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Abstract Quantum dots encompass a broad spectrum of optical, catalytic, and electrochemical properties bringing in novel applications in catalysis, imaging, displays, and optoelectronics. Herein, the unanticipated broad‐spectrum light absorption and high fluorescence quantum yield in fluorinated boron nitride (FBN) quantum dots are discussed. A heterostructure of FBN quantum dots with a wide‐bandgap semiconductor, titania nanotube arrays, exhibits high photocatalytic activity as evidenced by high external quantum efficiency extending from ultraviolet to green region of the solar spectrum (≈24% at 400 nm). The high activity is confirmed using photoelectrochemical hydrogen evolution experiments. Further, it is demonstrated that high fluorescence quantum yield could be tapped for the detection of glycolytic activity in cancer cells compared to normal cells. This finding could shift the paradigm of molecular detection using quantum dots. The 0D structure and the gap states introduced through fluorination are believed to be responsible for these unprecedented characteristics of boron nitride.
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Metasurface-enhanced photochemical activity in visible light absorbing semiconductors
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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- Award ID(s):
- 2112550
- PAR ID:
- 10534429
- Publisher / Repository:
- The Journal of Chemical Physics
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 160
- Issue:
- 14
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1063/5.0199589
