Showing papers on "Quantum dot published in 2015"
TL;DR: The compelling combination of enhanced optical properties and chemical robustness makes CsPbX3 nanocrystals appealing for optoelectronic applications, particularly for blue and green spectral regions (410–530 nm), where typical metal chalcogenide-based quantum dots suffer from photodegradation.
Abstract: Metal halides perovskites, such as hybrid organic–inorganic CH3NH3PbI3, are newcomer optoelectronic materials that have attracted enormous attention as solution-deposited absorbing layers in solar cells with power conversion efficiencies reaching 20%. Herein we demonstrate a new avenue for halide perovskites by designing highly luminescent perovskite-based colloidal quantum dot materials. We have synthesized monodisperse colloidal nanocubes (4–15 nm edge lengths) of fully inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I or mixed halide systems Cl/Br and Br/I) using inexpensive commercial precursors. Through compositional modulations and quantum size-effects, the bandgap energies and emission spectra are readily tunable over the entire visible spectral region of 410–700 nm. The photoluminescence of CsPbX3 nanocrystals is characterized by narrow emission line-widths of 12–42 nm, wide color gamut covering up to 140% of the NTSC color standard, high quantum yields of up to 90%, and radiativ...
6,170 citations
TL;DR: The demonstration of these novel quantum-dot light-emitting diodes based on all-inorganic perovskite CsPbX3 (X = Cl, Br, I) nanocrystals opens a new avenue toward designing optoelectronic devices, such as displays, photodetectors, solar cells, and lasers.
Abstract: Novel quantum-dot light-emitting diodes based on all-inorganic perovskite CsPbX3 (X = Cl, Br, I) nanocrystals are reported. The well-dispersed, single-crystal quantum dots (QDs) exhibit high quantum yields, and tunable light emission wavelength. The demonstration of these novel perovskite QDs opens a new avenue toward designing optoelectronic devices, such as displays, photodetectors, solar cells, and lasers.
2,311 citations
TL;DR: The actual mechanism of photoluminescence (PL) of fluorescent carbon dots (CDs) is still an open debate among researchers as mentioned in this paper, and three types of fluorescent CDs were involved: graphene quantum dots (GQDs), carbon nanodots (CNDs), and polymer dots (PDs).
Abstract: At present, the actual mechanism of the photoluminescence (PL) of fluorescent carbon dots (CDs) is still an open debate among researchers. Because of the variety of CDs, it is highly important to summarize the PL mechanism for these kinds of carbon materials; doing so can guide the development of effective synthesis routes and novel applications. This review will focus on the PL mechanism of CDs. Three types of fluorescent CDs were involved: graphene quantum dots (GQDs), carbon nanodots (CNDs), and polymer dots (PDs). Four reasonable PL mechanisms have been confirmed: the quantum confinement effect or conjugated π-domains, which are determined by the carbon core; the surface state, which is determined by hybridization of the carbon backbone and the connected chemical groups; the molecule state, which is determined solely by the fluorescent molecules connected on the surface or interior of the CDs; and the crosslink-enhanced emission (CEE) effect. To give a thorough summary, the category and synthesis routes, as well as the chemical/physical properties for the CDs, are briefly introduced in advance.
1,987 citations
TL;DR: A ligand-assisted reprecipitation strategy is developed to fabricate brightly luminescent and color-tunable colloidal CH3NH3PbX3 quantum dots with absolute quantum yield up to 70% at room temperature and low excitation fluencies, expected to exhibit interesting nanoscale excitonic properties.
Abstract: Organometal halide perovskites are inexpensive materials with desirable characteristics of color-tunable and narrow-band emissions for lighting and display technology, but they suffer from low photoluminescence quantum yields at low excitation fluencies. Here we developed a ligand-assisted reprecipitation strategy to fabricate brightly luminescent and color-tunable colloidal CH3NH3PbX3 (X = Br, I, Cl) quantum dots with absolute quantum yield up to 70% at room temperature and low excitation fluencies. To illustrate the photoluminescence enhancements in these quantum dots, we conducted comprehensive composition and surface characterizations and determined the time- and temperature-dependent photoluminescence spectra. Comparisons between small-sized CH3NH3PbBr3 quantum dots (average diameter 3.3 nm) and corresponding micrometer-sized bulk particles (2–8 μm) suggest that the intense increased photoluminescence quantum yield originates from the increase of exciton binding energy due to size reduction as well a...
1,756 citations
TL;DR: An overview of the theoretical principles involved, as well as applications ranging from high-precision quantum electrodynamics experiments to quantum-information processing can be found in this paper.
Abstract: Quantum dots embedded in photonics nanostructures provide unprecedented control over the interaction between light and matter. This review gives an overview of the theoretical principles involved, as well as applications ranging from high-precision quantum electrodynamics experiments to quantum-information processing.
1,240 citations
TL;DR: All-inorganic colloidal cesium lead halide perovskite quantum dots are revealed to be a new class of favorable optical-gain materials, which show combined merits of both colloidal quantum dots and halideperovskites.
Abstract: All-inorganic colloidal cesium lead halide perovskite quantum dots (CsPbX3 , X = Cl, Br, I) are revealed to be a new class of favorable optical-gain materials, which show -combined merits of both colloidal quantum dots and halide perovskites. Low-threshold and -ultrastable stimulated emission is -demonstrated under atmospheric conditions with wavelength tunability across the whole -visible spectrum via either size or composition control.
1,047 citations
TL;DR: This paper presents a meta-modelling system that automates the very labor-intensive and therefore time-heavy and expensive and therefore expensive and expensive process of designing and installing solar panels.
Abstract: Graham H. Carey,† Ahmed L. Abdelhady,‡ Zhijun Ning, Susanna M. Thon, Osman M. Bakr,‡ and Edward H. Sargent*,† †Department of Electrical and Computer Engineering, University of Toronto, 10 King’s College Road, Toronto, Ontario M5S 3G4, Canada ‡Division of Physical Sciences and Engineering, Solar & Photovoltaics Engineering Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia School of Physical Science and Technology, ShanghaiTech University, 100 Haike Road, Shanghai 201210, China Department of Electrical and Computer Engineering, Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States
1,036 citations
TL;DR: This work highlights the advantages in both ensemble and single-nanocrystal PL of colloidal CsPbBr3 nanocrystals (NCs) over the traditional cQDs and investigates batch-to-batch reproducibility of NCs exhibiting PL peaks within ±1 nm.
Abstract: Traditional CdSe-based colloidal quantum dots (cQDs) have interesting photoluminescence (PL) properties. Herein we highlight the advantages in both ensemble and single-nanocrystal PL of colloidal CsPbBr3 nanocrystals (NCs) over the traditional cQDs. An ensemble of colloidal CsPbBr3 NCs (11 nm) exhibits ca. 90 % PL quantum yield with narrow (FWHM=86 meV) spectral width. Interestingly, the spectral width of a single-NC and an ensemble are almost identical, ruling out the problem of size-distribution in PL broadening. Eliminating this problem leads to a negligible influence of self-absorption and Forster resonance energy transfer, along with batch-to-batch reproducibility of NCs exhibiting PL peaks within ±1 nm. Also, PL peak positions do not alter with measurement temperature in the range of 25 to 100 °C. Importantly, CsPbBr3 NCs exhibit suppressed PL blinking with ca. 90 % of the individual NCs remain mostly emissive (on-time >85 %), without much influence of excitation power.
917 citations
TL;DR: In this paper, a red, green and blue quantum-dot LEDs are realized by customizing the nanostructure of the quantum dots. But their performance was not as good as those of traditional LEDs.
Abstract: Bright, efficient red, green and blue quantum-dot LEDs are realized by customizing the nanostructure of the quantum dots.
832 citations
TL;DR: In this paper, optical micro-spectroscopy studies of thin layers of tungsten diselenide (WSe2), a representative semiconducting dichalcogenide with a bandgap in the visible spectral range.
Abstract: Single photon emitters can form at the interfaces between layers of WSe2. Crystal structure imperfections in solids often act as efficient carrier trapping centres, which, when suitably isolated, act as sources of single photon emission. The best known examples of such attractive imperfections are well-width or composition fluctuations in semiconductor heterostructures1,2 (resulting in the formation of quantum dots) and coloured centres in wide-bandgap materials such as diamond3,4,5. In the recently investigated thin films of layered compounds, the crystal imperfections may logically be expected to appear at the edges of commonly investigated few-layer flakes of these materials exfoliated on alien substrates. Here, we report comprehensive optical micro-spectroscopy studies of thin layers of tungsten diselenide (WSe2), a representative semiconducting dichalcogenide with a bandgap in the visible spectral range. At the edges of WSe2 flakes (transferred onto Si/SiO2 substrates) we discover centres that, at low temperatures, give rise to sharp emission lines (100 μeV linewidth). These narrow emission lines reveal the effect of photon antibunching, the unambiguous attribute of single photon emitters. The optical response of these emitters is inherently linked to the two-dimensional properties of the WSe2 monolayer, as they both give rise to luminescence in the same energy range, have nearly identical excitation spectra and have very similar, characteristically large Zeeman effects. With advances in the structural control of edge imperfections, thin films of WSe2 may provide added functionalities that are relevant for the domain of quantum optoelectronics.
778 citations
TL;DR: In this article, a zero-dimensional photonic quantum emitters can be realized using defects in the two-dimensional dichalcogenides, which can be used to construct a two dimensional quantum emitter.
Abstract: Zero-dimensional photonic quantum emitters can be realized using defects in the two-dimensional dichalcogenides.
TL;DR: In this article, uniform molybdenum disulfide (MoS2)/tungsten disulfides (WS2) quantum dots are synthesized by the combination of sonication and solvothermal treatment of bulk MoS2/WS2 at a mild temperature.
Abstract: In this work, uniform molybdenum disulfide (MoS2)/tungsten disulfide (WS2) quantum dots are synthesized by the combination of sonication and solvothermal treatment of bulk MoS2/WS2 at a mild temperature. The resulting products possess monolayer thickness with an average size about 3 nm. The highly exfoliated and defect-rich structure renders these quantum dots plentiful active sites for the catalysis of hydrogen evolution reaction (HER). The MoS2 quantum dots exhibit a small HER overpotential of ≈120 mV and long-term durability. Moreover, the strong fluorescence, good cell permeability, and low cytotoxicity make them promising and biocompatible probes for in vitro imaging. In addition, this work may provide an alternative facile approach to synthesize the quantum dots of transition metal dichalcogenides or other layered materials on a large scale.
TL;DR: A hybrid phototransistor consisting of colloidal PbS quantum dots and few layers of MoS2 (≥2 layers) is demonstrated and shows responsivity of up to 10(6) A W(-1) and backgate-dependent sensitivity.
Abstract: A hybrid phototransistor consisting of colloidal PbS quantum dots and few layers of MoS2 (≥2 layers) is demonstrated. The hybrid benefits from tailored light absorption in the quantum dots throughout the visible/near infrared region, efficient charge-carrier separation at the p-n interface, and fast carrier transport through the MoS2 channel. It shows responsivity of up to 10(6) A W(-1) and backgate-dependent sensitivity.
TL;DR: ZMOF-derived ZnO@ZnO Quantum Dots/C core-shell nanorod arrays grown on flexible carbon cloth are successfully fabricated as a binder-free anode for Li-ion storage and shows superior rate capability and excellent cycling stability.
Abstract: MOF-derived ZnO@ZnO Quantum Dots/C core-shell nanorod arrays grown on flexible carbon cloth are successfully fabricated as a binder-free anode for Li-ion storage. In combination with the advantages from the ZnO/C core-shell architecture and the 3D nanorod arrays, this material satisfies both efficient ion and fast electron transport, and thus shows superior rate capability and excellent cycling stability.
TL;DR: By using BPQDs mixed with polyvinylpyrrolidone as the active layer, a flexible memory device was successfully fabricated that exhibits a nonvolatile rewritable memory effect with a high ON/OFF current ratio and good stability.
Abstract: As a unique two-dimensional nanomaterial, layered black phosphorus (BP) nanosheets have shown promising applications in electronics. Although mechanical exfoliation was successfully used to prepare BP nanosheets, it is still a challenge to produce novel BP nanostructures in high yield. A facile top-down approach for preparation of black phosphorus quantum dots (BPQDs) in solution is presented. The obtained BPQDs have a lateral size of 4.9±1.6 nm and thickness of 1.9±0.9 nm (ca. 4±2 layers). As a proof-of-concept application, by using BPQDs mixed with polyvinylpyrrolidone as the active layer, a flexible memory device was successfully fabricated that exhibits a nonvolatile rewritable memory effect with a high ON/OFF current ratio and good stability.
TL;DR: It is demonstrated that the electroluminescence (EL) mechanism of the inverted quantum dot light-emitting diodes (QD-LEDs) with a ZnO nanoparticle electron injection/transport layer should be direct charge-injection from charge transport layers into the QDs.
Abstract: Through introducing a probe layer of bis(4,6-difluorophenylpyridinato-N,C2)picolinatoiridium (FIrpic) between QD emission layer and 4, 4-N, N- dicarbazole-biphenyl (CBP) hole transport layer, we successfully demonstrate that the electroluminescence (EL) mechanism of the inverted quantum dot light-emitting diodes (QD-LEDs) with a ZnO nanoparticle electron injection/transport layer should be direct charge-injection from charge transport layers into the QDs. Further, the EL from QD-LEDs at sub-bandgap drive voltages is achieved, which is in contrast to the general device in which the turn-on voltage is generally equal to or greater than its bandgap voltage (the bandgap energy divided by the electron charge). This sub-bandgap EL is attributed to the Auger-assisted energy up-conversion hole-injection process at the QDs/organic interface. The high energy holes induced by Auger-assisted processes can be injected into the QDs at sub-bandgap applied voltages. These results are of important significance to deeply understand the EL mechanism in QD-LEDs and to further improve device performance.
TL;DR: The possibility of leveraging the atomically thin semiconductor tungsten diselenide (WSe2) as a host for quantum dot-like defects is demonstrated and it is reported that this previously unexplored solid-state quantum emitter in WSe2 generates single photons with emission properties that can be controlled via the application of external d.c. electric and magnetic fields.
Abstract: Single photons can be emitted by defects in WSe2 with emission properties that can be controlled through an applied voltage.
TL;DR: This article highlights carbon dots, which are small carbon nanoparticles with some form of surface passivation, and graphene quantum dots in various configurations by focusing on their syntheses, on their photoexcited state properties and redox processes, and on their applications as photocatalysts in visible-light carbon dioxide reduction and in water-splitting.
Abstract: Quantum dots (QDs) generally refer to nanoscale particles of conventional semiconductors that are subject to the quantum-confinement effect, though other nanomaterials of similar optical and redox properties are also named as QDs even in the absence of strictly defined quantum confinement. Among such nanomaterials that have attracted tremendous recent interest are carbon dots, which are small carbon nanoparticles with some form of surface passivation, and graphene quantum dots in various configurations. In this article, we highlight these carbon-based QDs by focusing on their syntheses, on their photoexcited state properties and redox processes, and on their applications as photocatalysts in visible-light carbon dioxide reduction and in water-splitting, as well as on their mechanistic similarities and differences.
TL;DR: Biosynthesis and Bioconjugation to Biomedical Application Juan Zhou,‡,§ Yong Yang, and Chun-yang Zhang*,†,§ †College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education.
Abstract: Biosynthesis and Bioconjugation to Biomedical Application Juan Zhou,‡,§ Yong Yang, and Chun-yang Zhang*,†,§ †College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals, Shandong Normal University, Jinan 250014, China ‡State Key Laboratory of Virology, Wuhan Institute of Virology, Chinese Academy of Sciences, Wuhan 430071, China Single-Molecule Detection and Imaging Laboratory, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
TL;DR: Emission color controlled, high quantum yield CH3NH3PbBr3 perovskite quantum dots are obtained by changing the temperature of a bad solvent during synthesis to achieve good spectral purity and short radiative lifetimes.
Abstract: Emission color controlled, high quantum yield CH3NH3PbBr3 perovskite quantum dots are obtained by changing the temperature of a bad solvent during synthesis. The products for temperatures between 0 and 60 °C have good spectral purity with narrow emission line widths of 28-36 nm, high absolute emission quantum yields of 74% to 93%, and short radiative lifetimes of 13-27 ns.
TL;DR: Centrifugally cast films retain bright photoluminescence and achieve dense and homogeneous morphologies and offer a platform for optoelectronic applications of perovskite quantum dot solids.
Abstract: Nanocrystals of CsPbX3 perovskites are promising materials for light-emitting optoelectronics because of their colloidal stability, optically tunable bandgap, bright photoluminescence, and excellent photoluminescence quantum yield. Despite their promise, nanocrystal-only films of CsPbX3 perovskites have not yet been fabricated; instead, highly insulating polymers have been relied upon to compensate for nanocrystals’ unstable surfaces. We develop solution chemistry that enables single-step casting of perovskite nanocrystal films and overcomes problems in both perovskite quantum dot purification and film fabrication. Centrifugally cast films retain bright photoluminescence and achieve dense and homogeneous morphologies. The new materials offer a platform for optoelectronic applications of perovskite quantum dot solids.
TL;DR: Passivated perovskite QD films showed remarkable photostability under continuous pulsed laser excitation in ambient conditions for at least 34 h, substantially exceeding the stability of other colloidal QD systems in which ASE has been observed.
Abstract: We demonstrate ultra-air- and photostable CsPbBr3 quantum dots (QDs) by using an inorganic–organic hybrid ion pair as the capping ligand. This passivation approach to perovskite QDs yields high photoluminescence quantum yield with unprecedented operational stability in ambient conditions (60 ± 5% lab humidity) and high pump fluences, thus overcoming one of the greatest challenges impeding the development of perovskite-based applications. Due to the robustness of passivated perovskite QDs, we were able to induce ultrastable amplified spontaneous emission (ASE) in solution processed QD films not only through one photon but also through two-photon absorption processes. The latter has not been observed before in the family of perovskite materials. More importantly, passivated perovskite QD films showed remarkable photostability under continuous pulsed laser excitation in ambient conditions for at least 34 h (corresponds to 1.2 × 108 laser shots), substantially exceeding the stability of other colloidal QD sys...
TL;DR: In this paper, a wearable colloidal quantum dot light-emitting diode array utilizing the intaglio transfer printing technique is presented, which allows the alignment of red-green-blue pixels with high resolutions up to 2,460 pixels per inch.
Abstract: Deformable full-colour light-emitting diodes with ultrafine pixels are essential for wearable electronics, which requires the conformal integration on curvilinear surface as well as retina-like high-definition displays. However, there are remaining challenges in terms of polychromatic configuration, electroluminescence efficiency and/or multidirectional deformability. Here we present ultra-thin, wearable colloidal quantum dot light-emitting diode arrays utilizing the intaglio transfer printing technique, which allows the alignment of red-green-blue pixels with high resolutions up to 2,460 pixels per inch. This technique is readily scalable and adaptable for low-voltage-driven pixelated white quantum dot light-emitting diodes and electronic tattoos, showing the best electroluminescence performance (14,000 cd m(-2) at 7 V) among the wearable light-emitting diodes reported up to date. The device performance is stable on flat, curved and convoluted surfaces under mechanical deformations such as bending, crumpling and wrinkling. These deformable device arrays highlight new possibilities for integrating high-definition full-colour displays in wearable electronics.
TL;DR: The advances in synthesis, assembly, ligand treatments and doping that have enabled high-mobility QD solids, as well as the experiments and theory that depict band-like transport in the QD solid state are reviewed.
Abstract: The emergence of high-mobility, colloidal semiconductor quantum dot (QD) solids has triggered fundamental studies that map the evolution from carrier hopping through localized quantum-confined states to band-like charge transport in delocalized and hybridized states of strongly coupled QD solids, in analogy with the construction of solids from atoms. Increased coupling in QD solids has led to record-breaking performance in QD devices, such as electronic transistors and circuitry, optoelectronic light-emitting diodes, photovoltaic devices and photodetectors, and thermoelectric devices. Here, we review the advances in synthesis, assembly, ligand treatments and doping that have enabled high-mobility QD solids, as well as the experiments and theory that depict band-like transport in the QD solid state. We also present recent QD devices and discuss future prospects for QD materials and device design.
TL;DR: It is demonstrated that CsPbX3 quantum dots (X = I, Br) can serve as room-temperature sources of quantum light, as indicated by strong photon antibunching detected in single-dot photoluminescence measurements.
Abstract: Lead-halide-based perovskites have been the subject of numerous recent studies largely motivated by their exceptional performance in solar cells. Electronic and optical properties of these materials have been commonly controlled by varying the composition (e.g., the halide component) and/or crystal structure. Use of nanostructured forms of perovskites can provide additional means for tailoring their functionalities via effects of quantum confinement and wave function engineering. Furthermore, it may enable applications that explicitly rely on the quantum nature of electronic excitations. Here, we demonstrate that CsPbX3 quantum dots (X = I, Br) can serve as room-temperature sources of quantum light, as indicated by strong photon antibunching detected in single-dot photoluminescence measurements. We explain this observation by the presence of fast nonradiative Auger recombination, which renders multiexciton states virtually nonemissive and limits the fraction of photon coincidence events to ∼6% on average....
TL;DR: In this article, a large-area quantum dot-luminescent solar concentrators free of toxic elements is presented, with reduced reabsorption and extended coverage of the solar spectrum.
Abstract: Luminescent solar concentrators serving as semitransparent photovoltaic windows could become an important element in net zero energy consumption buildings of the future. Colloidal quantum dots are promising materials for luminescent solar concentrators as they can be engineered to provide the large Stokes shift necessary for suppressing reabsorption losses in large-area devices. Existing Stokes-shift-engineered quantum dots allow for only partial coverage of the solar spectrum, which limits their light-harvesting ability and leads to colouring of the luminescent solar concentrators, complicating their use in architecture. Here, we use quantum dots of ternary I-III-VI2 semiconductors to realize the first large-area quantum dot-luminescent solar concentrators free of toxic elements, with reduced reabsorption and extended coverage of the solar spectrum. By incorporating CuInSexS2-x quantum dots into photo-polymerized poly(lauryl methacrylate), we obtain freestanding, colourless slabs that introduce no distortion to perceived colours and are thus well suited for the realization of photovoltaic windows. Thanks to the suppressed reabsorption and high emission efficiencies of the quantum dots, we achieve an optical power efficiency of 3.2%. Ultrafast spectroscopy studies suggest that the Stokes-shifted emission involves a conduction-band electron and a hole residing in an intragap state associated with a native defect.
TL;DR: A facile nonaqueous emulsion synthesis of colloidal halide perovskite quantum dots by controlled addition of a demulsifier into an emulsion of precursors is reported, which provides an alternative route toward high efficient solution-processed perovSkite-based light-emitting diodes.
Abstract: We report a facile nonaqueous emulsion synthesis of colloidal halide perovskite quantum dots by controlled addition of a demulsifier into an emulsion of precursors. The size of resulting CH3NH3PbBr3 quantum dots can be tuned from 2 to 8 nm by varying the amount of demulsifier. Moreover, this emulsion synthesis also allows the purification of these quantum dots by precipitation from the colloidal solution and obtains solid-state powder which can be redissolved for thin film coating and device fabrication. The photoluminescence quantum yields of the quantum dots is generally in the range of 80–92%, and can be well-preserved after purification (∼80%). Green light-emitting diodes fabricated comprising a spin-cast layer of the colloidal CH3NH3PbBr3 quantum dots exhibited maximum current efficiency of 4.5 cd/A, power efficiency of 3.5 lm/W, and external quantum efficiency of 1.1%. This provides an alternative route toward high efficient solution-processed perovskite-based light-emitting diodes. In addition, the...
TL;DR: It is shown that many of these limitations can be overcome by replacing interferometric optics with a two-dimensional absorptive filter array composed of colloidal quantum dots, which will be useful in applications where minimizing size, weight, cost and complexity of the spectrometer are critical.
Abstract: Spectroscopy is carried out in almost every field of science, whenever light interacts with matter. Although sophisticated instruments with impressive performance characteristics are available, much effort continues to be invested in the development of miniaturized, cheap and easy-to-use systems. Current microspectrometer designs mostly use interference filters and interferometric optics that limit their photon efficiency, resolution and spectral range. Here we show that many of these limitations can be overcome by replacing interferometric optics with a two-dimensional absorptive filter array composed of colloidal quantum dots. Instead of measuring different bands of a spectrum individually after introducing temporal or spatial separations with gratings or interference-based narrowband filters, a colloidal quantum dot spectrometer measures a light spectrum based on the wavelength multiplexing principle: multiple spectral bands are encoded and detected simultaneously with one filter and one detector, respectively, with the array format allowing the process to be efficiently repeated many times using different filters with different encoding so that sufficient information is obtained to enable computational reconstruction of the target spectrum. We illustrate the performance of such a quantum dot microspectrometer, made from 195 different types of quantum dots with absorption features that cover a spectral range of 300 nanometres, by measuring shifts in spectral peak positions as small as one nanometre. Given this performance, demonstrable avenues for further improvement, the ease with which quantum dots can be processed and integrated, and their numerous finely tuneable bandgaps that cover a broad spectral range, we expect that quantum dot microspectrometers will be useful in applications where minimizing size, weight, cost and complexity of the spectrometer are critical.
TL;DR: In this paper, transient absorption spectroscopy was used to show that the high PL QY can be attributed to negligible electron or hole trapping pathways in CsPbBr3 QDs: ∼94% of lowest excitonic states decayed with a singleexponential time constant of 4.5 ± 0.2 ns.
Abstract: Recently reported colloidal lead halide perovskite quantum dots (QDs) with tunable photoluminescence (PL) wavelengths covering the whole visible spectrum and exceptionally high PL quantum yields (QYs, 50-90%) constitute a new family of functional materials with potential applications in light-harvesting and -emitting devices. By transient absorption spectroscopy, we show that the high PL QYs (∼79%) can be attributed to negligible electron or hole trapping pathways in CsPbBr3 QDs: ∼94% of lowest excitonic states decayed with a single-exponential time constant of 4.5 ± 0.2 ns. Furthermore, excitons in CsPbBr3 QDs can be efficiently dissociated in the presence of electron or hole acceptors. The half-lives of electron transfer (ET) to benzoquinone and subsequent charge recombination are 65 ± 5 ps and 2.6 ± 0.4 ns, respectively. The half-lives for hole transfer (HT) to phenothiazine and the subsequent charge recombination are 49 ± 6 ps and 1.0 ± 0.2 ns, respectively. The lack of electron and hole traps and fast interfacial ET and HT rates are key properties that may enable the development of efficient lead halide perovskite QDs-based light-harvesting and -emitting devices.
TL;DR: The nanopatch antenna geometry can be tuned from the visible to the near infrared, providing a promising approach for nanophotonics based on ultrafast spontaneous emission and indicates a high radiative quantum efficiency of ∼50%.
Abstract: Typical emitters such as molecules, quantum dots and semiconductor quantum wells have slow spontaneous emission with lifetimes of 1–10 ns, creating a mismatch with high-speed nanoscale optoelectronic devices such as light-emitting diodes, single-photon sources and lasers. Here we experimentally demonstrate an ultrafast (<11 ps) yet efficient source of spontaneous emission, corresponding to an emission rate exceeding 90 GHz, using a hybrid structure of single plasmonic nanopatch antennas coupled to colloidal quantum dots. The antennas consist of silver nanocubes coupled to a gold film separated by a thin polymer spacer layer and colloidal core–shell quantum dots, a stable and technologically relevant emitter. We show an increase in the spontaneous emission rate of a factor of 880 and simultaneously a 2,300-fold enhancement in the total fluorescence intensity, which indicates a high radiative quantum efficiency of ∼50%. The nanopatch antenna geometry can be tuned from the visible to the near infrared, providing a promising approach for nanophotonics based on ultrafast spontaneous emission. Typical emitters such as molecules and quantum dots have slow spontaneous emission with lifetimes of 1–10 ns. Here, Hoang et al. have fabricated a hybrid structure of plasmonic nanopatch antennas coupled to quantum dots, achieving ultrafast spontaneous emission with a lifetime of 11 ps.