The detection of hot electrons and understanding the correlation between hot electron generation and surface phenomena are challenging questions in the surface science and catalysis community. Hot electron flow generated on a gold thin film by photon absorption (or internal photoemission) appears to be correlated with localized surface plasmon resonance.<br/>In this talk, I will show strategy to quantify the non-adiabatic energy transfer and detect hot electron flux during the elementary steps of the surface reactions occurring at solid-gas and solid-liquid interfaces. To detect and utilize the hot electron flows, the nanodiodes consisting of metal catalyst film, semiconductor layers, and Ohmic contact pads were constructed It was shown that the chemicurrent or hot electron flows were well correlated with the turnover rate of CO oxidation or hydrogen oxidation separately measured by gas chromatography, suggesting the intrinsic relation between catalytic reaction and hot electron generation. We show a novel scheme of graphene catalytic nanodiode composed of a Pt NPs array on graphene/TiO<sub>2</sub> Schottky nanodiode, which allows detection of hot electron flows induced by hydrogen oxidation on Pt NPs. By analyzing the correlation between the turnover rate (catalytic activity) and hot electron current (chemicurrent) measured on the graphene catalytic nanodiodes, we demonstrate that the catalytic nanodiodes utilizing a single graphene layer for electrical connection of Pt NPs are beneficial for the detection of hot electrons due to not only atomically thin nature of graphene but also reducing the height of the potential barrier existing at the Pt NPs/graphene interface. I will that hot electron flow generated on a gold thin film by photon absorption (or internal photoemission) is amplified by localized surface plasmon resonance. We report results obtained using metal/n-Si nanodiodes which show creation and transfer of hot electrons in the course of a catalytic decomposition of aqueous hydrogen peroxide (H2O2) on the surface of Ag, Pt and Au catalysts. The chemicurrent yield, the number of hot electrons detected per oxygen molecules, reaches values up to 0.1. Finally, The effect of surface plasmons on the catalytic and photocatalytic activity on metal–oxide hybrid nanocatalysts is also highlighted. These phenomena imply the efficient energy conversion from the photon energy to the chemical energy, with the potential application of hot electron-based photocatalytic devices.

Hot electron-mediated surface chemistry on solid-gas and solid-liquid interfaces

253rd National Meeting (2017)

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