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Abstract Due to their ability to strongly modify the local optical field through the excitation of surface plasmon polaritons (SPPs), plasmonic nanostructures are often used to reshape the emission direction and enhance the radiative decay rate of quantum emitters, such as semiconductor quantum dots (QDs). These features are essential for quantum information processing, nanoscale photonic circuitry, and optoelectronics. However, the modification and enhancement demonstrated thus far have typically led to drastic alterations of the local energy density of the emitters, and hence their intrinsic optical properties, leaving little room for active control. Here, dynamic tuning of the energy states of a single semiconductor QD is demonstrated by optically modifying its local dielectric environment with a nearby plasmonic structure, instead of directly coupling it to the QD. This technique leaves intact the intrinsic optical properties of the QD, while enabling a reversible all‐optical control mechanism that operates below the diffraction limit at low power levels.
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Ultrafast Symmetry Control in Photoexcited Quantum Dots
Abstract Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X‐ray scattering, in conjunction with atomic‐scale structural modeling and first‐principles calculations, it is revealed that symmetry‐broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off‐centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red‐shifts in the symmetry‐restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.
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- PAR ID:
- 10556719
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 37
- Issue:
- 4
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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