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At least 361 records · Page 20

Graphitic Carbon Nitride Quantum Dots (g‐C 3 N 4 QDs): From Chemistry to Applications

Since their emergence in 2014, graphitic carbon nitride quantum dots (g-C 3 N 4 QDs) have attracted much interest from the scientific community due to their distinctive physicochemical features, including structural, morphological, electrochemical, and optoelectronic properties. Owing to their desirable characteristics, such as non-zero band gap, ability to be chemically functionalized or doped, possessing tunable properties, outstanding dispersibility in different media, and biocompatibility, g-C 3 N 4 QDs have shown promise for photocatalysis, energy devices, sensing, bioimaging, solar cells, optoelectronics, among other applications. As these fields are rapidly evolving, it is very strenuous to pinpoint the emerging challenges of the g-C 3 N 4 QDs development and application during the last decade, mainly due to the lack of critical reviews of the innovations in the g-C 3 N 4 QDs synthesis pathways and domains of application. Herein, an extensive survey is conducted on the g-C 3 N 4 QDs synthesis, characterization, and applications. Scenarios for the future development of g-C 3 N 4 QDs and their potential applications are highlighted and discussed in detail. In conclusion, the provided critical section suggests a myriad of opportunities for g-C 3 N 4 QDs, especially for their synthesis and functionalization, where a combination of eco-friendly/single step synthesis and chemical modification may be used to prepare g-C 3 N 4 QDs with, for example, enhanced photoluminescence and production yields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gate-Defined Accumulation-Mode Quantum Dots in Monolayer and Bilayer WSe 2

Here, we report the fabrication and characterization of gate-defined hole quantum dots in monolayer and bilayer WSe 2 . The devices are operated with gates above and below the WSe 2 layer to accumulate a hole gas, which for some devices is then selectively depleted to define the dot. Temperature dependence of conductance in the Coulomb-blockade regime is consistent with transport through a single level, and excited-state transport through the dots is observed at temperatures up to 10 K. For adjacent charge states of a bilayer-WSe 2 dot, the magnetic field dependence of excited-state energies is used to estimate $\textit{g}$ factors between 0.8 and 2.4 for different states. These devices provide a platform to evaluate valley-spin states in monolayer and bilayer WSe 2 for application as qubits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dynamic performance and reflection sensitivity of quantum dot distributed feedback lasers with large optical mismatch

This work reports on a high-efficiency InAs/GaAs distributed feedback quantum dot laser. The large optical wavelength detuning at room temperature between the lasing peak and the gain peak causes the static, dynamic, and nonlinear intrinsic properties to all improve with temperature, including the lasing efficiency, the modulation dynamics, the linewidth enhancement factor, and consequently the reflection insensitivity. Results reported show an optimum operating temperature at 75°C, highlighting the potential of the large optical mismatch assisted single-frequency laser for the development of uncooled and isolator-free high-speed photonic integrated circuits.

Dong, Bozhang (ORCID:0000000158266723)↗

Modeling multihole Ge spins in quantum dot systems

Beyond the title, this talk is about improving the computational modeling of germanium hole spins in lithographic quantum dots to work towards a better understanding of how potential qubit properties of these systems are affected by the effective shell filling of these holes in the electric potential.

Brickson, Mitchell Ian↗

Atomically dispersed Pb ionic sites in PbCdSe quantum dot gels enhance room-temperature NO2 sensing

Abstract Atmospheric NO 2 is of great concern due to its adverse effects on human health and the environment, motivating research on NO 2 detection and remediation. Existing low-cost room-temperature NO 2 sensors often suffer from low sensitivity at the ppb level or long recovery times, reflecting the trade-off between sensor response and recovery time. Here, we report an atomically dispersed metal ion strategy to address it. We discover that bimetallic PbCdSe quantum dot (QD) gels containing atomically dispersed Pb ionic sites achieve the optimal combination of strong sensor response and fast recovery, leading to a high-performance room-temperature p-type semiconductor NO 2 sensor as characterized by a combination of ultra–low limit of detection, high sensitivity and stability, fast response and recovery. With the help of theoretical calculations, we reveal the high performance of the PbCdSe QD gel arises from the unique tuning effects of Pb ionic sites on NO 2 binding at their neighboring Cd sites.

36 MATERIALS SCIENCE↗

Observation of negative surface and interface energies of quantum dots

Surface energy is a fundamental property of materials and is particularly important in describing nanomaterials where atoms or molecules at the surface constitute a large fraction of the material. Traditionally, surface energy is considered to be a positive quantity, where atoms or molecules at the surface are less thermodynamically stable than their counterparts in the interior of the material because they have fewer bonds or interactions at the surface. Using calorimetric methods, we show that the surface energy is negative in some prototypical colloidal semiconductor nanocrystals, or quantum dots with organic ligand coatings. This implies that the surface atoms are more thermodynamically stable than those on the interior due to the strong bonds between these atoms and surfactant molecules, or ligands, that coat their surface. In addition, we extend this work to core/shell indium phosphide/zinc sulfide nanocrystals and show that the interfacial energy between these materials is highly thermodynamically favorable in spite of their large lattice mismatch. This work challenges many of the assumptions that have guided thinking about colloidal nanomaterial thermodynamics, investigates the fundamental stability of many technologically relevant colloidal nanomaterials, and paves the way for future experimental and theoretical work on nanocrystal thermodynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Controlled semiconductor quantum dot fabrication utilizing focus ion beam

In this project, we experimented the focused ion beam (FIB) based fabrications of semiconductor quantum dots (QDs) by using metal nano particles (NPs) (e.g., Al) on semiconductor as a template and by means of the FIB induced direct metal-to-QD conversion. We have examined effect of the experimental conditions, including Ga + ion energy and dose as well as substrate temperature. The results of experiments have shown AlGaSb QD formation on GaSb substrate can be achieved under certain conditions but there are many challenges about the techniques, including compositional nonuniformity of the QDs formed, partial conversion of the metal NP to QD, and high defect concentration in the QDs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Making Ternary Quantum Dots From Single-Source Precursors

A process has been devised for making ternary (specifically, CuInS2) nanocrystals for use as quantum dots (QDs) in a contemplated next generation of high-efficiency solar photovoltaic cells. The process parameters can be chosen to tailor the sizes (and, thus, the absorption and emission spectra) of the QDs.

Bailey, Sheila↗

Revealing the Phonon Bottleneck Limit in Negatively Charged CdS Quantum Dots

The capture of photoexcited hot electrons in semiconductors before they lose their excess energy to cooling is a long-standing goal in photon energy conversion. Semiconductor nanocrystals have large electron energy spacings that are expected to slow down electron relaxation by phonon emission, but hot electrons in photoexcited nanocrystals, nevertheless, cool rapidly by energy transfer to holes. This makes the intrinsic phonon-bottleneck-limited hot electron lifetime in nanocrystals elusive. For this work, we used a combination of theory and experiments to probe the hot-electron dynamics of negatively charged cadmium sulfide (CdS) colloidal quantum dots (QDs) in the absence of holes. Experiments found that these hot electrons cooled on a 100 ps time scale. Theoretical simulations predicted that pure phonon-bottleneck-limited hot electron cooling occurs on a similar time scale. This similarity suggests that the experimental measurements reflect the upper limit on the hot-electron lifetimes in these CdS QDs and the lower limit on the rates of processes that can harvest those hot electrons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Quantum Dot Nanobiosensor for Rapid Detection of Botulinum Neurotoxin Serotype E

Botulinum neurotoxins (BoNTs) are potent toxins produced by Clostridium bacteria that are responsible for the illness botulism and are listed as bioterrorism agents. BoNT serotype E (BoNT/E) is one of four BoNT serotypes that cause human botulism and is the second most frequent cause of foodborne botulism. Rapid detection and discrimination of BoNT serotypes implicated in human disease are critical for ensuring timely treatment of patients and identifying sources of toxins, but there have been few reported detection methods for BoNT/E and even fewer methods usable for BoNT serotyping. We report a nanobiosensor based on Forster resonance energy transfer (FRET) between semiconductor nanocrystals (quantum dots, QDs) and dark quencher-labeled peptide probes to detect biologically active BoNT/E in aqueous media. The peptide probes contain a specific cleavage site for active BoNT/E. QD photoluminescence, which changes intensity due to FRET when the peptide probe is cleaved, was used to indicate toxin presence and quantity. The detection of a BoNT/E light chain (LcE) and holotoxin was observed within 3 h. The limits of detection were 0.02 and 2 ng/mL for LcE and holotoxin, respectively. The nanobiosensor shows good specificity toward the target in tests with nontarget BoNT serotypes. The high sensitivity, simple operation, short detection time, and ability to be used in parallel with probes developed for other BoNT serotypes indicate that the nanobiosensor will be useful for rapid BoNT/E detection and serotype discrimination in food analysis.

botulinum neurotoxin E↗

Compositionally Tuning Electron Transfer from Photoexcited Core/Shell Quantum Dots via Cation Exchange

It is critical to find methods to control the thermodynamic driving force for photoexcited charge transfer from quantum dots (QDs) and explore how this affects charge transfer rates, since the efficiency of QD-based photovoltaic and photocatalysis technologies depends on both this rate and the associated energetic losses. In this work, we introduce a single-pot shell growth and Cu-catalyzed cation exchange method to synthesize Cd x Zn 1-x Se/Cd y Zn 1-y S QDs with tunable driving forces for electron transfer. Functionalizing them with two molecular electron acceptors—naphthalenediimide (NDI) and anthraquinone (AQ)—allowed us to probe nearly 1 eV of driving forces. For AQ, at lower driving forces, we find that higher Zn content results in a 130-fold increase of electron transfer rate constants. However, at higher driving forces electron transfer dynamics are unaltered. Here, the data are understood using an Auger-assisted electron transfer model and analyzed with computational work to determine approximate binding geometries of these electron acceptors. Our work provides a method to tune QD reducing power and produces useful metrics for optimizing QD charge transfer systems that maximize rates of electron transfer while minimizing energetic losses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metal Halide Perovskites in Quantum Dot Solar Cells: Progress and Prospects

“Go big or go home” could never be a truer statement, especially when it comes to energy. The world population is increasing, the energy use per person is growing more rapidly, and the total electricity use per person is growing even more quickly than that. To handle this demand, energy production must be increased, and it is vital for renewable sources to be used. Currently three quarters of a terawatt of power generated from photovoltaics (PVs) has been installed. At a somewhat optimistic average power-conversion efficiency of 18%, the distributed surface area of high purity optoelectronic grade semiconductor photovoltaic panels pointed at the sun is substantially larger than the area of the whole state of Rhode Island or nearly double the land mass of Luxembourg. While photovoltaic production continues to ramp to immense proportions, perovskite semiconductors are poised to greatly complement existing technology. On the other end of the size spectrum, the study of semiconductor nanocrystals or quantum dots (QDs) has led to advanced structures and deeper understanding within halide perovskite semiconductors. In this article, we show how the development of nanoscale metal halide perovskite semiconductors have gained prominence surpassing all other QD materials in terms of efficiency, and are becoming a platform for further improving technology to solve big energy challenges.

14 SOLAR ENERGY↗

Ultrafast hole relaxation dynamics in quantum dots revealed by two-dimensional electronic spectroscopy

Elucidating the population dynamics of correlated electron-hole pairs (bound excitons) in semiconducting quantum dots (QDs) is key for developing our fundamental understanding of nanoscale photophysics as well as for the optimal design of devices, such as lasers. For decades, it was assumed that holes did not contribute to band edge bleach signals in QDs. Here, we employ two-dimensional electronic spectroscopy to monitor electron and hole dynamics in both CdSe and CdSe/CdS/ZnS QDs to probe electron and hole dynamics. Based on a combination of time and frequency resolution, we observe a previously unresolved bleaching signal in CdSe QDs on timescales faster than 30 fs due to hole cooling. Atomistic semiempirical pseudopotential calculations are used to rationalize the order of magnitude difference in the observed hole dynamics in CdSe and CdSe/CdS/ZnS QDs. This picture advances our understanding of QD excitonics past the prevailing continuum effective mass theories generally used to describe QD electronic structure and dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Antibacterial Activity of Silver-Graphene Quantum Dots Nanocomposites Against Gram-Positive and Gram-Negative Bacteria

The invention provides a composite of silver nanoparticles decorated with graphene quantum dots (Ag-GQDs) using pulsed laser synthesis. The nanocomposites were functionalized with polyethylene glycol (PEG). A concentration of 150 .mu.g/mL of Ag-GQDs, a non-toxic level for human cells, exhibits strong antibacterial activity against both Gram-Positive and Gram-Negative Bacteria.

Habiba, Khaled↗

Enhancement in electro-optic performance of InAlGaAs/GaAs quantum dot lasers by ex situ thermal annealing

Here, this Letter reports the growth, fabrication, and characterization of molecular beam epitaxy (MBE)-grown quaternary InAlGaAs/GaAs quantum dot (QD) lasers emitting at sub-900 nm. The presence of Al in QD-based active regions acts as the origin of defects and non-radiative recombination centers. Applying optimized thermal annealing annihilates the defects in p-i-n diodes, thus lowering the reverse leakage current by six orders of magnitude compared to as-grown devices. A systematic improvement in the optical properties of the devices is also observed in the laser devices with increasing annealing time. At an annealing temperature of 700°C for 180 s, Fabry–Pérot lasers exhibit a lower pulsed threshold current density at infinite length of 570 A/cm 2 .

42 ENGINEERING↗

Electronic and Vibrational Spectra of InP Quantum Dots Formed by Sequential Ion Implantation

We have performed sequential ion implantation of indium and phosphorus into silica combined with controlled thermal annealing to fabricate InP quantum dots in a dielectric host. Electronic and vibrational spectra were measured for the as-implanted and annealed samples. The annealed samples show a peak in the infrared spectra near 320/cm which is attributed to a surface phonon mode and is in good agreement with the value calculated from Frolich's theory of surface phonon polaritons. The electronic spectra show the development of a band near 390 nm that is attributed to quantum confined InP.

Hall, C.↗