Heterogeneous photocatalysis is an important research problem relevant to a variety of sustainable energy technologies. However, obtaining high photocatalytic efficiency from visible light absorbing semiconductors is challenging due to a combination of weak absorption, transport losses, and low activity. Aspects of this problem have been addressed by multilayer approaches, which provide a general scheme for engineering surface reactivity and stability independent of electronic considerations. However, an analogous broad framework for optimizing light–matter interactions has not yet been demonstrated. Here, we establish a photonic approach using semiconductor metasurfaces that is highly effective in enhancing the photocatalytic activity of GaAs, a high-performance semiconductor with a near-infrared bandgap. Our engineered pillar arrays with heights of ∼150 nm exhibit Mie resonances near 700 nm that result in near-unity absorption and exhibit a field profile that maximizes charge carrier generation near the solid–liquid interface, enabling short transport distances. Our hybrid metasurface photoanodes facilitate oxygen evolution and exhibit enhanced incident photon-to-current efficiencies that are ∼22× larger than a corresponding thin film for resonant excitation and 3× larger for white light illumination. Key to these improvements is the preferential generation of photogenerated carriers near the semiconductor interface that results from the field enhancement profile of magnetic dipolar-type modes.
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14 April 2024
Research Article|
April 15 2024
Metasurface-enhanced photochemical activity in visible light absorbing semiconductors
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Festschrift in honor of Louis E. Brus
Yamuna Paudel;
Yamuna Paudel
(Conceptualization, Formal analysis, Investigation, Methodology, Visualization, Writing – original draft)
1
Photonics Initiative, Advanced Science Research Center, City University of New York
, New York, New York 10031, USA
2
Physics Department, CUNY Graduate Center, City University of New York
, New York, New York 10016, USA
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Diego J. Chachayma-Farfan;
Diego J. Chachayma-Farfan
(Formal analysis, Investigation, Writing – review & editing)
1
Photonics Initiative, Advanced Science Research Center, City University of New York
, New York, New York 10031, USA
3
Department of Electrical and Computer Engineering, The University of Texas at Austin
, Austin, Texas 78712, USA
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Andrea Alù
;
Andrea Alù
(Conceptualization, Formal analysis, Supervision, Writing – review & editing)
1
Photonics Initiative, Advanced Science Research Center, City University of New York
, New York, New York 10031, USA
2
Physics Department, CUNY Graduate Center, City University of New York
, New York, New York 10016, USA
3
Department of Electrical and Computer Engineering, The University of Texas at Austin
, Austin, Texas 78712, USA
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Matthew Y. Sfeir
Matthew Y. Sfeir
a)
(Conceptualization, Formal analysis, Funding acquisition, Investigation, Methodology, Supervision, Visualization, Writing – original draft)
1
Photonics Initiative, Advanced Science Research Center, City University of New York
, New York, New York 10031, USA
2
Physics Department, CUNY Graduate Center, City University of New York
, New York, New York 10016, USA
a)Author to whom correspondence should be addressed: [email protected]
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Yamuna Paudel
1,2
Diego J. Chachayma-Farfan
1,3
Andrea Alù
1,2,3
Matthew Y. Sfeir
1,2,a)
1
Photonics Initiative, Advanced Science Research Center, City University of New York
, New York, New York 10031, USA
2
Physics Department, CUNY Graduate Center, City University of New York
, New York, New York 10016, USA
3
Department of Electrical and Computer Engineering, The University of Texas at Austin
, Austin, Texas 78712, USA
a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 160, 144710 (2024)
Article history
Received:
January 23 2024
Accepted:
March 25 2024
Citation
Yamuna Paudel, Diego J. Chachayma-Farfan, Andrea Alù, Matthew Y. Sfeir; Metasurface-enhanced photochemical activity in visible light absorbing semiconductors. J. Chem. Phys. 14 April 2024; 160 (14): 144710. https://doi.org/10.1063/5.0199589
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