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Electronic Excitation on Surfaces During Chemical and Photon Processes

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Current Trends of Surface Science and Catalysis

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Abstract

Energy dissipation at surfaces and interfaces is mediated by excitation of elementary processes, including phonons and electronic excitation, once external energy is deposited to the surface during exothermic chemical processes [1–4]. Electron excitation in exothermic catalytic reactions or the incidence of photons on metal surfaces results in the flow of high-energy electrons with an energy of 1–3 eV, assuming that most of the chemical or photon energy is converted to electron flow on a short (femtosecond) time scale before atomic vibration adiabatically dissipates the energy (in picoseconds). These energetic electrons that are not in thermal equilibrium with the metal atoms are called “hot electrons” [5–8]. There have been a number of studies demonstrating the influence of hot electrons on atomic and molecular processes. The detection of hot electron flow under atomic or molecular processes and understanding its role in chemical reactions have been major topics in surface chemistry. Recent experimental and theoretical studies have demonstrated electronic excitation produced during atomic or molecular processes on surfaces [9, 10]. In this chapter, I will outline recent research developing energy conversion devices based on hot electrons. The chemicurrent, or hot electron flows, is well correlated with the turnover rate of CO oxidation or hydrogen oxidation measured separately by gas chromatography, suggesting an intrinsic relation between the catalytic reactions and hot electron generation. We found that photon energy can be directly converted to hot electron flow through the metal–semiconductor interface of catalytic nanodiodes. We showed that hot electron flow generated on a gold thin film by photon absorption (or internal photoemission) is amplified by localized surface plasmon resonance. The influence of the flow of hot charge carriers on the chemistry at the oxide–metal interface and the turnover rate for the chemical reaction, for the cases of Pt–CaSe–Pt nanodumbbells and Pt/GaN substrates, are discussed.

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Acknowledgments

The work was supported by the WCU (World Class University, R-31-2008-000-10055-0) program, and 2012R1A2A1A01009249 through the National Research Foundation (NRF) funded by the Ministry of Education, Science and Technology (MEST) and by the Research Center Program (CA1201) of IBS (Institute for Basic Science) of Republic of Korea.

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  1. Graduate School of EEWS (WCU) and NanoCentury KI, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 305-701, South Korea

    Jeong Young Park

  2. Center for Nanomaterials and Chemical Reactions, Institute for Basic Science, Daejeon, 305-701, South Korea

    Jeong Young Park

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    Jeong Young Park

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Park, J.Y. (2014). Electronic Excitation on Surfaces During Chemical and Photon Processes. In: Park, J. (eds) Current Trends of Surface Science and Catalysis., vol 1. Springer, New York, NY. https://doi.org/10.1007/978-1-4614-8742-5_10

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