An official website of the United States government
Quantum information processing demands efficient quantum light sources (QLS) capable of producing high-fidelity single photons or entangled photon pairs. Single epitaxial quantum dots (QDs) have long been proven to be efficient sources of deterministic single photons; however, their production via molecular-beam epitaxy presents scalability challenges. Conversely, colloidal semiconductor QDs offer scalable solution processing and tunable photoluminescence but suffer from broader linewidths and unstable emissions. This leads to spectrally inseparable emission from exciton (X) and biexciton (XX) states, complicating the production of single photons and triggered photon pairs. Here, we demonstrate that colloidal semiconductor quantum shells (QSs) achieve significant spectral separation (~ 75-80 meV) and long temporal stability of X and XX emissive states, enabling the observation of exciton-biexciton bunching in colloidal QDs. Our low-temperature single-particle measurements show cascaded XX-X emission of single photon pairs for over 200 seconds, with minimal overlap between X and XX features. The X-XX distinguishability allows for an in-depth theoretical characterization of cross-correlation strength, placing it in perspective with photon pairs of epitaxial counterparts. These findings highlight a strong potential of semiconductor quantum shells for applications in quantum information processing.
more »
« less
Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells
Quantum shells combine large two-photon cross-sections, long biexciton lifetimes, wide gain bandwidth, to produce stable, multimodal upconverted lasers.
more »
« less
- Award ID(s):
- 2208834
- PAR ID:
- 10509389
- Publisher / Repository:
- Nanoscale
- Date Published:
- Journal Name:
- Nanoscale
- Volume:
- 15
- Issue:
- 45
- ISSN:
- 2040-3364
- Page Range / eLocation ID:
- 18415 to 18422
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Arranging semiconducting nanocrystals into ordered superstructures is a promising platform to study fundamental light-matter interactions and develop programmable optical metamaterials. We investigated how the geometrical arrangement of CdS nanocrystals in hierarchical assemblies affects chiroptical properties. To create these structures, we controlled the evaporation of a colloidal CdS nanocrystal solution between two parallel plates. We combined in situ microscopy and computational modeling to establish a formation mechanism involving the shear-induced alignment of nanocrystal fibers and the subsequent mechanical relaxation of the stretched fibers to form Raman noodle–type band textures. The high linear anisotropy in these films shares many similarities with cholesteric liquid crystals. The films deposited on top and bottom surfaces exhibit opposite chirality. The mechanistic insights from this study are consequential to enable future advances in the design and fabrication of programmable optical metamaterials for further development of polarization-based optics toward applications in sensing, hyperspectral imaging, and quantum information technology.more » « less
-
Abstract Recent advances in device design and process optimizations have enabled the production of CdTe devices on flexible substrates, but the necessary high‐temperature processing (>450 °C) to recrystallize grains limits the use of alternative lightweight substrates. Here, a new synthesis method is reported to create a freestanding CdS/CdTe film by combining high‐temperature depositions (CdS/CdTe on Si/SiO2) and a simple lift‐off process in a water environment at room temperature. Analysis of the results indicate that the delamination is facilitated by the innate lattice mismatch as well as the presence of an unexpected Te‐rich layer (≈20 nm), which accumulates on the SiO2surface. High‐resolution electron microscopy and spectroscopy measurements confirm that the CdS/CdTe film is physically liberated from the substrate without leaving any residue, while also preserving their initial structural and compositional properties.more » « less
-
Isomerization, the process by which a molecule is coherently transformed into another molecule with the same molecular formula but a different atomic structure, is an important and well-known phenomenon of organic chemistry, but has only recently been observed for inorganic nanoclusters. Previously, CdS nanoclusters were found to isomerize between two end point structures rapidly and reversibly (the α-phase and β-phase), mediated by hydroxyl groups on the surface. This observation raised many significant structural and pathway questions. One critical question is why no intermediate states were observed during the isomerization; it is not obvious why an atomic cluster should only have two stable end points rather than multiple intermediate arrangements. In this study, we report that the use of amide functional groups can stabilize intermediate phases during the transformation of CdS magic-size clusters between the α-phase and the β-phase. When treated with amides in organic solvents, the amides not only facilitate the α-phase to β-phase isomerization but also exhibit three distinct excitonic features, which we call the β340-phase, β350-phase, and β367-phase. Based on pair distribution function analysis, these intermediates strongly resemble the β-phase structure but deviate greatly from the α-phase structure. All phases (β340-phase, β350-phase, and β367-phase) have nearly identical structures to the β-phase, with the β340-phase having the largest deviation. Despite these intermediates having similar atomic structures, they have up to a 583 meV difference in band gap compared to the β-phase. Kinetic studies show that the isomers and intermediates follow a traditional progression in the thermodynamic stability of β340-phase/β350-phase < α-phase < β367-phase < β-phase. The solvent identity and polarity play a crucial role in kinetically arresting these intermediates. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy studies paired with simple density functional theory calculations reveal that the likely mechanism is due to the multifunctional nature of the amides that form an amphoteric surface binding bond motif, which promotes a change in the carboxylic acid binding mode. This change from chelating binding modes to bridging binding modes initiates the isomerization. We propose that the carbonyl group is responsible for the direct interaction with the surface, acting as an L-type ligand which then pulls electron density away from the electron-poor nitrogen site, enabling them to interact with the carboxylate ligands and initiate the change in the binding mode. The isomerization of CdS nanoclusters continues to be a topic of interest, giving insight into fundamental nanoscale chemistry and physics.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/D3NR04203K
