Charged two-exciton emission from a single semiconductor nanocrystal

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Here, we study the photoluminescence (PL) time trajectories of single CdSe/ZnS nanocrystals (NCs) as a function of the laser excitation power. At the low laser power, the PL intensity of a single NC switches between the “on” and “off” levels arising from the neutral and positively charged single excitons, respectively. With the increasing laser power, an intermediate “grey” level is formed due to the optical emission from a charged multiexciton state composed of two excitons and an extra electron. Both the inter-photon correlation and the PL decay measurements demonstrate that lifetime-indistinguishable photon pairs are emitted from this negatively charged two-exciton state.

ReferencesShowing 10 of 28 papers
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Evidence for the Role of Holes in Blinking: Negative and Oxidized CdSe/CdS Dots
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Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals
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Biexciton state causes photoluminescence fluctuations in CdSe/ZnS core/shell quantum dots at high photoexcitation densities
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Surface-Related Emission in Highly Luminescent CdSe Quantum Dots
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Exciton−Trion Transitions in Single CdSe–CdS Core–Shell Nanocrystals
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Studying Quantum Dot Blinking through the Addition of an Engineered Inorganic Hole Trap
  • May 21, 2013
  • ACS Nano
  • Ron Tenne + 5 more

CitationsShowing 4 of 4 papers
  • Open Access Icon
  • Research Article
  • Cite Count Icon 149
  • 10.1021/acs.nanolett.6b02874
Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion.
  • Oct 4, 2016
  • Nano Letters
  • Fengrui Hu + 8 more

Over the last two decades, intensive research efforts have been devoted to the suppressions of photoluminescence (PL) blinking and Auger recombination in metal-chalcogenide nanocrystals (NCs), with significant progresses being made only very recently in few specific NC structures. Here we show that nonblinking PL is readily available in the newly synthesized perovskite CsPbI3 NCs and that their Auger recombination of charged excitons is greatly slowed down, as signified by a PL lifetime about twice shorter than that of neutral excitons. Moreover, spectral diffusion is completely absent in single CsPbI3 NCs at the cryogenic temperature, leading to a resolution-limited PL line width of ∼200 μeV.

  • Research Article
  • Cite Count Icon 11
  • 10.1021/acs.jpclett.9b03009
Few-Layer PbI2 Nanoparticle: A 2D Semiconductor with Lateral Quantum Confinement.
  • Dec 3, 2019
  • The Journal of Physical Chemistry Letters
  • Jinqiu Liu + 6 more

Inspired by the superior optoelectronic performances of various 2D semiconductors, their new compositions and structures are being actively pursued in order to foster novel fundamental physics and device applications. As a layered semiconductor with a direct bandgap, few-layer PbI2 should have drawn much research attention due to their capability of emitting photons at short wavelengths of the visible spectrum. Here we chemically synthesize few-layer PbI2 flakes and nanoparticles, which demonstrate unique exciton properties that have rare counterparts in other 2D semiconductors. For three layers and more, the single PbI2 flakes can be utilized to show how the bandgap energy of a 2D semiconductor evolves with the changing layer thickness. The single PbI2 nanoparticles are associated with an ultranarrow photoluminescence line width of ∼1 meV, thus reflecting the influence of lateral quantum confinement on the energy-level structures of a 2D semiconductor. The above findings mark the emergence of a potent 2D platform that is more than complementary to well-studied transition-metal dichalcogenide monolayers.

  • Research Article
  • Cite Count Icon 3
  • 10.1039/d2nr00761d
Observation of high-density multi-excitons in medium-size CdSe/CdZnS/ZnS colloidal quantum dots through transient spectroscopy and their optical gain properties.
  • Jan 1, 2022
  • Nanoscale
  • Hongyu Yang + 8 more

Semiconductor quantum dots have extremely significant advantages in terms of optoelectronic devices. However, it is unfeasible to avoid the generation of charged exciton states during operation. Such states can change the radiation recombination rate and bring additional non-radiative Auger recombination channels. Herein, we synthesize high photoluminescence quantum yield medium-size CdSe/CdZnS/ZnS core/alloy shell/shell QDs. Their multiexciton spectra and dynamics were systematically studied by pump-power-dependent fluorescence blinking and time-correlated spectroscopy. The lifetimes of positively/negatively charged trions and biexcitons are estimated to be 0.74/6.1 and 0.16 ns, respectively. It demonstrated that the band-edge biexciton is influenced by the Coulomb interaction and Stark effect. The amplified spontaneous emission threshold is only 81 μJ cm-2 and can retain a long operation lifetime under continuous pumping. A vertical microcavity surface-emitting laser device is fabricated using these QDs. The coupling factor between the spontaneous emission and cavity mode is 0.81, which benefits the low stimulated emission threshold. This work provides a new perspective of the charged states in the multiexciton AR process in the QDs, implying a promising application prospect of such QDs as optical gain materials in "zero-threshold" laser fabrication.

  • Research Article
  • Cite Count Icon 20
  • 10.1021/acsnano.6b08040
Shell-Dependent Photoluminescence Studies Provide Mechanistic Insights into the Off-Grey-On Transitions of Blinking Quantum Dots.
  • Feb 27, 2017
  • ACS Nano
  • Feng Gao + 3 more

The majority of quantum dot (QD) blinking studies have used a model of switching between two distinct fluorescence intensity levels, "on" and "off". However, a distinct intermediate intensity level has been identified in some recent reports, a so-called "grey" or "dim" state, which has brought this binary model into question. While this grey state has been proposed to result from the formation of a trion, it is still unclear under which conditions it is present in a QD. By performing shell-dependent blinking studies on CdSe QDs, we report that the populations of the grey state and the on state are strongly dependent on both the shell material and its thickness. We found that adding a ZnS shell did not result in a significant population of the grey state. Using ZnSe as the shell material resulted in a slightly higher population of the grey state, although it was still poorly resolved. However, adding a CdS shell resulted in the population of a grey state, which depended strongly on its thickness up to 5 ML. Interestingly, while the frequency of transitions to and from the grey state showed a very strong dependence on CdS shell thickness, the brightness of and the dwell time in the grey state did not. Moreover, we found that the grey state acts as an on-pathway intermediate state between on and off states, with the thickness of the shell determining the transition probability between them. We also identified two types of blinking behavior in QDs, one that showed long-lived but lower intensity on states and another that showed short-lived but brighter on states that also depended on the shell thickness. Intensity-resolved single QD fluorescence lifetime analysis was used to identify the relationship between the various exciton decay pathways and the resulting intensity levels. We used this data to propose a model in which multiple on, grey, and off states exist whose equilibrium populations vary with time that give rise to the various intensity levels of single QDs and which depends on shell composition and thickness.

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