Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.205
Publication date: 28th August 2024
Monocrystalline plasmonic nanostructures (e.g. Au, Ag, Cu, and Al) because of their well-defined crystallographic surfaces and low ohmic losses exhibit unique optical [1] and catalytic [2] properties, rendering them promising candidate catalysts for photo-electrochemistry and solar fuel production [3]. Importantly, high-definition monocrystalline nanostructures with well-controlled optical absorption characteristics can be used to obtain a fundamental understanding of the role of hot carriers in plasmonic photocatalysis [4]. However, despite many studies on the optical properties of high-definition monocrystalline gold (Au) nano-antennas, photocatalytic performance of these array structures has not been studied so far due to the challenges associated with fabricating cm-scale array structures and the incapability of the conventional photoelectrochemical systems in detecting signals from tiny reactions on um-scale array structures. In this work, we report on light-assisted scanning electrochemical microscopy (photo-SECM) studies of a series of um-scale Au nano-antenna arrays fabricated by electron beam lithography on high-aspect ratio Au micro-flakes [5] on a TiO2 and p-GaN semiconducting substrates [6,7]. Photo-SECM experiments were performed to quantify the wavelength-dependent photochemical response and internal quantum efficiency of the plasmonic-redox molecule systems. Combining experimental data with numerical/ab-initio modelling, we disentangled the roles of hot carrier generation, transport, and injection at both solid/solid and solid/liquid interfaces. We determined the energy-dependent injection efficiency of hot carriers and identified their transfer mechanisms at the metal/electrolyte interface, proving that they are highly impacted by the metal/molecule interaction. We discovered a tunneling hole transfer to the molecule in the Au/TiO2 photoanode and a combination of tunneling and direct electron transfer to the molecule in the Au/p-GaN photoanode systems. This work provides an unprecedented understanding of the interplay of hot-carrier-driven processes, shedding light on the important mechanisms governing the transport and injection of hot carriers across interfaces in hot-carrier-driven photocatalytic systems.
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