Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids

Rowland, Clare E.; Fedin, Igor; Zhang, Hui; Gray, Stephen K.; Govorov, Alexander O.; Talapin, Dmitri V.; Schaller, Richard D.

doi:10.1038/nmat4231

Cited by 220 publications

(361 citation statements)

References 29 publications

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“…The pictures shown in Fig. 205,206 Particularly, under higher excitation densities the fast ET suppress efficiently fluorescence quenching by Auger recombination, thus enabling more efficient collection of multiple excitons by the acceptor layers. This thickness dependence of the ET rate is completely counterintuitive as compared to that of the QD-graphene system discussed above, in which the ET rate is enhanced with the increase in the number of graphene layers.…”

Section: Et Involving 2d Materialsmentioning

confidence: 99%

Recent advances in energy transfer in bulk and nanoscale luminescent materials: from spectroscopy to applications

2015

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Transfer of energy occurs endlessly in our universe by means of radiation. Compared to energy transfer (ET) in free space, in solid state materials the transfer of energy occurs in a rather confined manner, which is usually mediated by real or virtual particles, including not only photons, but also electrons, phonons, and excitons. In the present review, we discuss the recent advances in optical ET by resonance mediated with photons in solid materials as well as their nanoscale counterparts, with focus on the photoluminescence behavior pertaining to ET between optically active centers, such as rare earth (RE) ions. This review begins with a brief discussion on the classification of optical ET together with an overview of the theoretical formulations and experimental method for the examination of ET. We will then present a comprehensive discussion on the ET in practical systems in which normal photoluminescence, upconversion and quantum cutting resulted from ET involving metal ions, QDs, organic species, 2D materials and plasmonic nanostructures. Diverse ET systems are therefore simply categorized into cases of ion-ion interactions and non-ion interactions. Special attention has been paid to the progress in the manipulation of spatially confined ET in nanostructured systems including core-shell structures, as well as the ET in multiple exciton generation found in QDs and organic molecules, which behave quite similarly to resonance ET between metal ion centers. Afterwards, we will discuss the broad spectrum of applications of ET in the aforementioned systems, including solid state lighting, solar energy utilization, bio-imaging and diagnosis, and sensing. In the closing part, along with a short summary, we discuss further research focus regarding the problems and possible future directions of optical ET in solids.

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Section: Et Involving 2d Materialsmentioning

confidence: 99%

Recent advances in energy transfer in bulk and nanoscale luminescent materials: from spectroscopy to applications

2015

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“…Yet, the shifts also introduce sensitivity to the exact lateral width, which is less controllable than the thickness, and hence give rise to increased linewidths. The latter effect could be detrimental, e.g., for energy-transfer processes [12].…”

Section: A Core-only Nplsmentioning

confidence: 99%

Excitons in core-only, core-shell and core-crown CdSe nanoplatelets: Interplay between in-plane electron-hole correlation, spatial confinement, and dielectric confinement

2017

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Using semianalytical models we calculate the energy, effective Bohr radius, and radiative lifetime of neutral excitons confined in CdSe colloidal nanoplatelets (NPLs). The excitonic properties are largely governed by the electron-hole in-plane correlation, which in NPLs is enhanced by the quasi-two-dimensional motion and the dielectric mismatch with the organic environment. In NPLs with lateral size L 20 nm the exciton behavior is essentially that in a quantum well, with super-radiance leading to exciton lifetimes of 1 ps or less, only limited by the NPL area. However, for L < 20 nm excitons enter an intermediate confinement regime, hence departing from the quantum well behavior. In heterostructured NPLs, a different response is observed for core-shell and core-crown configurations. In the former, the strong vertical confinement limits separation of electrons and holes even for type-II band alignment. The exciton behavior is then similar to that in core-only NPL, albeit with weakened dielectric effects. In the latter, charge separation is also inefficient if band alignment is quasi-type-II (e.g., in CdSe/CdS), because electron-hole interaction drives both carriers into the core. However, it becomes very efficient for type-II alignment, for which we predict exciton lifetimes reaching microseconds.

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“…14,15 From a fundamental viewpoint, colloidal semiconductor nanosheets provide an ideal 2D model system to investigate 1D quantum confinement, surface chemistry, and 2D NC growth mechanism, etc. [20][21][22][23] Recently, lead halide perovskites have attracted substantial attention because of their excellent optoelectronic properties. 15 Significantly, the as-synthesized CdSe nanosheets are found to exhibit superior optical properties originating from their unique 2D geometry, including extreme color purity, high photoluminescence (PL) quantum yield (QY), and fast radiative lifetime.…”

Section: Introductionmentioning

confidence: 99%

Generalized colloidal synthesis of high-quality, two-dimensional cesium lead halide perovskite nanosheets and their applications in photodetectors

et al. 2016

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All-inorganic cesium lead halide perovskite (CsPbX3, X = Cl, Br, and I) nanocrystals (NCs) are emerging as an important class of semiconductor materials with superior photophysical properties and wide potential applications in optoelectronic devices. So far, only a few studies have been conducted to control the shape and geometry of CsPbX3 NCs. Here we report a general approach to directly synthesize two-dimensional (2D) CsPbX3 perovskite and mixed perovskite nanosheets with uniform and ultrathin thicknesses down to a few monolayers. The key to the high-yield synthesis of perovskite nanosheets is the development of a new Cs-oleate precursor. The as-synthesized CsPbX3 nanosheets exhibit bright photoluminescence with broad wavelength tunability by composition modulation. The excellent optoelectronic properties of CsPbX3 nanosheets combined with their unique 2D geometry and large lateral dimensions make them ideal building blocks for building functional devices. To demonstrate their potential applications in optoelectronics, photodetectors based on CsPbBr3 nanosheets are fabricated, which exhibit high on/off ratios with a fast response time.

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Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids

Cited by 220 publications

References 29 publications

Recent advances in energy transfer in bulk and nanoscale luminescent materials: from spectroscopy to applications

Recent advances in energy transfer in bulk and nanoscale luminescent materials: from spectroscopy to applications

Excitons in core-only, core-shell and core-crown CdSe nanoplatelets: Interplay between in-plane electron-hole correlation, spatial confinement, and dielectric confinement

Generalized colloidal synthesis of high-quality, two-dimensional cesium lead halide perovskite nanosheets and their applications in photodetectors

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