skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Amplified Spontaneous Emission from Electron–Hole Quantum Droplets in Colloidal CdSe Nanoplatelets
Two-dimensional cadmium selenide nanoplatelets (NPLs) exhibit large absorption cross sections and homogeneously broadened band-edge transitions that offer utility in wide-ranging optoelectronic applications. Here, we examine the temperature-dependence of amplified spontaneous emission (ASE) in 4- and 5-monolayer thick NPLs and show that the threshold for close-packed (neat) films decreases with decreasing temperature by a factor of 2–10 relative to ambient temperature owing to extrinsic (trapping) and intrinsic (phonon-derived line width) factors. Interestingly, for pump intensities that exceed the ASE threshold, we find development of intense emission to lower energy in particular provided that the film temperature is ≤200 K. For NPLs diluted in an inert polymer, both biexcitonic ASE and low-energy emission are suppressed, suggesting that described neat-film observables rely upon high chromophore density and rapid, collective processes. Transient emission spectra reveal ultrafast red-shifting with the time of the lower energy emission. Taken together, these findings indicate a previously unreported process of amplified stimulated emission from polyexciton states that is consistent with quantum droplets and constitutes a form of exciton condensate. For studied samples, quantum droplets form provided that roughly 17 meV or less of thermal energy is available, which we hypothesize relates to polyexciton binding energy. Polyexciton ASE can produce pump-fluence-tunable red-shifted ASE even 120 meV lower in energy than biexciton ASE. Our findings convey the importance of biexciton and polyexciton populations in nanoplatelets and show that quantum droplets can exhibit light amplification at significantly lower photon energies than biexcitonic ASE.  more » « less
Award ID(s):
1808590
PAR ID:
10561598
Author(s) / Creator(s):
; ; ; ; ; ;
Publisher / Repository:
American Chemical Society
Date Published:
Journal Name:
ACS Nano
Volume:
18
Issue:
13
ISSN:
1936-0851
Page Range / eLocation ID:
9605 to 9612
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; (, Nano Letters)
    Colloidal PbS/PbCl2 core/shell nanoplatelets were synthesized via wet-chemical methods using lead oleate and lead chloride as lead precursors. The resulting heterostructures consist of a PbS core, a PbCl2 shell, and an intermediate layer of lead sulfochloride alloy. These nanoplatelets exhibit a photoluminescence quantum yield of approximately 20%, nearly an order of magnitude higher than that of unshelled PbS nanoplatelets. Cyclic voltammetry measurements reveal a type-I band alignment between the core and shell. Despite the presence of strong attractive biexciton Auger recombination, as observed in transient absorption spectroscopy, the nanoplatelets achieve amplified spontaneous emission at a low pump threshold of 76 μJ cm–2. Their large lateral dimensions support the spatial distribution of multiple excitons, including repulsive biexcitons, enabling efficient light amplification. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, Nanoscale)
    null (Ed.)
    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. 
    more » « less
  3. ; (, Chemical Science)
    Cadmium chalcogenide nanoplatelets (NPLs) and their heterostructures have been reported to have low gain thresholds and large gain coefficients, showing great potential for lasing applications. However, the further improvement of the optical gain properties of NPLs is hindered by a lack of models that can account for their optical gain characteristics and predict their dependence on the properties (such as lateral size, concentration, and/or optical density). Herein, we report a systematic study of optical gain (OG) in 4-monolayer thick CdSe NPLs by both transient absorption spectroscopy study of colloidal solutions and amplified spontaneous emission (ASE) measurement of thin films. We showed that comparing samples with the same optical density at the excitation, the OG threshold is not dependent of the NPL lateral area, while the saturation gain amplitude is dependent on the NPL lateral area when comparing samples with the same optical density at the excitation wavelength. Both the OG and ASE thresholds increase with the optical density at the excitation wavelength for samples of the same NPL thickness and lateral area. We proposed an OG model for NPLs that can successfully account for the observed lateral area and optical density dependences. The model reveals that OG originates from stimulated emission from the bi-exciton states and the OG threshold is reached when the average number of excitons per NPL is about half the occupation of the band-edge exciton states. The model can also rationalize the much lower OG thresholds in the NPLs compared to QDs. This work provides a microscopic understanding of the dependence of the OG properties on the morphology of the colloidal nanocrystals and important guidance for the rational optimization of the lasing performance of NPLs and other 1- and 2-dimensional nanocrystals. 
    more » « less
  4. ; ; ; ; ; ; ; ; ; ; et al (, The Journal of Chemical Physics)
    The generation of exciton–polaritons through strong light–matter interactions represents an emerging platform for exploring quantum phenomena. A significant challenge in colloidal nanocrystal-based polaritonic systems is the ability to operate at room temperature with high fidelity. Here, we demonstrate the generation of room-temperature exciton–polaritons through the coupling of CdSe nanoplatelets (NPLs) with a Fabry–Pérot optical cavity, leading to a Rabi splitting of 74.6 meV. Quantum–classical calculations accurately predict the complex dynamics between the many dark state excitons and the optically allowed polariton states, including the experimentally observed lower polariton photoluminescence emission, and the concentration of photoluminescence intensities at higher in-plane momenta as the cavity becomes more negatively detuned. The Rabi splitting measured at 5 K is similar to that at 300 K, validating the feasibility of the temperature-independent operation of this polaritonic system. Overall, these results show that CdSe NPLs are an excellent material to facilitate the development of room-temperature quantum technologies. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; ; et al (, Advanced Energy Materials)
    Abstract Metal halide perovskite nanocrystals (NCs) have emerged as highly promising light emitting materials for various applications, ranging from perovskite light‐emitting diodes (PeLEDs) to lasers and radiation detectors. While remarkable progress has been achieved in highly efficient and stable green, red, and infrared perovskite NCs, obtaining efficient and stable blue‐emitting perovskite NCs remains a great challenge. Here, a facile synthetic approach for the preparation of blue emitting CsPbBr3nanoplatelets (NPLs) with treatment by an organic sulfate is reported, 2,2‐(ethylenedioxy) bis(ethylammonium) sulfate (EDBESO4), which exhibit remarkably enhanced photoluminescence quantum efficiency (PLQE) and stability as compared to pristine CsPbBr3NPLs coated with oleylamines. The PLQE is improved from ≈28% for pristine CsPbBr3NPLs to 85% for EDBESO4treated CsPbBr3NPLs. Detailed structural characterizations reveal that EDBESO4treatment leads to surface passivation of CsPbBr3NPLs by both EDBE2+and SO42–ions, which helps to prevent the coalescence of NPLs and suppress the degradation of NPLs. A simple proof‐of‐concept device with emission peaked at 462 nm exhibits an external quantum efficiency of 1.77% with a luminance of 691 cd m−2and a half‐lifetime of 20 min, which represents one of the brightest pure blue PeLEDs based on NPLs reported to date. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email