Room-Temperature Ordered Photon Emission from Multiexciton States in Single CdSe Core-Shell Nanocrystals

Fisher, Brent; Caruge, Jean-Michel; Zehnder, Don; Bawendi, Moungi G.

doi:10.1103/physrevlett.94.087403

Cited by 172 publications

(240 citation statements)

References 24 publications

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“…Although the PL blinking effect was completely suppressed in most of the single CsPbI 3 NCs excited at low power, it was triggered in all of the single CsPbI 3 NCs studied in our experiment with high-power excitation due to the formation of charged excitons from the multi-exciton ionization process [9,25]. In Fig.…”

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confidence: 72%

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Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion

et al. 2016

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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 several specific heterostructures. Here we show that nonblinking PL is readily available in the newly-synthesized perovskite CsPbI 3 (cesium lead iodide) NCs, and 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 CsPbI 3 NCs at the cryogenic temperature, leading to a resolution-limited PL linewidth of ~200 μeV.

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confidence: 72%

“…For regular metal-chalcogenide NCs (e.g., CdSe), the Auger processes of multi-excitons and charged excitons normally occur at the sub-nanosecond timescale [2], much shorter than the radiative lifetime of tens of nanoseconds for single neutral excitons [3].…”

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confidence: 99%

Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion

et al. 2016

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“…Auger process in colloidal nanocrystals is at the origin of single-photon emission 4,14 and it is suggested to be involved in blinking process 11,15,16 in such structures. Auger effect is a three-charge process in which the recombination energy of an electron-hole pair is transferred to an additional charge.…”

Section: Introductionmentioning

confidence: 99%

“…Wet-chemically synthesized colloidal core/shell nanocrystals (NCs) have been shown to emit nonclassical light at room temperature [1][2][3][4] making them suitable for applications in the field of quantum optics. Among colloidal NCs, CdSe/CdS dot-in-rods (DRs) made up by a spherical core of CdSe surrounded by a rod-like shell of CdS 5 have interesting features as single photon emitters such as a high degree of linear polarization [6][7][8][9][10] and a strongly reduced emission intermittency (non-blinking emission) when synthesized with thick CdS shells 11 .…”

Section: Introductionmentioning

confidence: 99%

Effect of charging on CdSe/CdS dot-in-rods single-photon emission

et al. 2014

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The photon statistics of CdSe/CdS dot-in-rods nanocrystals is studied with a method involving post-selection of the photon detection events based on the photoluminescence count rate. We show that flickering between two states needs to be taken into account to interpret the single-photon emission properties. With post-selection we are able to identify two emitting states: the exciton and the charged exciton (trion), characterized by different lifetimes and different second order correlation functions. Measurements of the second order autocorrelation function at zero delay with postselection shows a degradation of the single photon emission for CdSe/CdS dot-in-rods in a charged state that we explain by deriving the neutral and charged biexciton quantum yields.

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“…As the lowest level is a dark state [3,4], we calculate E 10 from the radiative lifetime obtained from the long component of the kinetics together with the quantum yield, obtaining E 10 ≈ 0.02 · A 01 . Using relative multiexciton emission strengths from literature data [5] and extrapolation we obtain A n,n+1 for n = 1 to 4 and recalculate these to absorption cross sections.…”

Section: Calculation Of Absorption Cross Sections For N-excitonsmentioning

confidence: 99%

Multiexciton Absorption Cross Sections of CdSe Nanocrystals at Band-Edge Energy

Lenngren

Garting

Zheng

et al. 2013

EPJ Web of Conferences

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Abstract.Picosecond transient absorption signals of two kinds of cadmium selenide quantum dots were measured at various excitation intensities. The average number of excitons per quantum dot was calculated from a Poisson model, which together with kinetic parameters was used to determine exciton population kinetics. Exciton and multiexciton absorption cross sections were determined and analyzed in terms of the electronic states of the quantum dots. BackgroundSemiconductor nanocrystals, called quantum dots (QDs), are attracting broad scientific attention both from fundamental and applied research. The interest is related to the intriguing opto-electronic properties of QDs, such as quantized energy levels and size-tunable bandgap. The effects are due to quantum confinement, occurring if the size of the QD is similar or smaller than the exciton Bohr radius.In the context of solar energy, the potential of QDs in breaking the Shockley-Queisser thermodynamic limit via multiple exciton generation (MEG) is particularly attractive. However, the reported yields of the process are contradictory, and understanding of the basic principles is still obscure. The process is commonly described in terms of impact ionization where multiple excitons are generated in a sequential process. The observed dynamics are very fast -within the time resolution of the experiments carried out so far (50 fs) multiple excitons are formed.MEG yields are usually determined from the relative amplitude of the characteristic fast multiexciton component of the band edge photoemission or photobleaching dynamics. For quantitative analyses one needs to have a good knowledge of the oscillator strengths of the transitions which contribute to the signal. As a preparation for quantitative analysis of MEG yields, we analyze transient absorption at the band edge to determine absorption cross sections for multiple excitons. ExperimentalTwo kinds of QDs were used: CdSe QDs with diameter 5 nm (Lumidot, Sigma-Aldrich, called core QDs in the following) and core-shell (CdSe)ZnS QDs with core diameter 3 nm (synthesized by us, called core-shell QDs in the following). The pump pulse intensity, denoted in the text as factors of a reference intensity I 0 , was varied by using neutral density filters. After the pump pulse, a probe pulse interacted with the sample providing transient absorption (TA) traces on a subpicosecond to EPJ Web of Conferences

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Room-Temperature Ordered Photon Emission from Multiexciton States in Single CdSe Core-Shell Nanocrystals

Cited by 172 publications

References 24 publications

Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion

Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion

Effect of charging on CdSe/CdS dot-in-rods single-photon emission

Multiexciton Absorption Cross Sections of CdSe Nanocrystals at Band-Edge Energy

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