Redefining near-unity luminescence in quantum dots with photothermal threshold quantum yield

Hanifi, David; Bronstein, Noah D.; Koscher, Brent A.; Nett, Zach; Swabeck, Joseph K.; Takano, Kaori; Schwartzberg, Adam M.; Maserati, Lorenzo; Vandewal, Koen; Burgt, Yoeri van de; Salleo, Alberto; Alivisatos, A. Paul

doi:10.1126/science.aat3803

Cited by 219 publications

(257 citation statements)

References 30 publications

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“…the situation where recombination is predominantly radiative in nature [17]. Approaching the radiative limit was so far only possible in III-V materials [18][19][20][21] or in low conductivity quantum dot films [22] but not in solution-processed, three dimensional semiconductors. Better understanding the fundamental reasons for the observed properties of halide perovskites would therefore be highly valuable [23,24].…”

Section: Introductionmentioning

confidence: 99%

Effect of reabsorption and photon recycling on photoluminescence spectra and transients in lead-halide perovskite crystals

et al. 2020

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Explaining the time-dependent evolution of photoluminescence spectra of halide perovskite single crystals after pulsed excitation requires the consideration of a range of physical mechanisms, including electronic transport, recombination and reabsorption. The latter process of reabsorption and regeneration of electron-hole pairs from a photon created by radiative recombination in the single crystal itself is termed photon recycling and has been a highly controversial topic. We use photoluminescence experiments performed under different illumination conditions combined with numerical simulations that consider photon recycling to show which parameters affect temporal decays, spectral shifts and differences in the illumination direction. In addition, we use numerical simulations with and without photon recycling to understand the relative importance of chargecarrier transport and photon recycling. We conclude that under most relevant illumination conditions and times after the pulse, electronic transport is more important than photon recycling for the spectral behavior of the transients. However, inclusion of photon recycling is imperative for the understanding of the absolute density of electrons and holes present in the crystal during a certain time after the pulse.

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Section: Introductionmentioning

confidence: 99%

Effect of reabsorption and photon recycling on photoluminescence spectra and transients in lead-halide perovskite crystals

et al. 2020

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“…olloidal quantum dots (QDs) are solution-processable semiconductor nanocrystals coated with a monolayer of surface ligands 1 . Progresses on synthetic chemistry of core/shell QDs have led to a unique class of emissive materials with efficient, stable, and high colour-purity photoluminescence properties [2][3][4][5][6] . Electroluminescence of the core/shell QDs is expected to harness the unique combination of their superior photoluminescence properties and excellent solution processability, enabling high-performance and cost-effective QD lightemitting-diodes (QLEDs), electrically driven single-photon sources, and potentially electrically pumped lasers [7][8][9][10][11][12][13][14][15][16][17] .…”

mentioning

confidence: 99%

Electrochemically-stable ligands bridge the photoluminescence-electroluminescence gap of quantum dots

et al. 2020

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Colloidal quantum dots are promising emitters for quantum-dot-based light-emitting-diodes. Though quantum dots have been synthesized with efficient, stable, and high colour-purity photoluminescence, inheriting their superior luminescent properties in light-emitting-diodes remains challenging. This is commonly attributed to unbalanced charge injection and/or interfacial exciton quenching in the devices. Here, a general but previously overlooked degradation channel in light-emitting-diodes, i.e., operando electrochemical reactions of surface ligands with injected charge carriers, is identified. We develop a strategy of applying electrochemically-inert ligands to quantum dots with excellent luminescent properties to bridge their photoluminescence-electroluminescence gap. This material-design principle is general for boosting electroluminescence efficiency and lifetime of the light-emitting-diodes, resulting in record-long operational lifetimes for both red-emitting light-emitting-diodes (T 95 > 3800 h at 1000 cd m −2) and blue-emitting light-emitting-diodes (T 50 > 10,000 h at 100 cd m −2). Our study provides a critical guideline for the quantum dots to be used in optoelectronic and electronic devices.

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“…The second approach uses a fluorophore or molecular probe that is visible by both fluorescence imaging and another imaging modality, such as TEM and SEM. Examples include quantum dots (Hanifi et al, 2019), which can be conjugated to antibodies (Giepmans et al, 2005;Killingsworth and Bobryshev, 2016;Peckys and de Jonge, 2015), and a fluorophore and a gold cluster conjugated to antibodies (FluoroNanogold) (Takizawa et al, 2015). This approach has multiple variants.…”

Section: Methods For Spatial Registration In Correlative Microscopymentioning

confidence: 99%

Correlating cell function and morphology by performing fluorescent immunocytochemical staining on the light-microscope stage

Kawano

Kakazu

Iwabuchi

et al. 2020

Preprint

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ABSTRACTBackgroundCorrelation of fluorescence signals from functional changes in live cells with those from immunocytochemical indicators of their morphology following chemical fixation can be highly informative with regard to function-structure relationship. Such analyses can be technically challenging because they need consistently aligning the images between imaging sessions. Existing solutions include introducing artificial spatial landmarks and modifying the microscopes. However, these methods can require extensive changes to the experimental systems.New methodHere we introduce a simple approach for aligning images. It is based on two procedures: performing immunocytochemistry while a specimen stays on a microscope stage (on-stage), and aligning images using biological structures as landmarks after they are observed with transmitted-light optics in combination with fluorescence-filter sets.ResultsWe imaged a transient functional signal from a fluorescent Ca2+ indicator, and mapped it to neurites based on immunocytochemical staining of a structural marker. In the same preparation, we could identify presynaptically silent synapses, based on a lack of labeling with an indicator for synaptic vesicle recycling and on positive immunocytochemical staining for a structural marker of nerve terminals. On-stage immunocytochemistry minimized lateral translations and eliminated rotations, and transmitted-light images of neurites were sufficiently clear to enable spatial registration, effective at a single-pixel level.Comparison with existing methodsThis method aligned images with minimal change or investment in the experimental systems.ConclusionsThis method facilitates information retrieval across multiple imaging sessions, even when functional signals are transient or local, and when fluorescent signals in multiple imaging sessions do not match spatially.

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Redefining near-unity luminescence in quantum dots with photothermal threshold quantum yield

Cited by 219 publications

References 30 publications

Effect of reabsorption and photon recycling on photoluminescence spectra and transients in lead-halide perovskite crystals

Effect of reabsorption and photon recycling on photoluminescence spectra and transients in lead-halide perovskite crystals

Electrochemically-stable ligands bridge the photoluminescence-electroluminescence gap of quantum dots

Correlating cell function and morphology by performing fluorescent immunocytochemical staining on the light-microscope stage

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