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Journal article
Critical Coupling of Visible Light Extends Hot-Electron Lifetimes for H2O2 Synthesis
ACS applied materials & interfaces, v 12(20), pp 22778-22788
20 May 2020
PMID: 32338494
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
Devices driven by above-equilibrium “hot” electrons are appealing for photocatalytic technologies, such as in situ H2O2 synthesis, but currently suffer from low (<1%) overall quantum efficiencies. Gold nanostructures excited by visible light generate hot electrons that can inject into a neighboring semiconductor to drive electrochemical reactions. Here, we designed and studied a metal–insulator–metal (MIM) structure of Au nanoparticles on a ZnO/TiO2/Al film stack, deposited through room-temperature, lithography-free methods. Light absorption, electron injection efficiency, and photocatalytic yield in this device are superior in comparison to the same stack without Al. Our device absorbs >60% of light at the Au localized surface plasmon resonance (LSPR) peak near 530 nma 5-fold enhancement in Au absorption due to critical coupling to an Al film. Furthermore, we show through ultrafast pump–probe spectroscopy that the Al-coupled samples exhibit a nearly 5-fold improvement in hot-electron injection efficiency as compared to a non-Al device, with the hot-electron lifetimes extending to >2 ps in devices photoexcited with fluence of 0.1 mJ cm−2. The use of an Al film also enhances the photocatalytic yield of H2O2 more than 3-fold in a visible-light-driven reactor. Altogether, we show that the critical coupling of Al films to Au nanoparticles is a low-cost, lithography-free method for improving visible-light capture, extending hot-carrier lifetimes, and ultimately increasing the rate of in situ H2O2 generation.
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Details
- Title
- Critical Coupling of Visible Light Extends Hot-Electron Lifetimes for H2O2 Synthesis
- Creators
- Daniel E Willis - Louisiana State UniversityMohammad M Taheri - Drexel UniversityOrhan Kizilkaya - Louisiana State University Center for Advanced Microstructures & Devices, Baton Rouge, Louisiana 70806, United StatesTiago R Leite - Louisiana State UniversityLaibao Zhang - Louisiana State UniversityTochukwu Ofoegbuna - Louisiana State UniversityKunlun Ding - Louisiana State UniversityJames A Dorman - Louisiana State UniversityJason B Baxter - Drexel UniversityKevin M McPeak - Louisiana State University
- Publication Details
- ACS applied materials & interfaces, v 12(20), pp 22778-22788
- Publisher
- American Chemical Society; Washington, DC
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering
- Web of Science ID
- WOS:000537394100037
- Scopus ID
- 2-s2.0-85085533146
- Other Identifier
- 991019168988804721
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InCites Highlights
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Materials Science, Multidisciplinary
- Nanoscience & Nanotechnology