All‐optical modulation based on silicon quantum dot doped SiOx:Si‐QD waveguide

All‐optical modulation based on silicon quantum dot doped SiO_x:Si‐QD waveguide is demonstrated. By shrinking the Si‐QD size from 4.3 nm to 1.7 nm in SiO_x matrix (SiO_x:Si‐QD) waveguide, the free‐carrier absorption (FCA) cross section of the Si‐QD is decreased to 8 × 10⁻¹⁸ cm² by enlarging the electron/hole effective masses, which shortens the PL and Auger lifetime to 83 ns and 16.5 ps, respectively. The FCA loss is conversely increased from 0.03 cm⁻¹ to 1.5 cm⁻¹ with the Si‐QD size enlarged from 1.7 nm to 4.3 nm due to the enhanced FCA cross section and the increased free‐carrier density in large Si‐QDs. Both the FCA and free‐carrier relaxation processes of Si‐QDs are shortened as the radiative recombination rate is enlarged by electron–hole momentum overlapping under strong quantum confinement effect. The all‐optical return‐to‐zero on‐off keying (RZ‐OOK) modulation is performed by using the SiO_x:Si‐QD waveguides, providing the transmission bit rate of the inversed RZ‐OOK data stream conversion from 0.2 to 2 Mbit/s by shrinking the Si‐QD size from 4.3 to 1.7 nm.     

Spectroscopic study of oscillator strength and radiative decay time of colloidal CdSe quantum dots

Characterization of samples of cadmium selenide quantum dots (CdSe) QDs dissolved in toluene colloidal solutions at a concentration of 1.4 mg/ml was carried out through UV–Vis absorption and photoluminescence (PL) spectroscopy. The size-dependent absorption and red-shifted PL emission peak wavelengths could be tuned between 510–576 and 545–606 nm respectively. Optical absorption spectral measurements yielded CdSe QDs having diameters about ~ 2.44–3.69 nm with energy gaps 2.32–2.08 eV which are higher than the bulk CdSe (1.74 eV) reminiscent of quantum confinement. This is found to be in good agreement with the semi-empirical pseudopotential model. In addition, the first excitonic absorption transition 1S_(e)1S_3/2(h) oscillator strength and the corresponding fluorescence radiative decay time of CdSe QDs are assessed using relevant Einstein relations for absorption and emission in a two-level system. The elaborated calculations would anticipate that the transition oscillator scale with the CdSe QD radius as ~ R^2.54. Correspondingly, the calculated radiative decay times decrease from 56.4 to 23.2 ns which scale with CdSe QDs radius as ~ R^?2.155 in fairly good agreement with experimental values reported in the literature.     

Formation of InAs quantum dots at ultrahigh growth rates

We fabricated quantum dot (QD) structures at ultrahigh growth rates. Smaller fluctuations in QD size were observed when they were grown at a rate of 1.0 ML/s under conventional growth conditions (growth temperature of 500 °C and As₄ flux of 9×10⁻⁶ Torr). For QDs grown at high rates, growth interruption played an important role in the fabrication of QD structures; this was confirmed by carrying out reflection high-energy electron diffraction. Photoluminescence for QDs grown at high and low growth rates, with growth interruption and with low-temperature capping was observed at around 1250 nm at room temperature, indicating that high-quality QDs can be fabricated by employing high growth rates.     

Drop‐cast and dye‐sensitized ZnO nanorod‐based visible‐light photodetectors

We report the facile fabrication of metal–semiconductor–metal (MSM) photodetectors with dye‐sensitized ZnO nanorods (NRs) operating at wavelengths of ～405–638 nm by a simple drop casting method. The ZnO NRs were synthesized by the hydrothermal synthesis method at 75 °C. The droplet of ethanol solution containing ZnO NRs was dropped between two metal electrodes and dried at 65 °C, which allows the ZnO NRs to be adhered and contacted to both metal electrodes. When a violet light of 405 nm was illuminated into the MSM ZnO NRs‐based photodetector, the photocurrent gain was obtained as ～3.9 × 10³ at the applied bias voltage of 5 V. By increasing the bias voltage from 10 V to 15 V, the device exhibited good recovery performance with a largely reduced reset time from 85.68 s to 2.47 s and an increased on–off ratio from 17.9 to 77.4. To extend the photodetection range towards the long visible spectral region, the ZnO NRs were sensitized by the N719 dye and then drop‐cast. The dye‐sensitized ZnO NRs‐based photodetector also exhibited good photocurrent switching under 638 nm of light illumination. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

In Situ Self-Assembly of Quantum Dots at the Plasma Membrane Mediates Energy Transfer-Based Activation of Channelrhodopsin

The use of nanoparticle (NP) bioconjugates to control the activity of membrane ion channels has recently emerged as a new paradigm for the activation of electrically excitable cells. An NP-based strategy is reported for the specific activation of channelrhodopsin C1V1 (ChR-C1V1) expressed in the plasma membrane of HEK 293T/17 cells. Hydrophilic CdSe/ZnS core–shell semiconductor quantum dots (QDs) are self-assembled to the exofacial face of recombinantly expressed ChR-C1V1 by metal affinity-driven interaction of the QD ZnS shell with an N-terminal hexahistidine tag displayed on ChR-C1V1. This configuration enables the Förster resonance energy transfer (FRET)-based excitation and activation of the 11-cis-retinal moiety of ChR-C1V1 using the QD as a light harvesting transducer/energy donor. It is shown that the specific laser-induced opening of the ChR-C1V1 channel wherein the photoexcited QD (405 nm excitation, 530 nm emission) iteratively activates ChR-C1V1 channels as confirmed using the voltage-sensitive dye (VSD) bis-(1,3-diethylthiobarbituric acid)trimethine oxonol (DiSBAC ₂ (3)). In the absence of the QD transducer, excitation of ChR-C1V1-expressing cells at 405 nm results in no activation of ChR-C1V1. The results demonstrate the ability to controllably interface QDs with living cells for the activation of ChR membrane proteins and detail a new NP-bioconjugate hybrid system for the specific activation of ion channels.     

Fe<Subscript>3</Subscript>O<Subscript>4</Subscript> quantum dots on 3D-framed graphene aerogel as an advanced anode material in lithium-ion batteries

Three-dimensional fabricated Fe₃O₄ quantum dots/graphene aerogel materials (Fe₃O₄ QDs/GA) were obtained from a facile hydrothermal strategy, followed by a subsequently heat treatment process. The Fe₃O₄ QDs (2–5 nm) are anchored tightly and dispersed uniformly on the surface of three-dimensional GA. The as-prepared anode materials exhibit a high reversible capacity of 1078 mAh g^?1 at a current density of 100 mA g^?1 after 70 cycles in lithium-ion batteries (LIBs) system. Moreover, the rate capacity still remains 536 mAh g^?1 at 1000 mA g^?1. The enhanced electrochemical performance is attributed to that the GA not only acts as a three-dimensional electronic conductive matrix for the fast transportation of Li⁺ and electrons, but also provides with double protection against the aggregation and pulverization of Fe₃O₄ QDs during cycling. Apparently, the synergistic effects of the three-dimensional GA and the quantum dots are fully utilized. Therefore, the Fe₃O₄ QDs/GA composites are promising materials as advanced anode materials for LIBs.     

Ultrasensitive PbS‐Quantum‐Dot Photodetectors for Visible–Near‐Infrared Light Through Surface Atomic‐Ligand Exchange

A surface atomic‐ligand exchange method is applied the first time in the construction of photodetectors (PDs) based on PbS quantum dots (QDs) for ultrasensitivity. The device thus produces a high photosensitivity to visible and near‐infrared light with a photoresponsivity up to 7.5 × 10³ A W^?1 and a high stability in air. In particular, these PbS‐QD‐based PDs show the capability of following a pulse light with a frequency up to 100 kHz well at a relatively fast response time/recovery time of ≈4/40 μs, much faster than most previous QD‐based PDs. The short response time is attributed to modification for the surface of the PbS‐QDs by cetyltrimethylammonium bromide treatment, which effectively improves the contact between the QDs and the Au electrodes, leading to extracting a high carrier mobility (≈0.142 cm² V^?1 s^?1). These findings show the great potential of PbS‐QDs as high‐speed nano‐photodetectors, and, more importantly, demonstrate the importance of the surface atomic‐ligand exchange method in the construction of QD‐based devices.     

Exploring spatial resolution in high-sensitivity nanogap quantum dot photodetectors

We propose a new approach to experimentally determine the spatial resolution of nanogap quantum dot (QD) photodetectors consist of solution-processed QDs. Cross talk between a pair of closely positioned QD photodetectors was measured. Devices with 200?nm spacing exhibit low crosstalk of 8.4%. A single QD photodetector also shows high sensitivity, with a lowest detectable optical intensity of 95.3 fW/μm² achieved. The results show the potential of nanogap QD photodetectors for applications in high-density imaging/sensing arrays.     

Differential capacitance of hybrid organic/inorganic CdSe/ZnS quantum dots light-emitting device

We have studied the differential capacitance of self-assembly hybrid organic/inorganic quantum dot (QD) light-emitting devices (QD-OLEDs) at room temperature in the frequency range of 1×10³ to 1×10⁶ Hz. Self-assembly CdSe/ZnS QDs monolayer was used to fabricate trilayer hybrid QD-OLEDs on indium tin oxide coated glass substrates. We observed negative differential capacitance (NDC) in both OLED and QD-OLEDs for the first time in the intermediate frequency range of 5×10³ to 5×10⁵ Hz. The onset and frequency range of NDC are strongly depended on the applied bias voltage. This behavior is described by a mathematical model. The simulated results showed that the NDC was due to the time-dependent transient current from the QDs and organic/metal interfacial states in the device. The probable mechanisms of NDC in organic devices are discussed.     

Improvement of the optical property and uniformity of self-assembled InAs/InGaAs quantum dots by layer-by-layer temperature and substrate rotation

The influence of layer-by-layer temperature and substrate rotation on the optical property and uniformity of self-assembled InAs/In_0.2Ga_0.8As/GaAs quantum dots (QDs) gown with an As₂ source was investigated. An improvement in the optical property of QDs was obtained by the precise control and optimization of growth temperature utilized for each layer, i.e., InAs QDs, InGaAs quantum wells, GaAs barriers and AlGaAs layers, respectively. By using a substrate rotation, the QD density increased from ∼1.4×10¹⁰ to ∼3.2×10¹⁰ cm⁻² and its size also slightly increased, indicating a good quality of QDs. It is found that the use of an appropriate substrate rotation during growth improves the room-temperature (RT) optical property and uniformity of QDs across the wafer. For the QD sample with a substrate rotation of 6 rpm, the RT photoluminescence (PL) intensity is much higher and the standard deviation of RT-PL full-width at half-maximum is decreased by 35% compared to that grown without substrate rotation.     

Energy transfer in associates of semiconductor quantum dots with tetrapyridinoporphyrazine molecules

The interaction of CdSe/ZnS quantum dots (QDs) with metal-free tetrapyridinoporphyrazine (TPPA) molecules in chloroform has been investigated. It was found that, at QD concentrations lower than ～3 × 10^?7 M, QD luminescence is quenched in the presence of TPPA and characteristic changes occur in the absorption and luminescence spectra of TPPA, which reflect the interaction of TPPA molecules with the QD surface. Along with the QD luminescence quenching, sensitized luminescence of TPPA molecules adsorbed on QDs was observed. The luminescence excitation spectra of adsorbed TPPA molecules unambiguously indicate the presence of energy transfer from QDs to TPPA. The efficiency of energy transfer from QDs to TPPA is estimated from the quantum yield of sensitized TPPA luminescence.     

Mid-infrared photodetectors based on quaternary InAsSbP nanostructures

Quaternary InAsSbP quantum dots (QD) with the surface concentration of (3–5)×10⁹ cm⁻² have been grown on the InAs(100) substrate by the modified version of liquid-phase epitaxy. Morphology and distribution of densities of QDs were studied by means of atomic-force microscope. Diameter distribution of QDs was revealed to be Gaussian. The mean value of QD diameter is 23.1 nm with the variance of 6.9 nm. Two types of infrared photodetectors (IRPD) on the basis of InAs(100), with and without InAsSbP-QDs on the substrate surface, were fabricated and studied. Spectra of photoresponse of both types of IRPD at room temperature were measured and analyzed and a red shift was revealed for structures with QDs. Capacitance characteristics of IRPD and relative change in their surface resistance after irradiation with cw He-Ne laser have been studied.     

Synthesis of 2-Mercaptonicotinic Acid-Capped CdSe Quantum Dots and its Application to Spectrofluorometric Determination of Cr(VI) in Water Samples

The CdSe quantum dots (QDs) capped with 2-mercaptonicotinic acid (H₂MN) were prepared through a controllable process at 80 °C. The prepared QDs were characterized by XRD, TEM, IR, UV–Vis and fluorescence (FL) techniques. It was found that the QDs were nearly mono-disperse with the diameters in the range of 8–10 nm. These QDs are capable to exhibit strong FL even in concentrated acidic media. They exhibit an enhanced fluorescence in the presence of Cr(VI), which was used for the determination of Cr(VI) in water samples. The linear range was found to be 1?×?10^?7–6.0?×?10^?6 M with the RSD and DL of 0.92 % and 5?×?10^?8 M, respectively. Except that Ca²⁺ and Fe³⁺ which can be eliminated through a simple precipitation process, the other co-existent ions present in natural water were not interfered. The recoveries obtained for the added amounts of Cr(VI) were in the range of 96.9–103.2 %, which denote on application of the method, satisfactorily.     

Luminescence of CdS:Ag Quantum Dots in a Polymethacrylate Matrix

Semiconductor quantum dots (QDs) exhibit intense luminescence and reproduce optical characteristics. Doping with metal ions has a positive effect on their properties. Introduction of QDs into polymer matrices leads to the formation of a required morphology of composites. There is a problem in synthesis of optically transparent polymer composites containing QDs of the А²В⁶ group that consists in the extremely low solubility of metal chalcogenides and most of their precursors in monomers. To solve this problem, we used colloidal synthesis. CdS QDs were synthesized by the method of appearing reagents in situ in methylmethacrylate (MMA). Doping with Ag⁺ ions was performed by adding a silver salt into the reaction mixture during the synthesis of CdS QDs. The PMMA/CdS:Ag luminescent polymer glasses were synthesized by radical block polymerization of MMA. The transparency of the composites at wavelengths exceeding 500 nm reaches 92% (5 mm). The luminescence excitation is related to the interband electron transitions in CdS crystals. Luminescence in the range of 500–600 nm is observed due to electron relaxation via a system of levels in the band gap of doped CdS crystals. The positions and intensities of the spectral bands depend on the Ag⁺ concentration, particle size, excitation wavelength, and other factors. The formation of Cd(Ag)S/Ag₂S structures at Ag⁺ concentrations higher than 5.0 × 10^–3 mol/L quenches the luminescence.     

Generation of MoS<Subscript>2</Subscript> quantum dots by laser ablation of MoS<Subscript>2</Subscript> particles in suspension and their photocatalytic activity for H<Subscript>2</Subscript> generation

MoS₂ quantum dots (QDs) have been obtained in colloidal suspensions by 532 nm laser ablation (7 ns fwhp/pulse, 50 mJ/pulse) of commercial MoS₂ particles in acetonitrile. High-resolution transmission electron microscopy images show a lateral size distribution from 5 to 20 nm, but a more homogeneous particle size of 20 nm can be obtained by silica gel chromatography purification in acetonitrile. MoS₂ QDs obtained by laser ablation are constituted by 3–6 MoS₂ layers (1.8–4 nm thickness) and exhibit photoluminescence whose λ_PL varies from 430 to 530 nm depending on the excitation wavelength. As predicted by theory, the confinement effect and the larger periphery in MoS₂ QDs increasing the bandgap and having catalytically active edges are reflected in an enhancement of the photocatalytic activity for H₂ generation upon UV–Vis irradiation using CH₃OH as sacrificial electron donor due to the increase in the reduction potential of conduction band electrons and the electron transfer kinetics.     

The transport properties of Dirac fermions in chemical vapour-deposited single-layer graphene

Abstract

The electronic transport properties of Dirac fermions in chemical vapour-deposited single-layer epitaxial graphene on anSiO₂/Si substrate have been investigated using the Shubnikov–de Haas (SdH) oscillations technique. The magnetoresistance measurements were performed in the temperature range between 1.8 and 43 K and at magnetic fields up to 11 T. The 2D carrier density and the Fermi energy have been determined from the period of the SdH oscillations. In addition, the in-plane effective mass as well as the quantum lifetime of 2D carriers have been calculated from the temperature and magnetic field dependences of the SdH oscillation amplitude. The sheet carrier density (1.42 × 10¹³ cm^?2 at 1.8 K), obtained from the low-field Hall Effect measurements, is larger than that of 2D carrier density (8.13 × 10¹² cm^?2). On the other hand, the magnetoresistance includes strong magnetic field dependent positive, non-oscillatory background magnetoresistance. The strong magnetic field dependence of the magnetoresistance and the differences between sheet carrier and 2D carrier density can be attributed to the 3D carriers between the graphene sheet and the SiO₂/Si substrate.     

Photoluminescence from Zinc Oxide Quantum Dots Embedded in Silicon Dioxide Matrices

ABSTRACT

ZnO quantum dots (QDs) embedded in SiO₂ matrix are fabricated by ion implantation and annealing treatment methods. When the Zn-doping dose is (2, 3, 5, and 7) × 10¹⁶ cm^?2, the size of quantum dots is in the range of ～4–10 nm in diameter according to the XRD and HR-TEM results. Ultraviolet and green light emissions from the specimen are obtained at room temperature. With the increase of the Zn-doping dose, the PL peak in the ultraviolet region red shifts from 3.32 to 3.10 eV. This PL peak is related to the size of ZnO QDs, which is ascribed to the free exciton recombination in QDs. The green light emissions centered at 2.43 and 2.25 eV are independent of the Zn-doping dose and annealing temperature, which are attributed to the deep-level defect and the small peroxy radical (SPR) defect, respectively.     

Raman spectroscopy of very small Cd1−xCoxS quantum dots grown by a novel protocol: direct observation of acoustic‐optical phonon coupling

Glass‐embedded Cd_1−xCo_xS quantum dots (QDs) with mean radius of R ≈ 1.70 nm were successfully synthesized by a novel protocol on the basis of the melting‐nucleation synthesis route and herein investigated by several experimental techniques. Incorporation of Co²⁺ ions into the QD lattice was evidenced by X‐ray diffraction and magnetic force microscopy results. Optical absorption features with irregular spacing in the ligand field region confirmed that the majority of the incorporated Co²⁺ ions are under influence of a low‐symmetry crystal field located near to the Cd_1−xCo_xS QD surface. Electron paramagnetic resonance data confirmed the presence of Co²⁺ ions in a highly inhomogeneous crystal field environment identified at the interface between the hosting glass matrix (amorphous) and the crystalline QD. The acoustic‐optical phonon coupling in the Cd_1−xCo_xS QDs (x ≠ 0.000) was directly observed by Raman measurements, which have shown a high‐frequency shoulder of the longitudinal optical phonon peak. This effect is tuned by the size‐dependent sp‐d exchange interaction due to the magnetic doping, causing variations in the coupling between electrons and longitudinal optical phonon. Copyright © 2013 John Wiley & Sons, Ltd.     

The effect of spacer layer thickness on vertical alignment of InGaAs/GaNAs quantum dots grown on GaAs(3 1 1)B substrate

We fabricated multiple stacked self-organized InGaAs quantum dots (QDs) on GaAs (3 1 1)B substrate by atomic hydrogen-assisted molecular beam epitaxy (H-MBE) to realize an ordered three-dimensional QD array. High quality stacked QDs with good size uniformity were achieved by using strain-compensation growth technique, in which each In_0.35Ga_0.65As QD layer was embedded by GaNAs strain-compensation layer (SCL). In order to investigate the effect of spacer layer thickness on vertical alignment of InGaAs/GaNAs QDs, the thickness of GaNAs SCL was varied from 40 to 20 nm. We observed that QDs were vertically aligned in [3 1 1] direction when viewed along [0 1 −1], while the alignment was inclined when viewed along [−2 3 3] for all samples with different SCL thickness. This is due to their asymmetric shape along [−2 3 3] with two different dominant facets thereby the local strain field around QD extends further outward from the lower-angle facet. Furthermore, the inclination angle of vertical alignment QDs became monotonously smaller from 22° to 2° with decreasing SCL thickness from 40 to 20 nm. These results suggest that the strain field extends asymmetrically resulting in vertically tilted alignment of QDs for samples with thick SCLs, while the propagated local strain field is strong enough to generate the nucleation site of QD formation just above lower QD in the sample with thinner SCLs.     

基于PdSe2/GaAs异质结的高灵敏近红外光伏型探测器的制备和图像传感的应用

本文制备了一种基于PdSe₂/GaAs异质结的高灵敏近红外光电探测器，该探测器是通过将多层PdSe₂薄膜转移到平面GaAs上制成的. 所制备的PdSe₂/GaAs异质结器件在808 nm光照下表现出明显的光伏特性，这表明近红外光电探测器可以用作自驱动器件. 进一步的器件分析表明，这种杂化异质结在零偏电压和808 nm光照下具有1.16×10⁵的高开关比. 光电探测器的响应度和比探测度分别约为171.34 mA/W和2.36×10¹¹ Jones. 而且，该器件显示出优异的稳定性和可靠的重复性. 在空气中2个月后，近红外光电探测器的光电特性几乎没有下降，这归因于PdSe₂的良好稳定性. 最后，基于PdSe₂/GaAs的异质结器件还可以用作近红外光传感器.