuki; Najarian, Amin; McCreery, Richard; ... - Journal of Physical Chemistry Letters

We present a combined experimental and theoretical study of photoinduced current in molecular junctions consisting of monolayers of nitroazobenzene oligomers chemisorbed on carbon surfaces and illuminated by ultraviolet-visible light through a transparent electrode. Experimentally observed dependence of the photocurrent on light frequency, temperature, and monolayer thickness is analyzed within first-principles simulations employing the Hubbard nonequilibrium Green’s function diagrammatic technique. We reproduce qualitatively correct behavior and discuss mechanisms leading to the characteristic behavior of dark and photoinduced currents in response to changes in bias, frequency of radiation, temperature, and thickness of molecular layer.
Cited by 8
https://doi.org/10.1021/acs.jpclett.9b00270

Full Text Available
Efficient grid-based method in nonequilibrium Green's function calculations: Application to model atoms and molecules

Journal Article Balzer, K; Bauch, S; Bonitz, M - Physical Review. A

The finite-element discrete variable representation is proposed to express the nonequilibrium Green's function for strongly inhomogeneous quantum systems. This method is highly favorable against a general basis approach with regard to numerical complexity, memory resources, and computation time. Its flexibility also allows for an accurate representation of spatially extended Hamiltonians and thus opens the way toward a direct solution of the two-time Schwinger-Keldysh-Kadanoff-Baym equations on spatial grids, including, for example, the description of highly excited states in atoms. As benchmarks, we compute and characterize, in Hartree-Fock and second Born approximations, the ground states of the He atom, the H{sub 2}more »« less
https://doi.org/10.1103/PHYSREVA.81.022510

Similar Records