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Abstract Plasmonic hot‐electron‐assisted control of emission intensities and dynamics of CdSe/ZnS and infrared PbS quantum dots are studied. This is done by exploring the impact of Au/Si and Ag/Si Schottky junctions on the decay rates of such quantum dots when these junctions are placed in close vicinity of a Si/Al oxide charge barrier, forming metal‐oxide plasmonic metafilms. Such structures are used to investigate how metal‐dependent distributions of hot electrons and their capture via Schottky junctions can lead to suppression of the defect environments of quantum dots, offering a novel platform wherein off‐resonant (non‐Purcell) plasmonic processes are used to control exciton dynamics. These results show that Ag metafilms can enhance the emission of CdSe/ZnS quantum dots and elongate their lifetimes more than Au metafilms. This highlights the more efficient nature of Ag/Si Schottky junctions for hot electron excitation and capture. These results also show that such junctions can significantly suppress the nonradiative decay rates of PbS quantum dots at frequencies far from the plasmon resonances. These results demonstrate a field‐effect passivation of quantum dot defects via entrapment of hot electrons and control of emission intensities and dynamics of quantum dots via the nearly frequency‐independent electrostatic field of such electrons.
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Perspective on functional metal-oxide plasmonic metastructures
Plasmonic nanostructures and metasurfaces are appealing hosts for investigation of novel optical devices and exploration of new frontiers in physical/optical processes and materials research. Recent studies have shown that these structures hold the promise of greater control over the optical and electronic properties of quantum emitters, offering a unique horizon for ultra-fast spin-controlled optical devices, quantum computation, laser systems, and sensitive photodetectors. In this Perspective, we discuss how heterostructures consisting of metal oxides, metallic nanoantennas, and dielectrics can offer a material platform wherein one can use the decay of plasmons and their near fields to passivate the defect sites of semiconductor quantum dots while enhancing their radiative decay rates. Such a platform, called functional metal-oxide plasmonic metasubstrates (FMOPs), relies on formation of two junctions at very close vicinity of each other. These include an Au/Si Schottky junction and an Si/Al oxide charge barrier. Such a double junction allows one to use hot electrons to generate a field-passivation effect, preventing migration of photo-excited electrons from quantum dots to the defect sites. Prospects of FMOP, including impact of enhancement exciton–plasmon coupling, collective transport of excitation energy, and suppression of quantum dot fluorescence blinking, are discussed.
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- Award ID(s):
- 1917544
- PAR ID:
- 10398204
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- Journal of Applied Physics
- Volume:
- 133
- Issue:
- 7
- ISSN:
- 0021-8979
- Page Range / eLocation ID:
- Article No. 070901
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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