Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots.
Ontology highlight
ABSTRACT:
SUBMITTER: Lubin G
PROVIDER: S-EPMC8397400 | biostudies-literature |
REPOSITORIES: biostudies-literature
Similar Datasets
Project description:We have measured the intrinsic exciton dephasing in high-quality zinc blende CdSe/CdS colloidal quantum dots in the temperature range from 5 to 170 K using a sensitive three-beam photon echo technique in heterodyne detection, which is not affected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing. From the temperature dependence of the zero-phonon line dephasing, the exciton lifetime, and the exciton thermalization within its fine structure, we show that the zero-phonon line dephasing of the lowest bright state originates from the phonon-assisted spin-flip to dark exciton states. Importantly, we can control the dephasing by tailoring the exciton fine structure through its dependence on the dot core size and shell thickness, as expected from the spin-flip mechanism. By reducing the electron-hole exchange interaction with increasing core size and delocalization of the electron wave function in the quasi-type-II core/shell band alignment, we find the longest zero-phonon line dephasing time of ?110 ps at 5 K in dots with the largest core diameter (5.7 nm) and the thickest CdSe shell (9 monolayers) in the series studied.
| S-EPMC3590878 | biostudies-other
Project description:We investigate the photoluminescence (PL) spectra and the time-resolved PL decay process from colloidal quantum dots on SiN/SiO2 wet etched via BOE (HF:NH4F:H2O). The spectrum displays multi-peak shapes that vary with irradiation time. The evolution of the spectral peaks with irradiation time and collection angle demonstrates that the strong coupling of the charged-exciton emission to the leaky modes of the SiN/SiO2 slab waveguide predominantly produces short-wavelength spectral peaks, resulting in multi-peak spectra. We conclude that BOE etching enhances the charged-exciton emission efficiency and its contribution to the total emission compared with the unetched case. BOE etching smoothes the electron confinement potential, thus decreasing the Auger recombination rate. Therefore, the charged-exciton emission efficiency is high, and the charged-exciton-polariton emission can be further enhanced through strong coupling to the leaky mode of the slab waveguide.
| S-EPMC4437026 | biostudies-literature
Project description:We report a single molecule detection scheme to investigate excitation spectra of single emitters at room temperature. We demonstrate the potential of single emitter photoluminescence excitation spectroscopy by recording excitation spectra of single CdSe nanocrystals over a wide spectral range of 100 nm. The spectra exhibit emission intermittency, characteristic of single emitters. We observe large variations in the spectra close to the band edge, which represent the individual heterogeneity of the observed quantum dots. We also find specific excitation wavelengths for which the single quantum dots analyzed show an increased propensity for a transition to a long-lived dark state. We expect that the additional capability of recording excitation spectra at room temperature from single emitters will enable insights into the photophysics of emitters that so far have remained inaccessible.
| S-EPMC3190622 | biostudies-literature
Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.
| S-EPMC4879659 | biostudies-other
Project description:Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single-quantum dot light-emitting diodes. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than 12 electrons and 1 hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot photodynamics, with an observed 210-fold increase in the decay rate, accompanied by 12-fold decrease in the emission intensity, while preserving single-photon emission characteristics. These results pave the way for deterministic control over the charge state, and room-temperature decay rate engineering for colloidal quantum dot-based classical and quantum communication technologies.
| S-EPMC7500932 | biostudies-literature
Project description:Understanding multiple-exciton generation (MEG) in quantum dots (QDs) requires in-depth measurements of transient exciton dynamics. Because MEG typically faces competing ultrafast energy-loss intra-band relaxation, it is of central importance to investigate the emerging time-scale of the MEG kinetics. Here, we present ultrafast spectroscopic measurements of the MEG in PbS QDs via probing the ground-state biexciton transients. Specifically, we directly compare the biexciton spectra with the single-exciton ones before and after the intra-band relaxation. Early emergence of MEG is evidenced by observing transient Stark shift and quasi-instantaneous linewidth broadening, both of which take place before the intra-band relaxation. Photon-density-dependent study shows that the broadened biexciton linewidth strongly depends on the MEG-induced extra-exciton generation. Long after the intra-band relaxation, the biexciton broadening is small and the single-exciton state filling is dominant.
| S-EPMC3826098 | biostudies-other
Project description:Despite recent advances, the synthesis of colloidal InSb quantum dots (QDs) remains underdeveloped, mostly due to the lack of suitable precursors. In this work, we use Lewis acid-base interactions between Sb(III) and In(III) species formed at room temperature in situ from commercially available compounds (viz., InCl3, Sb[NMe2]3 and a primary alkylamine) to obtain InSb adduct complexes. These complexes are successfully used as precursors for the synthesis of colloidal InSb QDs ranging from 2.8 to 18.2 nm in diameter by fast coreduction at sufficiently high temperatures (≥230 °C). Our findings allow us to propose a formation mechanism for the QDs synthesized in our work, which is based on a nonclassical nucleation event, followed by aggregative growth. This yields ensembles with multimodal size distributions, which can be fractionated in subensembles with relatively narrow polydispersity by postsynthetic size fractionation. InSb QDs with diameters below 7.0 nm have the zinc blende crystal structure, while ensembles of larger QDs (≥10 nm) consist of a mixture of wurtzite and zinc blende QDs. The QDs exhibit photoluminescence with small Stokes shifts and short radiative lifetimes, implying that the emission is due to band-edge recombination and that the direct nature of the bandgap of bulk InSb is preserved in InSb QDs. Finally, we constructed a sizing curve correlating the peak position of the lowest energy absorption transition with the QD diameters, which shows that the band gap of colloidal InSb QDs increases with size reduction following a 1/d dependence.
| S-EPMC7596776 | biostudies-literature
Project description:Colloidal quantum dots (CQDs) are highly promising materials for light amplification thanks to their efficient photoluminescence, tunable emission wavelength and low-cost synthesis. Unfortunately, CQDs are suffering from band-edge state degeneracy which demands multiple excitons to achieve population inversion. As a result, non-radiative Auger recombination increases the lasing threshold and limits the gain lifetime. Here, benefiting from the negative charging, we demonstrate that the amplified spontaneous emission (ASE) threshold is controllable in a device where CQD film is exposed to an external electric field. Specifically, singly charged CQDs lower the threshold due to the preexisting electron in the conduction band, while strongly enhanced Auger recombination in doubly charged CQDs stymies the ASE. Experimental results and kinetic equation model show that ASE threshold reduces 10% even if our device only charges ~17% of the CQD population. Our results open new possibilities for controlling exciton recombination dynamics and achieving electrically pumped CQD lasers.
| S-EPMC6814376 | biostudies-literature
Project description:Minimizing decoherence due to coupling of a quantum system to its fluctuating environment is at the forefront of quantum information and photonics research. Nature sets the ultimate limit, however, given by the strength of the system's coupling to the electromagnetic field. Here, we establish the ability to electronically control this coupling and enhance the optical coherence time of the charged exciton transition in quantum dots embedded in a photonic waveguide. By manipulating the electronic wave functions through an applied lateral electric field, we increase the coherence time from ?1.4 to ?2.7??ns. Numerical calculations reveal that longer coherence arises from the separation of charge carriers by up to ?6??nm, which leads to a 30% weaker transition dipole moment. The ability to electronically control the coherence time opens new avenues for quantum communication and novel coupling schemes between distant qubits.
| S-EPMC4822415 | biostudies-literature
Project description:Excitonics, an alternative to romising for processing information since semiconductor electronics is rapidly approaching the end of Moore's law. Currently, the development of excitonic devices, where exciton flow is controlled, is mainly focused on electric-field modulation or exciton polaritons in high-Q cavities. Here, we show an all-optical strategy to manipulate the exciton flow in a binary colloidal quantum well complex through mediation of the Förster resonance energy transfer (FRET) by stimulated emission. In the spontaneous emission regime, FRET naturally occurs between a donor and an acceptor. In contrast, upon stronger excitation, the ultrafast consumption of excitons by stimulated emission effectively engineers the excitonic flow from the donors to the acceptors. Specifically, the acceptors' stimulated emission significantly accelerates the exciton flow, while the donors' stimulated emission almost stops this process. On this basis, a FRET-coupled rate equation model is derived to understand the controllable exciton flow using the density of the excited donors and the unexcited acceptors. The results will provide an effective all-optical route for realizing excitonic devices under room temperature operation.
| S-EPMC7046609 | biostudies-literature