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Colloidal semiconductor nanocrystals (NCs) have emerged as promising candidates for developing solutionprocessable optical gain media with potential applications in integrated photonic circuits and lasers. However, the deployment of NCs in these technologies has been hindered by the nonradiative Auger recombination of multiexciton states, which shortens the optical gain lifetime and reduces its spectral range. Here, we demonstrate that these limitations can be overcome by using giant colloidal quantum shells (g-QSs), comprising a quantum-confined CdSe shell grown over a large (∼14 nm) CdS bulk core. Such bulk-nanoscale architecture minimizes exciton− exciton interactions, leading to suppressed Auger recombination and one of the broadest gain bandwidths reported for colloidal nanomaterials, spanning energies both above and, remarkably, below the bandgap. Ultrafast transient absorption and photoluminescence measurements demonstrate that the high-energy portion of optical gain arises from states containing more than 15 excitons per particle, while the unusual sub-bandgap gain behavior results from an Auger-assisted radiative recombination, a mechanism that has traditionally been viewed as a loss pathway. Collectively, these results reveal a unique gain regime associated with bulk-nanocrystal hybrid systems, which offers a promising path toward solution-processable light sources.
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Low-threshold laser medium utilizing semiconductor nanoshell quantum dots
Colloidal semiconductor nanocrystals (NCs) represent a promising class of nanomaterials for lasing applications. Currently, one of the key challenges facing the development of high-performance NC optical gain media lies in enhancing the lifetime of biexciton populations. This usually requires the employment of charge-delocalizing particle architectures, such as core/shell NCs, nanorods, and nanoplatelets. Here, we report on a two-dimensional nanoshell quantum dot (QD) morphology that enables a strong delocalization of photoinduced charges, leading to enhanced biexciton lifetimes and low lasing thresholds. A unique combination of a large exciton volume and a smoothed potential gradient across interfaces of the reported CdS bulk /CdSe/CdS shell (core/shell/shell) nanoshell QDs results in strong suppression of Auger processes, which was manifested in this work though the observation of stable amplified stimulated emission (ASE) at low pump fluences. An extensive charge delocalization in nanoshell QDs was confirmed by transient absorption measurements, showing that the presence of a bulk-size core in CdS bulk /CdSe/CdS shell QDs reduces exciton–exciton interactions. Overall, present findings demonstrate unique advantages of the nanoshell QD architecture as a promising optical gain medium in solid-state lighting and lasing applications.
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- Award ID(s):
- 1710063
- PAR ID:
- 10283086
- Date Published:
- Journal Name:
- Nanoscale
- Volume:
- 12
- Issue:
- 33
- ISSN:
- 2040-3364
- Page Range / eLocation ID:
- 17426 to 17436
- 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/10.1039/D0NR03582C
