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The optical appeal and sustainability of carbon quantum dots (CQDs) have led to these nanoparticles swiftly gaining attention and emerging as a new, multifunctional class of nanomaterials. This work centers on the hydrothermal preparation of CQDs utilizing starch, an abundant and renewable biopolymer, as the precursor. Extensive characterization via spectroscopy and microscopy techniques revealed that the starch-derived CQDs exhibit a spherical nanoscale morphology averaging a ∼ 4 nm diameter, demonstrating a red-orange photoluminescence emission. Diffuse reflectance spectroscopic analysis verified their semiconductor behavior, with an estimated direct band gap of 4.1 eV comparable to conventional semiconductors. The prepared CQDs demonstrated considerable promise as metal-free, semiconductor photocatalysts for degrading aqueous dye pollutants under UV irradiation. High photodegradation efficiencies of 45.11 %, 62.94 %, and 91.21 % were achieved for Acid Blue 21, Reactive Blue 94, and Reactive TB 133 dyes, respectively. Systematic investigations of critical process parameters like pH, CQDs dosage, dye concentration, and contact time provided vital insights into the photocatalytic mechanism. The bio-sourced CQD nanomaterials offer a sustainable pathway for effective environmental remediation., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Fluorescence biosensors that enable highly sensitive detection of glutathione (GSH) are in great demand for various biological investigations and early disease diagnoses. Here, we report a turn-on fluorescence nanoplatform based on fluorescent semiconducting polymer nanoparticle@MnO 2 nanosheets (P-dot@MnO 2 ) nanocomposites for rapid homogeneous determination of GSH. The near-infrared (NIR) fluorescent P-dots were prepared by doping NIR dyes into polymer matrix and then encompassed by MnO 2 , which resulted in a remarkable fluorescence quenching. Owing to the selective decomposition of MnO 2 by GSH, the fluorescence recovery was achieved in the presence of GSH. On the basis of the target-induced turn-on fluorescence response, the developed nanoplatform can readily detect GSH with a high sensitivity up to 0.26 μM, as well as a superior specificity. Furthermore, it was successfully applied in monitoring the intracellular GSH in living cells, revealing its great potential in biomedical applications. Graphical abstract.

There is a growing need for brighter luminescent materials to improve the detection and imaging of biomarkers. Relevant contexts include low-abundance biomarkers and technology-limited applications, where an example of the latter is the emerging use of smartphones and other nonoptimal but low-cost and portable devices for point-of-care diagnostics. One approach to achieving brighter luminescent materials is incorporating multiple copies of a luminescent material into a larger supra-nanoparticle (supra-NP) assembly. Here, we present a facile method for the preparation and immunoconjugation of supra-NP assemblies (SiO 2 @QDs) that comprised many quantum dots (QDs) around a central silica nanoparticle (SiO 2 NP). The assembly was entirely driven by spontaneous affinity interactions between the constituent materials, which included imidazoline-functionalized silica nanoparticles, ligand-coated QDs, imidazole-functionalized dextran, and tetrameric antibody complexes (TACs). The physical and optical properties of the SiO 2 @QDs were characterized at both the ensemble and single-particle levels. Notably, the optical properties of the QDs were preserved upon assembly into supra-NPs, and single SiO 2 @QDs were approximately an order of magnitude brighter than single QDs and nonblinking. In proof-of-concept applications, including selective immunolabeling of breast cancer cells, the SiO 2 @QDs provided higher sensitivity and superior signal-to-background ratios whether using research-grade fluorescence microscopy or smartphone-based imaging. Overall, the SiO 2 @QDs are promising materials for enhanced bioanalysis and imaging.

Bioluminescence resonance energy transfer (BRET) is the non-radiative transfer of energy from a bioluminescent protein donor to a fluorophore acceptor. It shares all the formalism of Förster resonance energy transfer (FRET) but differs in one key aspect: that the excited donor here is produced by biochemical means and not by an external illumination. Often the choice of BRET source is the bioluminescent protein Renilla luciferase, which catalyzes the oxidation of a substrate, typically coelenterazine, producing an oxidized product in its electronic excited state that, in turn, couples with a proximal fluorophore resulting in a fluorescence emission from the acceptor. The acceptors pertinent to this discussion are semiconductor quantum dots (QDs), which offer some unrivalled photophysical properties. Amongst other advantages, the QD's large Stokes shift is particularly advantageous as it allows easy and accurate deconstruction of acceptor signal, which is difficult to attain using organic dyes or fluorescent proteins. QD-BRET systems are gaining popularity in non-invasive bioimaging and as probes for biosensing as they don't require external optical illumination, which dramatically improves the signal-to-noise ratio by avoiding background auto-fluorescence. Despite the additional advantages such systems offer, there are challenges lying ahead that need to be addressed before they are utilized for translational types of research.

Quantum dot-DNA oligonucleotide (QD-DNA) conjugates have been used in many fields such as nucleic acid bioassays, intracellular probes, and drug delivery systems. A typical solid-phase method that achieves rapid loading of oligonucleotides on surfaces of QDs involves a two-step reaction and is performed in a batch-based approach. In contrast, droplet microfluidics offers many advantages that are unavailable when using batch processing, providing rapid and dense immobilized DNA oligonucleotides on QDs. The presented droplet microfluidic approach allows high-quality QD-DNA conjugates to be produced using one single device, which is designed to have two droplet generators, one droplet merger, and one mixer. One of the droplet generators coencapsulates QDs and magnetic beads (MBs) into nanoliter-sized droplets for the production of QD-MB conjugates and the other encapsulates oligonucleotides in nanoliter-sized droplets. These two streams of droplets then merge at a one-to-one ratio in a chamber. The merged droplets travel along the mixer, which is a serpentine microchannel with 30 turns, resulting in QD-DNA conjugation structures of high quality. This multifunctional microfluidic device provides advantages such as higher degree of control over the reaction conditions, minimized cross-contamination and impurities, and reduction of reagent consumption while eliminating any need for external vortexing and pipetting. To evaluate the quality of the QD-DNA conjugates, they were used as Forster resonance energy transfer (FRET) probes to quantify oligonucleic targets.

Conversion of vacuum fluctuations into real particles was first predicted by L. Parker considering an expanding universe, followed in S. Hawking's work on black hole radiation. Since their experimental observation is challenging, analogue systems have gained attention in the verification of this concept. Here we propose an experimental set-up consisting of two adjacent piezoelectric semiconducting layers, one of them carrying dynamic quantum dots (DQDs), and the other being p-doped with an attached gate on top, which introduces a space-dependent layer conductivity. The propagation of surface acoustic waves (SAWs) on the latter layer is governed by a wave equation with an effective metric. In the frame of the DQDs, this space- and time-dependent metric possesses a sonic horizon for SAWs and resembles that of a two dimensional non-rotating and uncharged black hole to some extent. The non-thermal steady state of the DQD spin indicates particle creation in form of piezophonons., Competing Interests: The authors have declared that no competing interests exist.

The extraordinary potential of semiconductor quantum dots (QDs) has resulted in their widespread application in various fields, from engineering technology and the development of laboratory techniques to biomedical imaging and therapeutic strategies. However, the toxicity of QDs remains a concern and has limited their applications in human health. Better understanding of the behavior of QDs as it relates to their composition will enable the exploration of their limitations and development of a strategy to control their toxicity for potential therapeutic applications. Here, we describe approaches to minimize their toxicities according to the specific cell type, organ, or animal species, summarizing recent promising research at the cellular, organ, and whole-organism level., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

The development of botanical applications of nanomaterials has produced a new generation of technologies that can profoundly impact botanical research. Semiconductor quantum dots (QDs) are an archetype nanomaterial and have received significant interest from diverse research communities, owing to their unique and optimizable optical properties. In this review, we describe the most recent progress on QD-based botanical research and discuss the uptake, translocation, and effects of QDs on plants and the potential applications of QDs in botany. A critical evaluation of the current limitations of QD technologies is discussed, along with the future prospects in QD-based botanical research.

Bright long-wavelength-excitable semiconducting polymer dots (LWE-Pdots) are highly desirable for in vivo imaging and multiplexed in vitro bioassays. LWE-Pdots have been obtained by incorporating a near-infrared (NIR) emitter into the backbone of a polymer host to develop a binary donor-acceptor (D-A) system. However, they usually suffer from severe concentration quenching and a trade-off between fluorescence quantum yield (Φ f ) and absorption cross-section (σ). Herein, we describe a ternary component (D 1 /D 2 -A) strategy to achieve ultrabright, green laser-excitable Pdots with narrow-band NIR emission by introducing a BODIPY-based assistant polymer donor as D 1 . The D 1 /D 2 -A Pdots possess improved Φ f and σ compared to corresponding binary D 2 -A Pdots. Their Φ f is as high as 40.2 %, one of the most efficient NIR Pdots reported. The D 1 /D 2 -A Pdots show ultrahigh single-particle brightness, 83-fold brighter than Qdot 705 when excited by a 532 nm laser. When injected into mice, higher contrast in vivo tumor imaging was achieved using the ternary Pdots versus the binary D-A Pdots., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Rationale: Despite growing use of engineered nanomaterials (ENM) in applications from electronics to medicine, the potential risk to human health remains a critical concern within clinical use. ENM exposure during pregnancy can potentially cause reproductive toxicity even at levels that produce no measurable harm to animals in normal conditions. Methods: Phospholipid micelle-encapsulated CdSe/CdS/ZnS semiconductor nanocrystals with an average hydrodynamic diameter of 60 nm were intravenously injected during pregnancy in both rodent and nonhuman primate animal models. Cadmium concentration levels and maternal haematological and biochemical markers were determined, along with histopathological examination of major organs. Results: Nanocrystals were found to have crossed the placenta from mother to fetus in both rodents and nonhuman primates. However, the animal models display different responses with respect to reproductive toxicity. In the rodent model, toxicity symptoms are absent in treated subjects, with no observed gestational or fetal abnormalities and complications. A significantly higher miscarriage rate of 60% is recorded for macaques after prenatal nanoparticle administration. There was a miscarriage rate of 15% in the general population despite only ~0.16% of the initial cadmium dose present in the fetus. Blood and biochemical markers of treated macaques indicate acute hepatocellular injury within a week after nanoparticle administration. Histology of major organs of the miscarried macaque fetuses show no abnormalities. Conclusion: The potential of nanomaterials to cross the placenta and impact fetal survival in primates suggest the necessity of precautionary measures to prevent gestational exposure of ENMs., Competing Interests: Competing Interests: The authors have declared that no competing interest exists.

A natural-artificial hybrid system was constructed to enhance photophosphorylation. The system comprises chloroplasts modified with optically matched quantum dots (chloroplast-QD) with a large Stokes shift. The QDs possess a unique optical property and transform ultraviolet light into available and highly effective red light for use by chloroplasts. This favorable feature enables photosystem II contained within the hybrid system to split more water and produce more protons than chloroplasts would otherwise do on their own. Consequently, a larger proton gradient is generated and photophosphorylation is improved. At optimal efficiency activity increased by up to 2.3 times compared to pristine chloroplasts. Importantly, the degree of overlap between emission of the QDs and absorption of chloroplasts exerts a strong influence on the photophosphorylation efficiency. The chloroplast-QD hybrid presents an efficient solar energy conversion route, which involves a rational combination of a natural system and an artificial light-harvesting nanomaterial., (© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Type-II quantum dots (QDs) are capable of light-driven charge separation between their core and the shell structures; however, their light absorption is limited in the longer-wavelength range. Biological light-harvesting complex II (LHCII) efficiently absorbs in the blue and red spectral domains. Therefore, hybrid complexes of these two structures may be promising candidates for photovoltaic applications. Previous measurements had shown that LHCII bound to QD can transfer its excitation energy to the latter, as indicated by the fluorescence emissions of LHCII and QD being quenched and sensitized, respectively. In the presence of methyl viologen (MV), both fluorescence emissions are quenched, indicating an additional electron transfer process from QDs to MV. Transient absorption spectroscopy confirmed this notion and showed that electron transfer from QDs to MV is much faster than fluorescence energy transfer between LHCII and QD. The action spectrum of MV reduction by LHCII-QD complexes reflected the LHCII absorption spectrum, showing that light absorbed by LHCII and transferred to QDs increased the efficiency of MV reduction by QDs. Under continuous illumination, at least 28 turnovers were observed for the MV reduction. Presumably, the holes in QD cores were filled by a reducing agent in the reaction solution or by the dihydrolipoic-acid coating of the QDs. The LHCII-QD construct can be viewed as a simple model of a photosystem with the QD component acting as reaction center., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Colloidal semiconductor quantum dot (QD) nanocrystals have ideal fluorescence properties for bioanalysis and bioimaging, but these materials must be functionalized with an inorganic shell, organic ligand or polymer coating, and conjugated with biomolecules to be useful in such applications. Several different analytical techniques are used to characterize QDs and their multiple layers of functionalization. Here, we revisit poly(acrylamide) gel electrophoresis (PAGE), which has been scarcely used for the characterization of QDs and their bioconjugates in deference to the routine use of agarose gel electrophoresis. We implemented PAGE in a novel "stubby" capillary format with spectrofluorimetric detection, the combination of which enabled more rapid and more detailed characterization of QDs than was possible with both poly(acrylamide) and agarose slab gels. Correlations between the peak photoluminescence (PL) emission wavelength and electropherogram peaks, especially when combined with Ferguson analysis, provided new and significant insight into the key factors that determine the electrophoretic mobility of QDs, and helped to resolve heterogeneity and sub-populations in ensembles of QDs. The method was useful for characterization of the inorganic core/shell nanocrystals, their organic ligand and polymer coatings, and their final bioconjugates, the latter of which were in the form of peptide and protein conjugates. With further development and optimization, we anticipate that capillary PAGE with spectrofluorimetric detection will become a valuable addition to the toolbox of characterization techniques suitable for QDs, their bioconjugates, and other nanoparticle materials as well.

Colloidal semiconductor quantum dots (QDs) are light-emitting ultra-small nanoparticles, which have emerged as a new class of nanoprobes with unique optical properties for bioimaging and biomedical diagnostic. However, to be used for most biomedical applications the biocompatibility and water-solubility are mandatory that can achieved through surface modification forming QD-nanoconjugates. In this study, semiconductor II-VI quantum dots of type MX (M=Cd, Pb, Zn, X=S) were directly synthesized in aqueous media and at room temperature using carboxymethylcellulose sodium salt (CMC) behaving simultaneously as stabilizing and surface biofunctional ligand. These nanoconjugates were extensively characterized using UV-visible spectroscopy, photoluminescence spectroscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, X-ray diffraction, transmission electron microscopy, dynamic light scattering and zeta potential. The results demonstrated that the biopolymer was effective on nucleating and stabilizing the colloidal nanocrystals of CdS, ZnS, and PbS with the average diameter ranging from 2.0 to 5.0nm depending on the composition of the semiconductor core, which showed quantum-size confinement effect. These QD/polysaccharide conjugates showed luminescent activity from UV-visible to near-infrared range of the spectra under violet laser excitation. Moreover, the bioassays performed proved that these novel nanoconjugates were biocompatible and behaved as composition-dependent fluorescent nanoprobes for in vitro live cell bioimaging with very promising perspectives to be used in numerous biomedical applications and nanomedicine., (Copyright © 2017 Elsevier B.V. All rights reserved.)

The powder form and low photoluminescence quantum yield (PLQY) of fluorescent metal-organic frameworks (MOFs) present a serious obstacle to fabricating high-efficiency film-like lighting devices. Here, we present a facile way to produce thin films of CdSe x S 1-x /ZnS quantum dots (QDs)@ZIF-8 with high PLQY by encapsulating red, green, and blue CdSe x S 1-x /ZnS QDs in ZIF-8 through a one-pot solid-confinement conversion process. The QDs@ZIF-8 thin film emits warm white light with good color quality and presents good thermal stability and long-term durability., (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Luminescent semiconductor quantum dots (QDs) are one of the more popular nanomaterials currently utilized within biological applications. However, what is not widely appreciated is their growing role as versatile energy transfer (ET) donors and acceptors within a similar biological context. The progress made on integrating QDs and ET in biological configurations and applications is reviewed in detail here. The goal is to provide the reader with (1) an appreciation for what QDs are capable of in this context, (2) how this field has grown over a relatively short time span, and, in particular, (3) how QDs are steadily revolutionizing the development of new biosensors along with a myriad of other photonically active nanomaterial-based bioconjugates. An initial discussion of QD materials along with key concepts surrounding their preparation and bioconjugation is provided given the defining role these aspects play in the QDs ability to succeed in subsequent ET applications. The discussion is then divided around the specific roles that QDs provide as either Förster resonance energy transfer (FRET) or charge/electron transfer donor and/or acceptor. For each QD-ET mechanism, a working explanation of the appropriate background theory and formalism is articulated before examining their biosensing and related ET utility. Other configurations such as incorporation of QDs into multistep ET processes or use of initial chemical and bioluminescent excitation are treated similarly. ET processes that are still not fully understood such as QD interactions with gold and other metal nanoparticles along with carbon allotropes are also covered. Given their maturity, some specific applications ranging from in vitro sensing assays to cellular imaging are separated and discussed in more detail. Finally a perspective on how this field will continue to evolve is provided.

Oligonucleotide-coated nanoparticles (NPs) have been used in numerous applications such as bioassays, as intracellular probes, and for drug delivery. One challenge that is confronted in the preparation of oligonucleotide-NP conjugates is derived from surface charge because nanoparticles are often stabilized and made water-soluble with a coating of negatively charged capping ligands. Therefore, an electrostatic repulsion is present when attempting to conjugate oligonucleotides. The result is that the conjugation can be a slow process, sometimes requiring 1 to 2 days to equilibrate at the highest surface density. The effect is compounded by electrostatic repulsion between neighboring oligonucleotide strands on the NP surfaces, which tends to lower the surface density. Herein, we report a novel method that enables conjugation in less than 1 min with a surface density of oligonucleotides up to the theoretical physical limit of occupancy. Negatively charged NPs are first adsorbed onto the surface of positively charged magnetic beads (MBs) to create MB-NP conjugates. Oligonucleotides are subsequently electrostatically adsorbed onto the MB surfaces when added to a suspension of MB-NP conjugates. This creates an oligonucleotide concentration 10 5 to 10 6 greater than in bulk solution in the vicinity of the nanoparticles, resulting in the promotion of the kinetics by over 1000-fold and achieving the maximum density possible for the conjugation reaction.

Neuro-inspired implementations have attracted strong interest as a power efficient and robust alternative to the digital model of computation with a broad range of applications. Especially, neuro-mimetic systems able to produce and process spike-encoding schemes can offer merits like high noise-resiliency and increased computational efficiency. Towards this direction, integrated photonics can be an auspicious platform due to its multi-GHz bandwidth, its high wall-plug efficiency and the strong similarity of its dynamics under excitation with biological spiking neurons. Here, we propose an integrated all-optical neuron based on an InAs/InGaAs semiconductor quantum-dot passively mode-locked laser. The multi-band emission capabilities of these lasers allows, through waveband switching, the emulation of the excitation and inhibition modes of operation. Frequency-response effects, similar to biological neural circuits, are observed just as in a typical two-section excitable laser. The demonstrated optical building block can pave the way for high-speed photonic integrated systems able to address tasks ranging from pattern recognition to cognitive spectrum management and multi-sensory data processing.

Water pollution is a cause for serious concern in today's world. A major contributor to water pollution is industrial effluents containing dyes and other organic molecules. Waste water treatment has become a priority area in today's applied scientific research as it seeks to minimize the toxicity of the effluents being discharged and increase the possibility of water recycling. An efficient and eco-friendly way of degrading toxic molecules is to use nano metal-oxide photocatalysts. The present study aims at enhancing the photocatalytic activity of a semiconductor metal oxide by doping it with nitrogen. A sol-gel cum combustion method was employed to synthesize the catalyst. The prepared catalyst was characterized by FT-IR, XRD, UV-DRS, FESEM and AFM techniques. UV-DRS result showed the catalyst to possess band gap energy of 2.97eV, thus making it active in the UV region of the spectrum. Its photocatalytic activity was evaluated by the degradation of a model pollutant-Orange G dye, under UV light irradiation. Preliminary experiments were carried out to study the effects of pH, catalyst dosage and initial dye concentration on the extent of dye degradation. Kinetic studies revealed that the reaction followed pseudo first order kinetics. The effect of electrolytes on catalyst efficiency was also studied. The progress of the reaction was monitored by absorption studies and measuring the reduction in COD. The catalyst thus prepared was seen to have a high photocatalytic efficiency. The use of this catalyst is a promising means of waste water treatment., (Copyright © 2016 Elsevier Inc. All rights reserved.)

Photochromic or photocaged ligands can be anchored to the outer shell of semiconductor quantum dots in order to control the photophysical properties of these inorganic nanocrystals with optical stimulations. One of the two interconvertible states of the photoresponsive ligands can be designed to accept either an electron or energy from the excited quantum dots and quench their luminescence. Under these conditions, the reversible transformations of photochromic ligands or the irreversible cleavage of photocaged counterparts translates into the possibility to switch luminescence with external control. As an alternative to regulating the photophysics of a quantum dot via the photochemistry of its ligands, the photochemistry of the latter can be controlled by relying on the photophysics of the former. The transfer of excitation energy from a quantum dot to a photocaged ligand populates the excited state of the species adsorbed on the nanocrystal to induce a photochemical reaction. This mechanism, in conjunction with the large two-photon absorption cross section of quantum dots, can be exploited to release nitric oxide or to generate singlet oxygen under near-infrared irradiation. Thus, the combination of semiconductor quantum dots and photoresponsive ligands offers the opportunity to assemble nanostructured constructs with specific functions on the basis of electron or energy transfer processes. The photoswitchable luminescence and ability to photoinduce the release of reactive chemicals, associated with the resulting systems, can be particularly valuable in biomedical research and can, ultimately, lead to the realization of imaging probes for diagnostic applications as well as to therapeutic agents for the treatment of cancer.

The efficient selection and isolation of individual cells of interest from a mixed population is desired in many biomedical and clinical applications. Here we show the concept of using photoswitchable semiconducting polymer dots (Pdots) as an optical 'painting' tool, which enables the selection of certain adherent cells based on their fluorescence, and their spatial and morphological features, under a microscope. We first develop a Pdot that can switch between the bright (ON) and dark (OFF) states reversibly with a 150-fold contrast ratio on irradiation with ultraviolet or red light. With a focused 633-nm laser beam that acts as a 'paintbrush' and the photoswitchable Pdots as the 'paint', we select and 'paint' individual Pdot-labelled adherent cells by turning on their fluorescence, then proceed to sort and recover the optically marked cells (with 90% recovery and near 100% purity), followed by genetic analysis.

This work developed a CdS/MoS2 heterojunction-based photoelectrochemical biosensor for sensitive detection of DNA under the enhanced chemiluminescence excitation of luminol catalyzed by hemin-DNA complex. The CdS/MoS2 photocathode was prepared by the stepwise assembly of MoS2 and CdS quantum dots (QDs) on indium tin oxide (ITO), and achieved about 280% increasing of photocurrent compared to pure CdS QDs electrode due to the formation of heterostructure. High photoconversion efficiency in the photoelectrochemical system was identified to be the rapid spatial charge separation of electron-hole pairs by the extension of electron transport time and electron lifetime. In the presence of target DNA, the catalytic hairpin assembly was triggered, and simultaneously the dual hemin-labeled DNA probe was introduced to capture DNA/CdS/MoS2 modified ITO electrode. Thus the chemiluminescence emission of luminol was enhanced via hemin-induced mimetic catalysis, leading to the physical light-free photoelectrochemical strategy. Under optimized conditions, the resulting photoelectrode was proportional to the logarithm of target DNA concentration in the range from 1 fM to 100 pM with a detection limit of 0.39 fM. Moreover, the cascade amplification biosensor demonstrated high selectivity, desirable stability and good reproducibility, showing great prospect in molecular diagnosis and bioanalysis., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Plasmonic nanoparticles are an attractive material for light harvesting applications due to their easily modified surface, high surface area and large extinction coefficients which can be tuned across the visible spectrum. Research into the plasmonic enhancement of optical transitions has become popular, due to the possibility of altering and in some cases improving photo-absorption or emission properties of nearby chromophores such as molecular dyes or quantum dots. The electric field of the plasmon can couple with the excitation dipole of a chromophore, perturbing the electronic states involved in the transition and leading to increased absorption and emission rates. These enhancements can also be negated at close distances by energy transfer mechanism, making the spatial arrangement of the two species critical. Ultimately, enhancement of light harvesting efficiency in plasmonic solar cells could lead to thinner and, therefore, lower cost devices. The development of hybrid core/shell particles could offer a solution to this issue. The addition of a dielectric spacer between a gold nanoparticles and a chromophore is the proposed method to control the exciton plasmon coupling strength and thereby balance losses with the plasmonic gains. A detailed procedure for the coating of gold nanoparticles with CdS and ZnS semiconductor shells is presented. The nanoparticles show high uniformity with size control in both the core gold particles and shell species allowing for a more accurate investigation into the plasmonic enhancement of external chromophores.

The photoluminescence (PL) characteristics of CdSe quantum dots (QDs) infiltrated into inverse opal SiO2 photonic crystals (PCs) are systemically studied. The special porous structure of inverse opal PCs enhanced the thermal exchange rate between the CdSe QDs and their surrounding environment. Finally, inverse opal SiO2 PCs suppressed the nonlinear PL enhancement of CdSe QDs in PCs excited by a continuum laser and effectively modulated the PL characteristics of CdSe QDs in PCs at high temperatures in comparison with that of CdSe QDs out of PCs. The final results are of benefit in further understanding the role of inverse opal PCs on the PL characteristics of QDs., (Copyright © 2015 John Wiley & Sons, Ltd.)

The salient optical properties of highly luminescent semiconductor nanocrystals render them ideal fluorophores for clinical diagnostics, therapeutics, and highly sensitive biochip applications. Microfluidic systems allow miniaturization and integration of multiple biochemical processes in a single device and do not require sophisticated diagnostic tools. Herein, we describe a microfluidic system that integrates RNA extraction, reverse transcription to cDNA, amplification and detection within one integrated device to detect histidine decarboxylase (HDC) gene directly from human white blood cells samples. When anisotropic semiconductor nanorods (NRs) were used as the fluorescent probes, the detection limit was found to be 0.4 ng of total RNA, which was much lower than that obtained using spherical quantum dots (QDs) or organic dyes. This was attributed to the large action cross-section of NRs and their high probability of target capture in a pull-down detection scheme. The combination of large scale integrated microfluidics with highly fluorescent semiconductor NRs may find widespread utility in point-of-care devices and multitarget diagnostics.

The intrinsic properties of quantum dots (QDs) and the growing ability to interface them controllably with living cells has far-reaching potential applications in probing cellular processes such as membrane action potential. We demonstrate that an electric field typical of those found in neuronal membranes results in suppression of the QD photoluminescence (PL) and, for the first time, that QD PL is able to track the action potential profile of a firing neuron with millisecond time resolution. This effect is shown to be connected with electric-field-driven QD ionization and consequent QD PL quenching, in contradiction with conventional wisdom that suppression of the QD PL is attributable to the quantum confined Stark effect.

Semiconductor quantum dots (QDs) and semiconducting polymer nanoparticles (Pdots) are brightly emissive materials that offer many advantages for bioanalysis and bioimaging, and are complementary to revolutionary advances in fluorescence technology. Within the context of biological applications, this review compares the evolution and different stages of development of these two types of nanoparticle, and addresses current perceptions about QDs. Although neither material is a wholesale replacement for fluorescent dyes, recent trends have demonstrated that both types of nanoparticle can excel in applications that are often too demanding for fluorescent dyes alone. Examples discussed in this review include single particle tracking and imaging, multicolor imaging and multiplexed detection, biosensing, point-of-care diagnostics, in vivo imaging and drug delivery., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Förster (or fluorescence) resonance energy transfer amongst semiconductor quantum dots (QDs) is reviewed, with particular interest in biosensing applications. The unique optical properties of QDs provide certain advantages and also specific challenges with regards to sensor design, compared to other FRET systems. The brightness and photostability of QDs make them attractive for highly sensitive sensing and long-term, repetitive imaging applications, respectively, but the overlapping donor and acceptor excitation signals that arise when QDs serve as both the donor and acceptor lead to high background signals from direct excitation of the acceptor. The fundamentals of FRET within a nominally homogeneous QD population as well as energy transfer between two distinct colors of QDs are discussed. Examples of successful sensors are highlighted, as is cascading FRET, which can be used for solar harvesting.

Hybrid materials composed of colloidal semiconductor quantum dots and π-conjugated organic molecules and polymers have attracted continuous interest in recent years, because they may find applications in bio-sensing, photodetection, and photovoltaics. Fundamental processes occurring in these nanohybrids are light absorption and emission as well as energy and/or charge transfer between the components. For future applications it is mandatory to understand, control, and optimize the wide parameter space with respect to chemical assembly and the desired photophysical properties. Accordingly, different approaches to tackle this issue are described here. Simple organic dye molecules (Dye)/quantum dot (QD) conjugates are studied with stationary and time-resolved spectroscopy to address the dynamics of energy and ultra-fast charge transfer. Micellar as well as lamellar nanostructures derived from diblock copolymers are employed to fine-tune the energy transfer efficiency of QD donor/dye acceptor couples. Finally, the transport of charges through organic components coupled to the quantum dot surface is discussed with an emphasis on functional devices., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Colloidal nanocrystal solids represent an emerging class of functional materials that hold strong promise for device applications. The macroscopic properties of these disordered assemblies are determined by complex trajectories of exciton diffusion processes, which are still poorly understood. Owing to the lack of theoretical insight, experimental strategies for probing the exciton dynamics in quantum dot solids are in great demand. Here, we develop an experimental technique for mapping the motion of excitons in semiconductor nanocrystal films with a subdiffraction spatial sensitivity and a picosecond temporal resolution. This was accomplished by doping PbS nanocrystal solids with metal nanoparticles that force the exciton dissociation at known distances from their birth. The optical signature of the exciton motion was then inferred from the changes in the emission lifetime, which was mapped to the location of exciton quenching sites. By correlating the metal-metal interparticle distance in the film with corresponding changes in the emission lifetime, we could obtain important transport characteristics, including the exciton diffusion length, the number of predissociation hops, the rate of interparticle energy transfer, and the exciton diffusivity. The benefits of this approach to device applications were demonstrated through the use of two representative film morphologies featuring weak and strong interparticle coupling.

Despite the bright and tuneable photoluminescence (PL) of semiconductor quantum dots (QDs), the PL instability induced by Auger recombination and oxidation poses a major challenge in single-molecule applications of QDs. The incomplete information about Auger recombination and oxidation is an obstacle in the resolution of this challenge. Here, we report for the first time that Auger-ionized QDs beat self-sensitized oxidation and the non-digitized PL intensity loss. Although high-intensity photoactivation insistently induces PL blinking, the transient escape of QDs into the ultrafast Auger recombination cycle prevents generation of singlet oxygen ((1) O2 ) and preserves the PL intensity. By the detection of the NIR phosphorescence of (1) O2 and evaluation of the photostability of single QDs in aerobic, anaerobic, and (1) O2 scavenger-enriched environments, we disclose relations of Auger ionization and (1) O2 -mediated oxidation to the PL stability of single QDs, which will be useful during the formulation of QD-based single-molecule imaging tools and single-photon devices., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The biological applications of luminescent semiconductor quantum dots (QDs) continue to grow at a nearly unabated pace. This growth is driven, in part, by their unique photophysical and physicochemical properties which have allowed them to be used in many different roles in cellular biology including: as superior fluorophores for a wide variety of cellular labeling applications; as active platforms for assembly of nanoscale sensors; and, more recently, as a powerful tool to understand the mechanisms of nanoparticle mediated drug delivery. Given that controlled cellular delivery is at the intersection of all these applications, the latest progress in delivering QDs to cells is examined here. A brief discussion of relevant considerations including the importance of materials preparation and bioconjugation along with the continuing issue of endosomal sequestration is initially provided for context. Methods for the cellular delivery of QDs are then highlighted including those based on passive exposure, facilitated strategies that utilize peptides or polymers and fully active modalities such as electroporation and other mechanically based methods. Following on this, the exciting advent of QD cellular delivery using multiple or combined mechanisms is then previewed. Several recent methods reporting endosomal escape of QD materials in cells are also examined in detail with a focus on the mechanisms by which access to the cytosol is achieved. The ongoing debate over QD cytotoxicity is also discussed along with a perspective on how this field will continue to evolve in the future., (© 2014 The Authors. WIREs Nanomedicine and Nanobiotechnology published by Wiley Periodicals, Inc.)

We reveal an easy, inexpensive, efficient one stepflame synthesis of semiconductor/metal oxide thin films at air-liquid interface, subsequently, transferred on suitable substrate. The method has been illustrated by the formation of CdS and WO3 QDs thin films. The features of the present method are (1) Growth of thin films consisting of0.5-2.0nm sized Quantum Dots (QDs)/(ultra-small nanoparticles) in a short time, at the air-liquid interface which can be suitably transferred by a well-known Blodgett technique to an appropriate substrate, (2) The method is suitable to apply layer by layer (LbL) technique to increase the film thickness as well as forming various compositions as revealed by AFM measurements. The films are characterized for their structure (SAED), morphology (TEM), optical properties (UV-Vis.) and photoluminescence (PL). Possible mechanism of formation of QDs thin film and effect of capping in case of CdS QDs is discussed., (Copyright © 2014 Elsevier Inc. All rights reserved.)

Pump-probe quantum state tomography was applied to the transmission of a coherent state through an In(Ga)As based quantum dot optical amplifier during the interaction with an optical pump pulse. The Wigner function and the statistical moments of the field were extracted and used to determine the degree of population inversion and the signal-to-noise ratio in a sub-picosecond time window.

Due to the intrinsic hole oxidation reaction occurred on the photoanode surface, currently developed photoelectrochemical biosensors suffer from the interference from coexisting reductive species (acting as electron donor) and a novel design strategy of photoelectrode for photoelectrochemical detection is urgently required. In this paper, a self-operating photocathode based on CdS quantum dots sensitized three-dimensional (3D) nanoporous NiO was designed and created, which showed highly selective and reversible response to dissolved oxygen (acting as electron acceptor) in the electrolyte solution. Using glucose oxidase (GOD) as a biocatalyst, a novel photoelectrochemical sensor for glucose was developed. The commonly encountered interferents such as H2O2, ascorbic acid (AA), cysteine (Cys), dopamine (DA), etc., almost had no effect for the cathodic photocurrent of the 3D NiO/CdS electrode, though these substances were proved to greatly influence the photocurrent of photoanodes, which indicated greatly improved selectivity of the method. The method was applied to detect glucose in real samples including serum and glucose injections with satisfactory results. This study could provide a new train of thought on designing of self-operating photocathode in photoelectrochemical sensing, promoting the application of semiconductor nanomaterials in photoelectrochemistry., (Copyright © 2014 Elsevier B.V. All rights reserved.)

We study the exciton contribution to the third-order optical susceptibility of one-dimensional semiconductor quantum dots and show that the screening of the electron-hole interaction has a strong influence on the nonlinear optical properties in the weak confinement regime. Based on a density matrix formulation, we estimate the spectrum of the third-order optical susceptibility and its contribution to the refraction index and absorption coefficient. In particular, we show that the multipeaked spectrum of the nonlinear susceptibility, which results from the hydrogenoid character of the exciton eigenstates for a purely Coulombian electron-hole coupling, is reverted towards a single peaked structure as the interaction becomes strongly screened, thus leading to a substantial enhancement of the nonlinear optical properties of semiconductor quantum dots.

A high-power tunable external cavity laser configuration with a tapered quantum-dot semiconductor optical amplifier at its core is presented, enabling a record output power for a broadly tunable semiconductor laser source in the 1.2 - 1.3 µm spectral region. Two distinct optical amplifiers are investigated, using either chirped or unchirped quantum-dot structures, and their merits are compared, considering the combination of tunability and high output power generation. At 1230 nm, the chirped quantum-dot laser achieved a maximum power of 0.62 W and demonstrated nearly 100-nm tunability. The unchirped laser enabled a tunability range of 32 nm and at 1254 nm generated a maximum power of 0.97 W, representing a 22-fold increase in output power compared with similar narrow-ridge external-cavity lasers at the same current density.

We present a comprehensive model for In(0.18)Ga(0.82)N/GaN self-assembled quantum dot (QD) active material. The strain distribution in the QD structure is studied using linear elastic theory with the application of the shrink-fit boundary condition at the material interface. Subsequent calculations also predict the strain-induced quantum-confined Stark effect (QCSE). Under carrier injection, the overall effect of band bending and charge screening is studied by solving the Schrödinger and Poisson equations self-consistently. The optical gain spectrum of the InGaN/GaN QD active material is calculated based on the electronic states solved from the Schrödinger-Poisson equation, and both the calculated material gain peak and emission wavelength agree well with the measured experimental data.

We propose a nanogap structure composed of semiconductor nanoparticles forming an optical cavity. The resonant excitation of excitons in the nanoparticles can generate a localized strong light field in the gap region, also called "hot spot". The spectral width of the hot spot is significantly narrow because of the small exciton damping and the dephasing at low temperature, so the semiconductor nanogap structure acts as a high-Q cavity. In addition, the interaction between light and matter at the nanogap is significantly larger than that in a conventional microcavity, because the former has a small cavity-mode volume beyond the diffraction limit. We theoretically demonstrate the large and well-defined vacuum-Rabi splitting of a two-level emitter placed inside the semiconductor nanogap cavity: the Rabi splitting energy of 1.7 meV for the transition dipole moment of the emitter (25 Debye) is about 6.3 times larger than the spectral width. An optical cavity providing such a large and well-defined Rabi splitting is highly suited for studying characteristic features of the cavity quantum electrodynamics and for the development of new applications.

Organic fluorophores and quantum dots are ubiquitous as contrast agents for bio-imaging and as labels in bioassays to enable the detection of biological targets and processes. Upconversion nanoparticles (UCNPs) offer a different set of opportunities as labels in bioassays and for bioimaging. UCNPs are excited at near-infrared (NIR) wavelengths where biological molecules are optically transparent, and their luminesce in the visible and ultraviolet (UV) wavelength range is suitable for detection using complementary metal-oxide-semiconductor (CMOS) technology. These nanoparticles provide multiple sharp emission bands, long lifetimes, tunable emission, high photostability, and low cytotoxicity, which render them particularly useful for bio-imaging applications and multiplexed bioassays. This paper surveys several key concepts surrounding upconversion nanoparticles and the systems that detect and process the corresponding luminescence signals. The principle of photon upconversion, tuning of emission wavelengths, UCNP bioassays, and UCNP time-resolved techniques are described. Electronic readout systems for signal detection and processing suitable for UCNP luminescence using CMOS technology are discussed. This includes recent progress in miniaturized detectors, integrated spectral sensing, and high-precision time-domain circuits. Emphasis is placed on the physical attributes of UCNPs that map strongly to the technical features that CMOS devices excel in delivering, exploring the interoperability between the two technologies.

Knowledge of sample temperatures during nuclear magnetic resonance (NMR) measurements is important for acquisition of optimal NMR data and proper interpretation of the data. Sample temperatures can be difficult to measure accurately for a variety of reasons, especially because it is generally not possible to make direct contact to the NMR sample during the measurements. Here I show that sample temperatures during magic-angle spinning (MAS) NMR measurements can be determined from temperature-dependent photoluminescence signals of semiconductor quantum dots that are deposited in a thin film on the outer surface of the MAS rotor, using a simple optical fiber-based setup to excite and collect photoluminescence. The accuracy and precision of such temperature measurements can be better than ±5K over a temperature range that extends from approximately 50K (-223°C) to well above 310K (37°C). Importantly, quantum dot photoluminescence can be monitored continuously while NMR measurements are in progress. While this technique is likely to be particularly valuable in low-temperature MAS NMR experiments, including experiments involving dynamic nuclear polarization, it may also be useful in high-temperature MAS NMR and other forms of magnetic resonance., (Published by Elsevier Inc.)

We have synthesized Er2S3/ZnS core/shell QDs by employing ErSt3, ZnSt2, and sulfur as precursors via a hot solution phase chemistry using a nucleation-doping strategy. X-ray diffraction (XRD), transmission electron microscope (TEM) and photoluminescence (PL) spectra were used to characterize the structure, morphology and luminescence properties of Er2S3/ZnS core/shell QDs. Moreover, the influence of overcoating temperatures on the infrared luminescence properties of QDs was investigated. PL spectra show that the emission intensity from the 4I13/2 --> 4I15/2 transition of Er3+ strongly increases with increasing overcoating temperatures, which was interpreted by the enhancing diffusion of Er3+ ions. IR-LEDs were fabricated combining commercial red GaAs LEDs with Er2S3/ZnS QDs, and luminescence properties of the IR-LED have been investigated.

We introduce a quantum dot in topological insulator nanofilm as a bump at the surface of the nanofilm. Such a quantum dot can localize an electron if the size of the dot is large enough, ≳5 nm. The quantum dot in topological insulator nanofilm has states of two types, which belong to two ('conduction' and 'valence') bands of the topological insulator nanofilm. We study the energy spectra of such defined quantum dots. We also consider intraband and interband optical transitions within the dot. The optical transitions of the two types have the same selection rules. While the interband absorption spectra have multi-peak structure, each of the intraband spectra has one strong peak and a few weak high frequency satellites.

Bio-functionalised luminescent organic semiconductors are attractive for biophotonics because they can act as efficient laser materials while simultaneously interacting with molecules. In this paper, we present and discuss a laser biosensor platform that utilises a gain layer made of such an organic semiconductor material. The simple structure of the sensor and its operation principle are described. Nanolayer detection is shown experimentally and analysed theoretically in order to assess the potential and the limits of the biosensor. The advantage conferred by the organic semiconductor is explained, and comparisons to laser sensors using alternative dye-doped materials are made. Specific biomolecular sensing is demonstrated, and routes to functionalisation with nucleic acid probes, and future developments opened up by this achievement, are highlighted. Finally, attractive formats for sensing applications are mentioned, as well as colloidal quantum dots, which in the future could be used in conjunction with organic semiconductors.

We present a diode incorporating a large number (12) of GaAs quantum wells that emits light from exciton-polariton states at room temperature. A reversely biased tunnel junction is placed in the cavity region to improve current injection into the device. Electroluminescence studies reveal two polariton branches which are spectrally separated by a Rabi splitting of 6.5 meV. We observe an anticrossing of the two branches when the temperature is lowered below room temperature as well as a Stark shift of both branches in a bias dependent photoluminescence measurement.

We present a series of non-stoichiometric cadmium sulfide quantum-dot (QD) models. Using density functional theory (DFT) and semi-empirical molecular orbital (MO) calculations, we explore the ligand binding and exchange chemistry of these models. Their surface morphology allows for these processes to be rationalized on the atomic scale. This is corroborated by ultraviolet-visible (UV-vis), infrared (IR), and inductively coupled plasma-optical emission spectroscopy (ICP-OES).

A CMOS tunable-wavelength multi-color photogate (CPG) sensor is presented. Sensing of a small set of well-separated wavelengths (e.g., > 50 nm apart) is achieved by tuning the spectral response of the device with a bias voltage. The CPG employs the polysilicon gate as an optical filter, which eliminates the need for an external color filter. A prototype has been fabricated in a standard 0.35 μm digital CMOS technology and demonstrates intensity measurements of blue (450 nm), green (520 nm), and red (620 nm) illumination with peak signal-to-noise ratios (SNRs) of 34.7 dB , 29.2 dB, and 34.8 dB, respectively. The prototype is applied to fluorescence detection of green-emitting quantum dots (gQDs) and red-emitting quantum dots (rQDs). It spectrally differentiates among multiple emission bands, effectively implementing on-chip emission filtering. The prototype demonstrates single-color measurements of gQD and rQD concentrations to a detection limit of 24 nM, and multi-color measurements of solutions containing both colors of QDs to a detection limit of 90 nM and 120 nM of gQD and rQD, respectively.

Understanding how semiconductor quantum dots (QDs) engage in photoinduced energy transfer with carbon allotropes is necessary for enhanced performance in solar cells and other optoelectronic devices along with the potential to create new types of (bio)sensors. Here, we systematically investigate energy transfer interactions between C60 fullerenes and four different QDs, composed of CdSe/ZnS (type I) and CdSe/CdS/ZnS (quasi type II), with emission maxima ranging from 530 to 630 nm. C60-pyrrolidine tris-acid was first coupled to the N-terminus of a hexahistidine-terminated peptide via carbodiimide chemistry to yield a C60-labeled peptide (pepC60). This peptide provided the critical means to achieve ratiometric self-assembly of the QD-(pepC60) nanoheterostructures by exploiting metal affinity coordination to the QD surface. Controlled QD-(pepC60)N bioconjugates were prepared by discretely increasing the ratio (N) of pepC60 assembled per QD in mixtures of dimethyl sulfoxide and buffer; this mixed organic/aqueous approach helped alleviate issues of C60 solubility. An extensive set of control experiments were initially performed to verify the specific and ratiometric nature of QD-(pepC60)N assembly. Photoinitiated energy transfer in these hybrid organic-inorganic systems was then interrogated using steady-state and time-resolved fluorescence along with ultrafast transient absorption spectroscopy. Coordination of pepC60 to the QD results in QD PL quenching that directly tracks with the number of peptides displayed around the QD. A detailed photophysical analysis suggests a competition between electron transfer and Förster resonance energy transfer from the QD to the C60 that is dependent upon a complex interplay of pepC60 ratio per QD, the presence of underlying spectral overlap, and contributions from QD size. These results highlight several important factors that must be considered when designing QD-donor/C60-acceptor systems for potential optoelectronic and biosensing applications.

A highly fluorescent fluorinated semiconducting polymer dot (Pdot) with a quantum yield of up to 49% was developed. The fluorinated Pdot was eight times brighter in cell-labeling applications than its non-fluorinated counterpart, and was rod shaped rather than spherical.