Bioengineered II-VI semiconductor quantum dot-carboxymethylcellulose nanoconjugates as multifunctional fluorescent nanoprobes for bioimaging live cells

NASA Astrophysics Data System (ADS)

Mansur, Alexandra A. P.; Mansur, Herman S.; Mansur, Rafael L.; de Carvalho, Fernanda G.; Carvalho, Sandhra M.

2018-01-01

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 5.0 nm 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.

Subpicosecond Photoinduced Hole Transfer from a CdS Quantum Dot to a Molecular Acceptor Bound Through an Exciton-Delocalizing Ligand.

PubMed

Lian, Shichen; Weinberg, David J; Harris, Rachel D; Kodaimati, Mohamad S; Weiss, Emily A

2016-06-28

This paper describes the enhancement of the rate of hole transfer from a photoexcited CdS quantum dot (QD), with radius R = 2.0 nm, to a molecular acceptor, phenothiazine (PTZ), by linking the donor and acceptor through a phenyldithiocarbamate (PTC) linker, which is known to lower the confinement energy of the excitonic hole. Upon adsorption of PTC, the bandgap of the QD decreases due to delocalization of the exciton, primarily the excitonic hole, into interfacial states of mixed QD/PTC character. This delocalization enables hole transfer from the QD to PTZ in <300 fs (within the instrument response of the laser system) when linked by PTC, but not when linked by a benzoate group, which has a similar length and conjugation as PTC but does not delocalize the excitonic hole. Comparison of the two systems was aided by quantification of the surface coverage of benzoate and PTC-linked PTZ by (1)H NMR. This work provides direct spectroscopic evidence of the enhancement of the rate of hole extraction from a colloidal QD through covalent linkage of a hole acceptor through an exciton-delocalizing ligand.

Colloidal-Quantum-Dot Ring Lasers with Active Color Control.

PubMed

le Feber, Boris; Prins, Ferry; De Leo, Eva; Rabouw, Freddy T; Norris, David J

2018-02-14

To improve the photophysical performance of colloidal quantum dots for laser applications, sophisticated core/shell geometries have been developed. Typically, a wider bandgap semiconductor is added as a shell to enhance the gain from the quantum-dot core. This shell is designed to electronically isolate the core, funnel excitons to it, and reduce nonradiative Auger recombination. However, the shell could also potentially provide a secondary source of gain, leading to further versatility in these materials. Here we develop high-quality quantum-dot ring lasers that not only exhibit lasing from both the core and the shell but also the ability to switch between them. We fabricate ring resonators (with quality factors up to ∼2500) consisting only of CdSe/CdS/ZnS core/shell/shell quantum dots using a simple template-stripping process. We then examine lasing as a function of the optical excitation power and ring radius. In resonators with quality factors >1000, excitons in the CdSe cores lead to red lasing with thresholds at ∼25 μJ/cm 2 . With increasing power, green lasing from the CdS shell emerges (>100 μJ/cm 2 ) and then the red lasing begins to disappear (>250 μJ/cm 2 ). We present a rate-equation model that can explain this color switching as a competition between exciton localization into the core and stimulated emission from excitons in the shell. Moreover, by lowering the quality factor of the cavity we can engineer the device to exhibit only green lasing. The mechanism demonstrated here provides a potential route toward color-switchable quantum-dot lasers.

Electronic structure robustness and design rules for 2D colloidal heterostructures

NASA Astrophysics Data System (ADS)

Chu, Audrey; Livache, Clément; Ithurria, Sandrine; Lhuillier, Emmanuel

2018-01-01

Among the colloidal quantum dots, 2D nanoplatelets present exceptionally narrow optical features. Rationalizing the design of heterostructures of these objects is of utmost interest; however, very little work has been focused on the investigation of their electronic properties. This work is organized into two main parts. In the first part, we use 1D solving of the Schrödinger equation to extract the effective masses for nanoplatelets (NPLs) of CdSe, CdS, and CdTe and the valence band offset for NPL core/shell of CdSe/CdS. In the second part, using the determined parameters, we quantize how the spectra of the CdSe/CdS heterostructure get affected by (i) the application of an electric field and (ii) by the presence of a dull interface. We also propose design strategies to make the heterostructure even more robust.

Optical and AFM study of electrostatically assembled films of CdS and ZnS colloid nanoparticles

NASA Astrophysics Data System (ADS)

Suryajaya; Nabok, A.; Davis, F.; Hassan, A.; Higson, S. P. J.; Evans-Freeman, J.

2008-05-01

CdS and ZnS semiconducting colloid nanoparticles coated with the organic shell, containing either SO 3- or NH 2+ groups, were prepared using the aqueous phase synthesis. The multilayer films of CdS (or ZnS) were deposited onto glass, quartz and silicon substrates using the technique of electrostatic self-assembly. The films produced were characterized with UV-vis spectroscopy, spectroscopic ellipsometry and atomic force microscopy. A substantial blue shift of the main absorption band with respect to the bulk materials was found for both CdS and ZnS films. The Efros equation in the effective mass approximation (EMA) theoretical model allowed the evaluation of the nanoparticle radius of 1.8 nm, which corresponds well to the ellipsometry results. AFM shows the formation of larger aggregates of nanoparticles on solid surfaces.

Cadmium sulfide quantum dots induce oxidative stress and behavioral impairments in the marine clam Scrobicularia plana.

PubMed

Buffet, Pierre-Emmanuel; Zalouk-Vergnoux, Aurore; Poirier, Laurence; Lopes, Christelle; Risso-de-Faverney, Christine; Guibbolini, Marielle; Gilliland, Douglas; Perrein-Ettajani, Hanane; Valsami-Jones, Eugenia; Mouneyrac, Catherine

2015-07-01

Cadmium sulfide (CdS) quantum dots have a number of current applications in electronics and solar cells and significant future potential in medicine. The aim of the present study was to examine the toxic effects of CdS quantum dots on the marine clam Scrobicularia plana exposed for 14 d to these nanomaterials (10 µg Cd L(-1) ) in natural seawater and to compare them with soluble Cd. Measurement of labile Cd released from CdS quantum dots showed that 52% of CdS quantum dots remained in the nanoparticulate form. Clams accumulated the same levels of Cd regardless of the form in which it was delivered (soluble Cd vs CdS quantum dots). However, significant changes in biochemical responses were observed in clams exposed to CdS quantum dots compared with soluble Cd. Increased activities of catalase and glutathione-S-transferase were significantly higher in clams exposed in seawater to Cd as the nanoparticulate versus the soluble form, suggesting a specific nano effect. The behavior of S. plana in sediment showed impairments of foot movements only in the case of exposure to CdS quantum dots. The results show that oxidative stress and behavior biomarkers are sensitive predictors of CdS quantum dots toxicity in S. plana. Such responses, appearing well before changes might occur at the population level, demonstrate the usefulness of this model species and type of biomarker in the assessment of nanoparticle contamination in estuarine ecosystems. © 2015 SETAC.

Influence of thermally induced structural and morphological changes, and UV irradiation on photoluminescence and optical absorption behavior of CdS nanoparticles

NASA Astrophysics Data System (ADS)

Osman, M. A.; El-Said, Waleed A.; Othman, A. A.; Abd-Elrahim, A. G.

2016-04-01

Polycrystalline cubic CdS nanoparticles (NPs) with a crystallite size ({{D}\\text{Sch}} ) ~3 nm were synthesized by chemical precipitation method at room temperature. Thermal induced structural and morphological changes have been investigated using x-ray diffraction, high-resolution transmission electron microscope, x-ray fluorescence, Fourier transform infrared and Raman spectroscopy. The influence of these changes on optical absorption and photoluminescence (PL) characteristics have been studied. It was found that increasing annealing temperature (T a), results in structural phase transitions at 300 and 700 °C, increasing {{D}\\text{Sch}} and red shift of the optical band gap (E\\text{g}\\text{opt} ) due to the improvement in crystallinity. The photoluminescence emission spectrum of nonstoichiometric CdS (Cd-rich) nanopowder reveals emission bands at 365, 397, and 434 nm. Furthermore, PL spectrum of colloidal solution exhibits additional green and red emission bands at 535, 570 and 622 nm. To explain the mechanism of PL emission in CdS NPs, trapping and radiative recombination levels have been identified and the corresponding energy band diagrams are suggested. Annealing process results in an overall enhancement in PL intensity due to the improvement in crystallinity associated with the reduction of nonradiative surface state defects. Irradiation of CdS NPs colloidal solution at UV irradiation dose  <13 J cm-2 leads to the enhancement of PL quantum efficiency and blue shift of E\\text{g}\\text{opt} (i.e. photo-brightening) due to the decrease in the particle size deduced from Brus equation ≤ft({{D}\\text{Brus}}\\right) , This behavior is due to UV irradiation effects such as photopolymerization, the formation of CdSO4 passivation layers due to photooxidation and the reduction in {{D}\\text{Brus}} by photocorrosion process. At UV irradiation dose  <13 J cm-2, PL emission intensity continuously enhances without any change in both E\\text{g}\\text{opt} and {{D}\\text{Brus}} . This behavior is discussed in terms of electron filling model. Boltzmann curve fitting successfully describes the dependence of both {{D}\\text{Brus}} and E\\text{g}\\text{opt} on UV irradiation dose.

Structural and optoelectronic studies on Ag-CdS quantum dots

NASA Astrophysics Data System (ADS)

Ibrahim Mohammed S., M.; Gubari, Ghamdan M. M.; Huse, Nanasaheb P.; Dive, Avinash S.; Sharma, Ramphal

2018-05-01

In the present study, we have successfully deposited CdS quantum dot thin films and Ag doped CdS on a glass slide by simple and economical chemical bath deposition at room temperature. The X-ray diffraction method analysis reveals that CdS thin films exhibit hexagonal structure when compared with standard JCPDS data. The estimated average crystallite size of the quantum dots and resulted in the least crystallite size of ˜9 nm. a comparison between the optical and electrical properties of the films before and after doping Ag was made through measuring and analyzing the curves for UV and I-V. From UV absorption spectra we observed that the samples exhibited a band edge near ˜400 nm with a slight deviation with the presence of excitonic peak for both CdS and Ag doped CdS. The presence of excitonic peak may be referred to the formation of quantum dots. The calculated band gap energy of thin films was found to be 3.45 eV and 3.15 eV for both CdS and Ag doped CdS thin films respectively, where the optical absorption spectra of Ag doped CdS nanoparticles also exhibit shift with respect to that of CdS quantum dots thin films. The photosensitive of CdS thin films show an increase in photocurrent when Ag doped CdS.

Direct observation of the core/double-shell architecture of intense dual-mode luminescent tetragonal bipyramidal nanophosphors

NASA Astrophysics Data System (ADS)

Kim, Su Yeon; Jeong, Jong Seok; Mkhoyan, K. Andre; Jang, Ho Seong

2016-05-01

Highly efficient downconversion (DC) green-emitting LiYF4:Ce,Tb nanophosphors have been synthesized for bright dual-mode upconversion (UC) and DC green-emitting core/double-shell (C/D-S) nanophosphors--Li(Gd,Y)F4:Yb(18%),Er(2%)/LiYF4:Ce(15%),Tb(15%)/LiYF4--and the C/D-S structure has been proved by extensive scanning transmission electron microscopy (STEM) analysis. Colloidal LiYF4:Ce,Tb nanophosphors with a tetragonal bipyramidal shape are synthesized for the first time and they show intense DC green light via energy transfer from Ce3+ to Tb3+ under illumination with ultraviolet (UV) light. The LiYF4:Ce,Tb nanophosphors show 65 times higher photoluminescence intensity than LiYF4:Tb nanophosphors under illumination with UV light and the LiYF4:Ce,Tb is adapted into a luminescent shell of the tetragonal bipyramidal C/D-S nanophosphors. The formation of the DC shell on the core significantly enhances UC luminescence from the UC core under irradiation of near infrared light and concurrently generates DC luminescence from the core/shell nanophosphors under UV light. Coating with an inert inorganic shell further enhances the UC-DC dual-mode luminescence by suppressing the surface quenching effect. The C/D-S nanophosphors show 3.8% UC quantum efficiency (QE) at 239 W cm-2 and 73.0 +/- 0.1% DC QE. The designed C/D-S architecture in tetragonal bipyramidal nanophosphors is rigorously verified by an energy dispersive X-ray spectroscopy (EDX) analysis, with the assistance of line profile simulation, using an aberration-corrected scanning transmission electron microscope equipped with a high-efficiency EDX. The feasibility of these C/D-S nanophosphors for transparent display devices is also considered.Highly efficient downconversion (DC) green-emitting LiYF4:Ce,Tb nanophosphors have been synthesized for bright dual-mode upconversion (UC) and DC green-emitting core/double-shell (C/D-S) nanophosphors--Li(Gd,Y)F4:Yb(18%),Er(2%)/LiYF4:Ce(15%),Tb(15%)/LiYF4--and the C/D-S structure has been proved by extensive scanning transmission electron microscopy (STEM) analysis. Colloidal LiYF4:Ce,Tb nanophosphors with a tetragonal bipyramidal shape are synthesized for the first time and they show intense DC green light via energy transfer from Ce3+ to Tb3+ under illumination with ultraviolet (UV) light. The LiYF4:Ce,Tb nanophosphors show 65 times higher photoluminescence intensity than LiYF4:Tb nanophosphors under illumination with UV light and the LiYF4:Ce,Tb is adapted into a luminescent shell of the tetragonal bipyramidal C/D-S nanophosphors. The formation of the DC shell on the core significantly enhances UC luminescence from the UC core under irradiation of near infrared light and concurrently generates DC luminescence from the core/shell nanophosphors under UV light. Coating with an inert inorganic shell further enhances the UC-DC dual-mode luminescence by suppressing the surface quenching effect. The C/D-S nanophosphors show 3.8% UC quantum efficiency (QE) at 239 W cm-2 and 73.0 +/- 0.1% DC QE. The designed C/D-S architecture in tetragonal bipyramidal nanophosphors is rigorously verified by an energy dispersive X-ray spectroscopy (EDX) analysis, with the assistance of line profile simulation, using an aberration-corrected scanning transmission electron microscope equipped with a high-efficiency EDX. The feasibility of these C/D-S nanophosphors for transparent display devices is also considered. Electronic supplementary information (ESI) available: XRD patterns, PL and PLE spectra, SEM and HR-TEM images, PL decay times, photographs showing the transparent nanophosphor solutions and their dual-mode luminescence, and additional EDX data. See DOI: 10.1039/c5nr05722a

Colloidal synthesis of monodispersed ZnS and CdS nanocrystals from novel zinc and cadmium complexes

NASA Astrophysics Data System (ADS)

Onwudiwe, Damian C.; Mohammed, Aliyu D.; Strydom, Christien A.; Young, Desmond A.; Jordaan, Anine

2014-06-01

Monodispersed spherical and hexagonal shaped ZnS and CdS nanocrystals respectively, have been synthesized using novel heteroleptic complexes of xanthate (S2CObu) and dithiocarbamate (S2CNMePh). The nanocrystals were prepared via colloidal route and stabilized in hexadecylamine (HDA). The morphology of the as-prepared nanocrystals was characterized using transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), and powdered X-ray diffraction (p-XRD) analysis. An average diameter of 7.2 nm and 8.6 nm were obtained for the ZnS and CdS respectively. The optical properties of the nanoparticles studied by UV-vis and photoluminescence (PL) spectroscopy showed a blue shift in the absorption spectra, and band edge emission respectively.

Strain-Driven Stacking Faults in CdSe/CdS Core/Shell Nanorods.

PubMed

Demortière, Arnaud; Leonard, Donovan N; Petkov, Valeri; Chapman, Karena; Chattopadhyay, Soma; She, Chunxing; Cullen, David A; Shibata, Tomohiro; Pelton, Matthew; Shevchenko, Elena V

2018-04-19

Colloidal semiconductor nanocrystals are commonly grown with a shell of a second semiconductor material to obtain desired physical properties, such as increased photoluminescence quantum yield. However, the growth of a lattice-mismatched shell results in strain within the nanocrystal, and this strain has the potential to produce crystalline defects. Here, we study CdSe/CdS core/shell nanorods as a model system to investigate the influence of core size and shape on the formation of stacking faults in the nanocrystal. Using a combination of high-angle annular dark-field scanning transmission electron microscopy and pair-distribution-function analysis of synchrotron X-ray scattering, we show that growth of the CdS shell on smaller, spherical CdSe cores results in relatively small strain and few stacking faults. By contrast, growth of the shell on larger, prolate spheroidal cores leads to significant strain in the CdS lattice, resulting in a high density of stacking faults.

Influence of Cd2+/S2- molar ratio and of different capping environments in the optical properties of CdS nanoparticles incorporated within a hybrid diureasil matrix

NASA Astrophysics Data System (ADS)

Gonçalves, Luis F. F. F.; Silva, Carlos J. R.; Kanodarwala, Fehmida K.; Stride, John A.; Pereira, Mario R.; Gomes, Maria J. M.

2014-09-01

The incorporation of CdS nanoparticles (NPs), as prepared through colloidal methods using reverse micelles, within diureasil hybrid organic-inorganic sol-gel matrices was investigated. Several experimental conditions, namely the influence of capping agent 3-mercaptopropyltrimethoxysilane (MPTMS) or the use of tetraethoxysilane (TEOS), were studied in order to assure the preservation of the original optical properties of colloidal CdS NPs after the incorporation of the NPs within the solid diureasil hybrid matrix. The diureasil matrix is based on a siliceous network cross linked through urea bonds to poly(oxyethylene)/poly(oxypropylene) (PEO/PPO) chains. The influence of the Cd2+/S2- molar ratio of the NPs in the stability and dispersion of the NPs within the diureasil matrix was also investigated. The obtained CdS doped hybrid matrix was characterized by absorption, steady-state and time-resolved photoluminescence (PL) spectroscopy and by transmission electron microscopy (TEM). The stability of the CdS NPs within the hybrid matrix showed to be dependent on the Cd2+/S2- molar ratio used in the synthesis of the NPs. The use of MPTMS proved to be crucial in the preservation of the original optical properties of the colloidal CdS NPs after the incorporation of the NPs within the hybrid matrix. The effect of MPTMS was in turn influenced by the Cd2+/S2- molar ratio employed in the synthesis of the CdS NPs. The use of MPTMS was less effective when Cd2+/S2- molar ratio equal to 0.5 was used. In the absence of MPTMS or TEOS larger NPs size distribution and clustering of the CdS NPs were obtained after the transfer of the NPs into the hybrid matrix.

Simulation of MeV electron energy deposition in CdS quantum dots absorbed in silicate glass for radiation dosimetry

NASA Astrophysics Data System (ADS)

Baharin, R.; Hobson, P. R.; Smith, D. R.

2010-09-01

We are currently developing 2D dosimeters with optical readout based on CdS or CdS/CdSe core-shell quantum-dots using commercially available materials. In order to understand the limitations on the measurement of a 2D radiation profile the 3D deposited energy profile of MeV energy electrons in CdS quantum-dot-doped silica glass have been studied by Monte Carlo simulation using the CASINO and PENELOPE codes. Profiles for silica glass and CdS quantum-dot-doped silica glass were then compared.

Designing Selectivity in Metal-Semiconductor Nanocrystals: Synthesis, Characterization, and Self-Assembly

NASA Astrophysics Data System (ADS)

Pavlopoulos, Nicholas George

This dissertation contains six chapters detailing recent advances that have been made in the synthesis and characterization of metal-semiconductor hybrid nanocrystals (HNCs), and the applications of these materials. Primarily focused on the synthesis of well-defined II-VI semiconductor nanorod (NR) and tetrapod (TP) based constructs of interest for photocatalytic and solar energy applications, the research described herein discusses progress towards the realization of key design rules for the synthesis of functional semiconductor nanocrystals (NCs). As such, a blend of novel synthesis, advanced characterization, and direct application of heterostructured nanoparticles are presented. The first chapter is a review summarizing the design, synthesis, properties, and applications of multicomponent nanomaterials composed of disparate semiconductor and metal domains. By coupling two compositionally distinct materials onto a single nanocrystal, synergistic properties can arise that are not present in the isolated components, ranging from self-assembly to photocatalysis. For semiconductor nanomaterials, this was first realized in the ability to tune nanomaterial dimensions from 0-D quantum dot (QD) structures to cylindrical (NR) and branched (TP) structures by exploitation of advanced colloidal synthesis techniques and understandings of NC facet reactivities. The second chapter is focused on the synthesis and characterization of well-defined CdSe-seeded-CdS (CdSe CdS) NR systems synthesized by overcoating of wurtzite (W) CdSe quantum dots with W-CdS shells. 1-dimensional NRs have been interesting constructs for applications such as solar concentrators, optical gains, and photocatalysis. Through synthetic control over CdSe CdS NR systems, materials with small and large CdSe seeds were prepared, and for each seed size, multiple NR lengths were prepared. Through transient absorption studies, it was found that band alignment did not affect the efficiency of charge localization in the CdSe core, whereas NR length had a profound effect. This work indicated that longer NRs resulted in poor exciton localization efficiencies owing to ultrafast trapping of photoexcited excitons generated in the CdS NR. The third chapter describes the synthesis of Au-tipped CdSe NRs and studies of the effects of selective metal nanoparticle deposition on the band edge energetics of these model photocatalytic systems. Previous studies had demonstrated ultrafast localization of photoexcited electrons in Au nanoparticles (AuNP) (and PtNP) deposited at the termini of CdSe and CdSe CdS NR constructs. Also, for similar systems, the hydrogen evolution reaction (HER) had been studied, for which it was found that noble metal nanoparticle tips were necessary to extract photoexcited electrons from the NR constructs and drive catalytic reactions. However, in these studies, energetic trap states, generally ascribed to surface defects on the NC surface, are often cited as contributing to loss of catalytic efficiency. Through a combination of ultraviolet photoelectron spectroscopy and waveguide based spectroelectrochemistry on films of 40 nm long CdSe NRs before and after AuNP functionalization, we found that metal deposition resulted in the formation of mid-gap energy states, which were assigned as metal-semiconductor interface states. The fourth chapter transitions from NR constructs to highly absorbing CdSe CdS TP materials, for which a single zincblende (ZB) CdSe NC is used to seed the growth of four identical CdS arms. These arms act as highly efficient light absorbers, resulting in absorption cross sections an order of magnitude greater than for comparable NR systems. In the past, many studies have been published on the striking properties of TP nanocrystals, such as dual wavelength fluorescence, multiple exciton generation, and inherent self-assembly owing to their unique geometry. Nonetheless, these materials have not been exploited for photocatalysis, primarily owing to challenges in preparing TP from ultrasmall ZB-CdSe seed size, thus preventing access to quasi-type II structures necessary for efficient photocatalysis. In this study, we successfully break through the type I/quasi-type II barrier for TP NCs, reclaiming lost ground in this field and demonstrating for the first time quasi-type II behavior in CdSe CdS TPs through transient absorption measurements. The fifth chapter continues with the study of CdSe CdS TPs, and elaborates on a new method for the selective functionalization of the highly symmetrical TP construct. TP materials have been notoriously difficult to selectively functionalize, owing to their symmetric nature. Using a novel photoinduced electrochemical Ostwald ripening process, we found that initially randomly deposited AuNPs could be ripened to a single, large AuNP tip at the end of one arm of a type I CdSe CdS TP with 40 nm arms. The sixth chapter elaborates further on the preparation of colloidal polymers, further extending the analogy between molecular and colloidal levels of synthetic control. One challenge in the field of colloidal science is the realization of new modes of self-assemble for compositionally distinct nanoparticles. In this work, it was found that Au Co nanoparticle dipole strength could be systematically varied by tuning of AuNP size on CdSe CdS nanorods/tetrapods. (Abstract shortened by ProQuest.).

Viscoelastic wormlike micelles formed by ionic liquid-type surfactant [C16imC8]Br towards template-assisted synthesis of CdS quantum dots.

PubMed

Hu, Yimin; Han, Jie; Ge, Lingling; Guo, Rong

2018-01-31

In this paper, viscoelastic wormlike micelles consisting of cationic liquid-type surfactant, 1-hexadecyl-3-octyl imidazolium bromide ([C 16 imC 8 ]Br), water and different additives were utilized for the synthesis of CdS quantum dots. First, the influence of different additives, such as [Cd(NH 3 ) 6 ]Cl 2 and ethanethioamid (precursors for the synthesis of CdS quantum dots), and temperature on the viscoelasticity of the [C 16 imC 8 ]Br aqueous solution was studied by dynamic and steady rheology. Furthermore, the synthesized CdS quantum dots and their photoluminescence properties were characterized by transmission electron microscopy (TEM), UV-Vis absorption spectroscopy, X-ray diffraction (XRD) and energy-dispersive X-ray spectroscopy (EDX). In the end, the mechanism for the synthesis of CdS quantum dots in [C 16 imC 8 ]Br wormlike micelles is proposed.

Polyaniline/carbon nanotube/CdS quantum dot composites with enhanced optical and electrical properties

NASA Astrophysics Data System (ADS)

Goswami, Mrinmoy; Ghosh, Ranajit; Maruyama, Takahiro; Meikap, Ajit Kumar

2016-02-01

A new kind of polyaniline/carbon nanotube/CdS quantum dot composites have been developed via in-situ polymerization of aniline monomer in the presence of dispersed CdS quantum dots (size: 2.7-4.8 nm) and multi-walled carbon nanotubes (CNT), which exhibits enhanced optical and electrical properties. The existences of 1st order, 2nd order, and 3rd order longitudinal optical phonon modes, strongly indicate the high quality of synthesized CdS quantum dots. The occurrence of red shift of free exciton energy in photoluminescence is due to size dependent quantum confinement effect of CdS. The conductivity of the composites (for example PANI/CNT/CdS (2 wt.% CdS)) is increased by about 7 of magnitude compared to that of pure PANI indicating a charge transfer between CNT and polymer via CdS quantum dots. This advanced material has a great potential for high-performance of electro-optical applications.

Quantum dots coupled ZnO nanowire-array panels and their photocatalytic activities.

PubMed

Liao, Yulong; Que, Wenxiu; Zhang, Jin; Zhong, Peng; Yuan, Yuan; Qiu, Xinku; Shen, Fengyu

2013-02-01

Fabrication and characterization of a heterojunction structured by CdS quantum dots@ZnO nanowire-array panels were presented. Firstly, ZnO nanowire-array panels were prepared by using a chemical bath deposition approach where wurtzite ZnO nanowires with a diameter of about 100 nm and 3 microm in length grew perpendicularly to glass substrate. Secondly, CdS quantum dots were deposited onto the surface of the ZnO nanowire-arrays by using successive ion layer absorption and reaction method, and the CdS shell/ZnO core heterojunction were thus obtained. Field emission scanning electron microscopy and transmission electron microscope were employed to characterize the morphological properties of the as-obtained CdS quantum dots@ZnO nanowire-array panels. X-ray diffraction was adopted to characterize the crystalline properties of the as-obtained CdS quantum dots@ZnO nanowire-array panels. Methyl orange was taken as a model compound to confirm the photocatalytic activities of the CdS shell/ZnO core heterojunction. Results indicate that CdS with narrow band gap not only acts as a visible-light sensitizer but also is responsible for an effective charge separation.

Interface formation during silica encapsulation of colloidal CdSe/CdS quantum dots observed by in situ Raman spectroscopy

NASA Astrophysics Data System (ADS)

Biermann, Amelie; Aubert, Tangi; Baumeister, Philipp; Drijvers, Emile; Hens, Zeger; Maultzsch, Janina

2017-04-01

We investigate the encapsulation of CdSe/CdS quantum dots (QDs) in a silica shell by in situ Raman spectroscopy and find a distinct shift of the CdS Raman signal during the first hours of the synthesis. This shift does not depend on the final silica shell thickness but on the properties of the initial core-shell QD. We find a correlation between the Raman shift rate and the speed of the silica formation and attribute this to the changing configuration of the outermost layers of the QD shell, where an interface to the newly formed silica is created. This dependence of Raman shift rate on the speed of silica formation process will give rise to many possible studies concerning the growth mechanism in the water-in-oil microemulsion, rendering in situ Raman a valuable instrument in monitoring this type of reaction.

In vivo characterization of hair and skin derived carbon quantum dots with high quantum yield as long-term bioprobes in zebrafish

PubMed Central

Zhang, Jing-Hui; Niu, Aping; Li, Jing; Fu, Jian-Wei; Xu, Qun; Pei, De-Sheng

2016-01-01

Carbon quantum dots (CDs) were widely investigated because of their tunable fluorescence properties and low toxicity. However, so far there have been no reports on in vivo functional studies of hair and skin derived CDs. Here, hair derived CDs (HCDs) and skin derived CDs (SCDs) were produced by using human hair and pig skin as precursors. The quantum yields (QYs) of HCDs and SCDs were quite high, compared to citric acid derived CDs (CCDs). HCDs and SCDs possess optimal photostability, hypotoxicity and biocompatibility in zebrafish, indicating that HCDs and SCDs possess the capacity of being used as fluorescence probes for in vivo biological imaging. The long-time observation for fluorescence alternation of CDs in zebrafish and the quenching assay of CDs by ATP, NADH and Fe3+ ions demonstrated that the decaying process of CDs in vivo might be induced by the synergistic effect of the metabolism process. All results indicated that large batches and high QYs of CDs can be acquired by employing natural and nontoxic hair and skin as precursors. To our knowledge, this is the first time to report SCDs, in vivo comparative studies of HCDs, SCDs and CCDs as bioprobes, and explore their mechanism of photostability in zebrafish. PMID:27886267

In vivo characterization of hair and skin derived carbon quantum dots with high quantum yield as long-term bioprobes in zebrafish.

PubMed

Zhang, Jing-Hui; Niu, Aping; Li, Jing; Fu, Jian-Wei; Xu, Qun; Pei, De-Sheng

2016-11-25

Carbon quantum dots (CDs) were widely investigated because of their tunable fluorescence properties and low toxicity. However, so far there have been no reports on in vivo functional studies of hair and skin derived CDs. Here, hair derived CDs (HCDs) and skin derived CDs (SCDs) were produced by using human hair and pig skin as precursors. The quantum yields (QYs) of HCDs and SCDs were quite high, compared to citric acid derived CDs (CCDs). HCDs and SCDs possess optimal photostability, hypotoxicity and biocompatibility in zebrafish, indicating that HCDs and SCDs possess the capacity of being used as fluorescence probes for in vivo biological imaging. The long-time observation for fluorescence alternation of CDs in zebrafish and the quenching assay of CDs by ATP, NADH and Fe 3+ ions demonstrated that the decaying process of CDs in vivo might be induced by the synergistic effect of the metabolism process. All results indicated that large batches and high QYs of CDs can be acquired by employing natural and nontoxic hair and skin as precursors. To our knowledge, this is the first time to report SCDs, in vivo comparative studies of HCDs, SCDs and CCDs as bioprobes, and explore their mechanism of photostability in zebrafish.

In vivo characterization of hair and skin derived carbon quantum dots with high quantum yield as long-term bioprobes in zebrafish

NASA Astrophysics Data System (ADS)

Zhang, Jing-Hui; Niu, Aping; Li, Jing; Fu, Jian-Wei; Xu, Qun; Pei, De-Sheng

2016-11-01

Carbon quantum dots (CDs) were widely investigated because of their tunable fluorescence properties and low toxicity. However, so far there have been no reports on in vivo functional studies of hair and skin derived CDs. Here, hair derived CDs (HCDs) and skin derived CDs (SCDs) were produced by using human hair and pig skin as precursors. The quantum yields (QYs) of HCDs and SCDs were quite high, compared to citric acid derived CDs (CCDs). HCDs and SCDs possess optimal photostability, hypotoxicity and biocompatibility in zebrafish, indicating that HCDs and SCDs possess the capacity of being used as fluorescence probes for in vivo biological imaging. The long-time observation for fluorescence alternation of CDs in zebrafish and the quenching assay of CDs by ATP, NADH and Fe3+ ions demonstrated that the decaying process of CDs in vivo might be induced by the synergistic effect of the metabolism process. All results indicated that large batches and high QYs of CDs can be acquired by employing natural and nontoxic hair and skin as precursors. To our knowledge, this is the first time to report SCDs, in vivo comparative studies of HCDs, SCDs and CCDs as bioprobes, and explore their mechanism of photostability in zebrafish.

White light emitting diode based on InGaN chip with core/shell quantum dots

NASA Astrophysics Data System (ADS)

Shen, Changyu; Hong, Yan; Ma, Jiandong; Ming, Jiangzhou

2009-08-01

Quantum dots have many applications in optoelectronic device such as LEDs for its many superior properties resulting from the three-dimensional confinement effect of its carrier. In this paper, single chip white light-emitting diodes (WLEDs) were fabricated by combining blue InGaN chip with luminescent colloidal quantum dots (QDs). Two kinds of QDs of core/shell CdSe /ZnS and core/shell/shell CdSe /ZnS /CdS nanocrystals were synthesized by thermal deposition using cadmium oxide and selenium as precursors in a hot lauric acid and hexadecylamine trioctylphosphine oxide hybrid. This two kinds of QDs exhibited high photoluminescence efficiency with a quantum yield more than 41%, and size-tunable emission wavelengths from 500 to 620 nm. The QDs LED mainly consists of flip luminescent InGaN chip, glass ceramic protective coating, glisten cup, QDs using as the photoluminescence material, pyroceram, gold line, electric layer, dielectric layer, silicon gel and bottom layer for welding. The WLEDs had the CIE coordinates of (0.319, 0.32). The InGaN chip white-light-emitting diodes with quantum dots as the emitting layer are potentially useful in illumination and display applications.

Direct Correlation of Excitonics with Efficiency in a Core-Shell Quantum Dot Solar Cell.

PubMed

Dana, Jayanta; Maiti, Sourav; Tripathi, Vaidehi S; Ghosh, Hirendra N

2018-02-16

Shell thickness dependent band-gap engineering of quasi type II core-shell material with higher carrier cooling time, lower interfacial defect states, and longer charge carrier recombination time can be a promising candidate for both photocatalysis and solar cell. In the present investigation, colloidal CdSe@CdS core-shells with different shell thickness (2, 4 and 6 monolayer CdS) were synthesized through hot injection method and have been characterized by high resolution transmission electron microscope (HRTEM) followed by steady state absorption and luminescence techniques. Ultrafast transient absorption (TA) studies suggest longer carrier cooling, lower interfacial surface states, and slower carrier recombination time in CdSe@CdS core-shell with increasing shell thickness. By TA spectroscopy, the role of CdS shell in power conversion efficiency (PCE) has been explained in detail. The measured PCE was found to initially increase and then decrease with increasing shell thickness. Shell thickness has been optimized to maximize the efficiency after correlating the shell controlled carrier cooling and recombination with PCE values and a maximum PCE of 3.88 % was obtained with 4 monolayers of CdS shell, which is found to be 57 % higher than compared to bare CdSe QDs. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Exceeding Conventional Photovoltaic Efficiency Limits Using Colloidal Quantum Dots

NASA Astrophysics Data System (ADS)

Pach, Gregory F.

Colloidal quantum dots (QDs) are a widely investigated field of research due to their highly tunable nature in which the optical and electronic properties of the nanocrystal can be manipulated by merely changing the nanocrystal's size. Specifically, colloidal quantum dot solar cells (QDSCs) have become a promising candidate for future generation photovoltaic technology. Quantum dots exhibit multiple exciton generation (MEG) in which multiple electron-hole pairs are generated from a single high-energy photon. This process is not observed in bulk-like semiconductors and allows for QDSCs to achieve theoretical efficiency limits above the standard single-junction Shockley-Queisser limit. However, the fast expanding field of QDSC research has lacked standardization of synthetic techniques and device design. Therefore, we sought to detail methodology for synthesizing PbS and PbSe QDs as well as photovoltaic device fabrication techniques as a fast track toward constructing high-performance solar cells. We show that these protocols lead toward consistently achieving efficiencies above 8% for PbS QDSCs. Using the same methodology for building single-junction photovoltaic devices, we incorporated PbS QDs as a bottom cell into a monolithic tandem architecture along with solution-processed CdTe nanocrystals. Modeling shows that near-peak tandem device efficiencies can be achieved across a wide range of bottom cell band gaps, and therefore the highly tunable band gap of lead-chalcogenide QDs lends well towards a bottom cell in a tandem architecture. A fully functioning monolithic tandem device is realized through the development of a ZnTe/ZnO recombination layer that appropriately combines the two subcells in series. Multiple recent reports have shown nanocrystalline heterostructures to undergo the MEG process more efficiency than several other nanostrucutres, namely lead-chalcogenide QDs. The final section of my thesis expands upon a recent publication by Zhang et. al., which details the synthesis of PbS/CdS heterostructures in which the PbS and CdS domains exist on opposite sides of the nanocrystal and are termed "Janus particles". Transient absorption spectroscopy shows MEG quantum yields above unity very the thermodynamic limit of 2Eg for PbS/CdS Janus particles. We further explain a mechanism for enhanced MEG using photoluminescence studies.

Design of intelligent mesoscale periodic array structures utilizing smart hydrogel

NASA Technical Reports Server (NTRS)

Sunkara, H. B.; Penn, B. G.; Frazier, D. O.; Weissman, J. M.; Asher, S. A.

1996-01-01

Mesoscale Periodic Array Structures (MPAS, also known as crystalline colloidal arrays), composed of aqueous or nonaqueous dispersions of self-assembled submicron colloidal spheres are emerging toward the development of advanced optical devices for technological applications. This is because of their unique optical diffraction properties and the ease with which these intriguing properties can be modulated experimentally. Moreover our recent advancements in this area which include 'locking' the liquid MPAS into solid or semisolid polymer matrices for greater stability with longer life span, and incorporation of CdS quantum dots and laser dyes into colloidal spheres to obtain nonlinear optical (NLO) responses further corroborate the use of MPAS in optical technology. Our long term goal is fabrication of all-optical and electro-optical devices such as spatial light modulators for optical signal processing and flat panel display devices by utilizing intelligent nonlinear periodic array structural materials. Here we show further progress in the design of novel linear MPAS which have the ability to sense and respond to an external source such as temperature. This is achieved by combining the self-assembly properties of polymer colloidal spheres and thermoshrinking properties of smart polymer gels. At selected temperatures the periodic array efficiently Bragg diffracts light and transmits most of the light at other temperatures. Hence these intelligent systems are of potential use as fixed notch filters optical switches or limiters to protect delicate optical sensors from high intensity laser radiation.

Biosynthesis of luminescent CdS quantum dots using plant hairy root culture

NASA Astrophysics Data System (ADS)

Borovaya, Mariya N.; Naumenko, Antonina P.; Matvieieva, Nadia A.; Blume, Yaroslav B.; Yemets, Alla I.

2014-12-01

CdS nanoparticles have a great potential for application in chemical research, bioscience and medicine. The aim of this study was to develop an efficient and environmentally-friendly method of plant-based biosynthesis of CdS quantum dots using hairy root culture of Linaria maroccana L. By incubating Linaria root extract with inorganic cadmium sulfate and sodium sulfide we synthesized stable luminescent CdS nanocrystals with absorption peaks for UV-visible spectrometry at 362 nm, 398 nm and 464 nm, and luminescent peaks at 425, 462, 500 nm. Transmission electron microscopy of produced quantum dots revealed their spherical shape with a size predominantly from 5 to 7 nm. Electron diffraction pattern confirmed the wurtzite crystalline structure of synthesized cadmium sulfide quantum dots. These results describe the first successful attempt of quantum dots synthesis using plant extract.

Parametric interactions in presence of different size colloids in semiconductor quantum plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vanshpal, R., E-mail: ravivanshpal@gmail.com; Sharma, Uttam; Dubey, Swati

2015-07-31

Present work is an attempt to investigate the effect of different size colloids on parametric interaction in semiconductor quantum plasma. Inclusion of quantum effect is being done in this analysis through quantum correction term in classical hydrodynamic model of homogeneous semiconductor plasma. The effect is associated with purely quantum origin using quantum Bohm potential and quantum statistics. Colloidal size and quantum correction term modify the parametric dispersion characteristics of ion implanted semiconductor plasma medium. It is found that quantum effect on colloids is inversely proportional to their size. Moreover critical size of implanted colloids for the effective quantum correction ismore » determined which is found to be equal to the lattice spacing of the crystal.« less

Eco-friendly intracellular biosynthesis of CdS quantum dots without changing Escherichia coli's antibiotic resistance.

PubMed

Yan, Zheng-Yu; Du, Qing-Qing; Qian, Jing; Wan, Dong-Yu; Wu, Sheng-Mei

2017-01-01

In the paper, a green and efficient biosynthetical technique was reported for preparing cadmium sulfide (CdS) quantum dots, in which Escherichia coli (E. coli) was chosen as a biomatrix. Fluorescence emission spectra and fluorescent microscopic photographs revealed that as-produced CdS quantum dots had an optimum fluorescence emission peak located at 470nm and emitted a blue-green fluorescence under ultraviolet excitation. After extracted from bacterial cells and located the nanocrystals' foci in vivo, the CdS quantum dots showed a uniform size distribution by transmission electron microscope. Through the systematical investigation of the biosynthetic conditions, including culture medium replacement, input time point of cadmium source, working concentrations of raw inorganic ions, and co-cultured time spans of bacteria and metal ions in the bio-manufacture, the results revealed that CdS quantum dots with the strongest fluorescence emission were successfully prepared when E. coli cells were in stationary phase, with the replacement of culture medium and following the incubation with 1.0×10 -3 mol/L cadmium source for 2 days. Results of antimicrobial susceptibility testing indicated that the sensitivities to eight types of antibiotics of E. coli were barely changed before and after CdS quantum dots were prepared in the mild temperature environment, though a slight fall of antibiotic resistance could be observed, suggesting hinted the proposed technique of producing quantum dots is a promising environmentally low-risk protocol. Copyright © 2016 Elsevier Inc. All rights reserved.

Biosynthesis of CdS nanoparticles in banana peel extract.

PubMed

Zhou, Guang Ju; Li, Shuo Hao; Zhang, Yu Cang; Fu, Yun Zhi

2014-06-01

Cadmium sulfide (CdS) nanoparticles (NPs) were synthesized by using banana peel extract as a convenient, non-toxic, eco-friendly 'green' capping agent. Cadmium nitrate and sodium sulfide are main reagents. A variety of CdS NPs are prepared through changing reaction conditions (banana extracts, the amount of banana peel extract, solution pH, concentration and reactive temperature). The prepared CdS colloid displays strong fluorescence spectrum. X-ray diffraction analysis demonstrates the successful formation of CdS NPs. Fourier transform infra-red (FTIR) spectrogram indicates the involvement of carboxyl, amine and hydroxyl groups in the formation of CdS NPs. Transmission electron microscope (TEM) result reveals that the average size of the NPs is around 1.48 nm.

Investigation of structural, morphological and opto-electronic properties of CdS quantum dot thin film

NASA Astrophysics Data System (ADS)

Ibrahim Mohammed S., M.; Gubari, Ghamdan M. M.; Huse, Nanasaheb P.; Dive, Avinash S.; Sharma, Ramphal

2018-05-01

We have successfully deposited CdS quantum dot thin film on the glass substrate by simple and economic chemical bath deposition method at ˜50 ˚C. The X-ray diffraction study confirms the formation of CdS when compared with standard JCPDS data with average crystallite size ˜3 nm. The morphology of the film was studied by FE-SEM, which suggests the homogeneous and uniform deposition of the CdS material over the entire glass substrate with a porous structure. From UV absorption spectra we observed that the sample exhibited a band edge near ˜400 nm with a slight deviation with the presence of excitonic peak for the sample. The presence of excitonic peak may be attributed to the formation of quantum dots. The calculated band gap energy of CdS quantum dot thin film was found to be ˜3.136 eV. The thin film further characterized to study electrical parameters and the sample show a drastic increase in current after light illumination.

Origins of low energy-transfer efficiency between patterned GaN quantum well and CdSe quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Xingsheng, E-mail: xsxu@semi.ac.cn

For hybrid light emitting devices (LEDs) consisting of GaN quantum wells and colloidal quantum dots, it is necessary to explore the physical mechanisms causing decreases in the quantum efficiencies and the energy transfer efficiency between a GaN quantum well and CdSe quantum dots. This study investigated the electro-luminescence for a hybrid LED consisting of colloidal quantum dots and a GaN quantum well patterned with photonic crystals. It was found that both the quantum efficiency of colloidal quantum dots on a GaN quantum well and the energy transfer efficiency between the patterned GaN quantum well and the colloidal quantum dots decreasedmore » with increases in the driving voltage or the driving time. Under high driving voltages, the decreases in the quantum efficiency of the colloidal quantum dots and the energy transfer efficiency can be attributed to Auger recombination, while those decreases under long driving time are due to photo-bleaching and Auger recombination.« less

Photovoltaic and Impedance Spectroscopy Study of Screen-Printed TiO₂ Based CdS Quantum Dot Sensitized Solar Cells.

PubMed

Atif, M; Farooq, W A; Fatehmulla, Amanullah; Aslam, M; Ali, Syed Mansoor

2015-01-19

Cadmium sulphide (CdS) quantum dot sensitized solar cells (QDSSCs) based on screen-printed TiO₂ were assembled using a screen-printing technique. The CdS quantum dots (QDs) were grown by using the Successive Ionic Layer Adsorption and Reaction (SILAR) method. The optical properties were studied by UV-Vis absorbance spectroscopy. Photovoltaic characteristics and impedance spectroscopic measurements of CdS QDSSCs were carried out under air mass 1.5 illuminations. The experimental results of capacitance against voltage indicate a trend from positive to negative capacitance because of the injection of electrons from the Fluorine doped tin oxide (FTO) electrode into TiO₂.

Effects of air annealing on CdS quantum dots thin film grown at room temperature by CBD technique intended for photosensor applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shaikh, Shaheed U.; Desale, Dipalee J.; Siddiqui, Farha Y.

2012-11-15

Graphical abstract: The effect of different intensities (40, 60 100 and 200 W) of light on CdS quantum dots thin film annealed at 350 °C indicating enhancement in (a) photo-current and (b) photosensitivity. Highlights: ► The preparation of CdS nanodot thin film at room temperature by M-CBD technique. ► Study of air annealing on prepared CdS nanodots thin film. ► The optimized annealing temperature for CdS nanodot thin film is 350 °C. ► Modified CdS thin films can be used in photosensor application. -- Abstract: CdS quantum dots thin-films have been deposited onto the glass substrate at room temperature usingmore » modified chemical bath deposition technique. The prepared thin films were further annealed in air atmosphere at 150, 250 and 350 °C for 1 h and subsequently characterized by scanning electron microscopy, ultraviolet–visible spectroscopy, electrical resistivity and I–V system. The modifications observed in morphology and opto-electrical properties of the thin films are presented.« less

Molecular differentiation of Leishmania protozoarium using CdS quantum dots as biolabels

NASA Astrophysics Data System (ADS)

Santos, Beate S.; de Farias, Patrícia M. A.; de Menezes, Frederico D.; Mariano, Erick L.; de C. Ferreira, Ricardo; Giorgio, Selma; Bosetto, Maira C.; Ayres, Diana C.; Lima, Paulo M.; Fontes, Adriana; de Thomas, André A.; Cesar, Carlos L.

2006-02-01

In this work we applied core-shell CdS/Cd(OH)2 quantum dots (QDs) as fluorescent labels in the Leishmania amazonensis protozoarium. The nanocrystals (8-9 nm) are obtained via colloidal synthesis in aqueous medium, with final pH=7 using sodium polyphosphate as the stabilizing agent. The surface of the particles is passivated with a cadmium hydroxide shell and the particle surface is functionalized with glutaraldehyde. The functionalized and non-functionalized particles were conjugated to Leishmania organisms in the promastigote form. The marked live organisms were visualized using confocal microscopy. The systems exhibit a differentiation of the emission color for the functionalized and non-functionalized particles suggesting different chemical interactions with the promastigote moieties. Two photon emision spectra (λ exc=795nm) were obtained for the promastigotes labeled with the functionalized QDs showing a significant spectral change compared to the original QDs suspension. These spectral changes are discussed in terms of the possible energy deactivation processes.

Structural, Optical, and Electrical Properties of Cobalt-Doped CdS Quantum Dots

NASA Astrophysics Data System (ADS)

Thambidurai, M.; Muthukumarasamy, N.; Velauthapillai, Dhayalan; Agilan, S.; Balasundaraprabhu, R.

2012-04-01

In the present work, a systematic study has been carried out to understand the influence of cobalt (Co) doping on various properties of CdS nanoparticles. CdS and Co-doped CdS quantum dots have been prepared at room temperature using a chemical precipitation method without using catalysts, capping agents, or surfactants. X-ray diffraction reveals that both undoped and Co-doped CdS nanoparticles exhibit hexagonal structure without any impurity phase, and the lattice constants of CdS nanoparticles are observed to decrease slightly with increasing cobalt concentration. High-resolution transmission electron microscopy (HRTEM) shows that the particle size of CdS and 5.02% Co-doped CdS nanoparticles is in the range of 2 nm to 4 nm. The Raman spectra of Co-doped CdS nanoparticles exhibit a red-shift compared with that of bulk CdS, which may be attributed to optical phonon confinement. The optical absorption spectra of Co-doped CdS nanoparticles also exhibit a red-shift with respect to that of CdS nanoparticles. The electrical conductivity of CdS and Co-doped CdS nanoparticles is found to increase with increasing temperature and cobalt concentration.

Synthesis and Characterization of Mercaptoacetic Acid Capped Cadmium Sulphide Quantum Dots.

PubMed

Wageh, S; Maize, Mai; Donia, A M; Al-Ghamdi, Ahmed A; Umar, Ahmad

2015-12-01

This paper reports the facile synthesis and detailed characterization of mercaptoacetic acid capped cadmium sulphide (CdS) quantum dots using various cadmium precursors. The mercaptoacetic acid capped CdS quantum dots were prepared by facile and simple wet chemical method and characterized by several techniques such as energy dispersive spectroscopy (EDS), X-ray diffraction, Fourier transform infrared (FTIR) spectroscopy, UV-vis. spectroscopy, photoluminescence spectroscopy, high-resolution transmission microscopy (HRTEM) and thremogravimetric analysis. The EDS studies revealed that the prepared quantum dots possess higher atomic percentage of sulfur compared to cadmium due to the coordination of thiolate to the quantum dots surfaces. The X-ray and absorption analyses exhibited that the size of quantum dots prepared by cadmium acetate is larger than the quantum dots prepared by cadmium chloride and cadmium nitrate. The increase in size can be attributed to the low stability constant of cadmium acetate in comparison with cadmium chloride and cadmium nitrate. The FTIR and thermogravimetric analysis showed that the nature of capping molecule on the surface of quantum dots are different depending on the cadmium precursors which affect the emission from CdS quantum dots. Photoemission spectroscopy revealed that the emission of quantum dots prepared by cadmium acetate has high intensity band edge emission along with low intensity trapping state emission. However the CdS quantum dots prepared by cadmium chloride and cadmium nitrate produced only trapping state emissions.

Study of electrostatically self-assembled thin films of CdS and ZnS nanoparticle semiconductors

NASA Astrophysics Data System (ADS)

Suryajaya

In this work, CdS and ZnS semiconducting colloid nanoparticles coated with organic shell, containing either SO[3-] or NH[2+] groups, were deposited as thin films using the technique of electrostatic self-assembly. The films produced were characterized with UV-vis spectroscopy and spectroscopic ellipsometry - for optical properties; atomic force microscopy (AFM) - for morphology study; mercury probe - for electrical characterisation; and photon counter - for electroluminescence study. UV-vis spectra show a substantial blue shift of the main absorption band of both CdS and ZnS, either in the form of solutions or films, with respect to the bulk materials. The calculation of nanoparticles' radii yields the value of about 1.8 nm for both CdS and ZnS.The fitting of standard ellipsometry data gave the thicknesses (d) of nanoparticle layers of around 5 nm for both CdS and ZnS which corresponds well to the size of particles evaluated from UV-vis spectral data if an additional thickness of the organic shell is taken into account. The values of refractive index (n) and extinction coefficient (k) obtained were about 2.28 and 0.7 at 633 nm wavelength, for both CdS and ZnS.Using total internal reflection (TIRE), the process of alternative deposition of poly-allylamine hydrochloride (PAH) and CdS (or ZnS) layers could be monitored in-situ. The dynamic scan shows that the adsorption kinetic of the first layer of PAH or nanoparticles was slower than that of the next layer. The fitting of TIRE spectra gavethicknesses of about 7 nm and 12 nm for CdS and ZnS, respectively. It supports the suggestion of the formation of three-dimensional aggregates of semiconductor nanoparticles intercalated with polyelectrolyte.AFM images show the formation of large aggregates of nanoparticles, about 40-50 nm, for the films deposited from original colloid solutions, while smaller aggregates, about 12-20 nm, were obtained if the colloid solutions were diluted.Current-voltage (I-V) and capacitance-frequency (C-f) measurements of polyelectrolyte/nanoparticles (CdS or ZnS) films suggest the tunnelling behaviour in the films while capacitance- voltage (C-V) and conductance-voltage (G-V) measurements suggest that these nanoparticles are conductive. The electroluminescence was detected in sandwich structures of (PAH/CdS/PAH)[N] using a photon counting detector, but not in the case of ZnS films.

A bifacial quantum dot-sensitized solar cell with all-cadmium sulfide photoanode

NASA Astrophysics Data System (ADS)

Ma, Chunqing; Tang, Qunwei; Liu, Danyang; Zhao, Zhiyuan; He, Benlin; Chen, Haiyan; Yu, Liangmin

2015-02-01

Pursuit of a high power conversion efficiency and reduction of electricity-generation cost has been a persistent objective for quantum dot-sensitized solar cells (QDSSCs). We present here the fabrication of a QDSSC comprising a nanoflower-structured CdS anode, a liquid electrolyte having S2-/Sn2- redox couples, and a transparent CoSe counter electrode. Nanoflower-structured CdS anodes are prepared by a successive ionic layer adsorption and reaction (SILAR) method and subsequently hydrothermal strategy free of any surfactant or template. The CdS nanoparticles synthesized by a SILAR method act as "seed crystal" for growth of CdS nanoflowers. The average electron lifetime is markedly elevated in nanoflower-structured CdS anode in comparison with CdS nanoparticle or nanoporous CdS microsphere anode. Herein, we study the effect of synthesis method on CdS morphology and solar cell's photovoltaic performance, showing a power conversion efficiency of 1.67% and 1.17% for nanoflower-structured CdS QDSSC under front and rear irradiations, respectively.

Fabrication of transparent TiO2 nanotube-based photoanodes for CdS/CdTe quantum co-sensitized solar cells

NASA Astrophysics Data System (ADS)

Gualdrón-Reyes, A. F.; Cárdenas-Arenas, A.; Martínez, C. A.; Kouznetsov, V. V.; Meléndez, A. M.

2017-01-01

In order to fabricate a solar cell, ordered TiO2 nanotube (TNT) arrays were prepared by double anodization. TNT arrays with variable lengths were obtained by changing the duration of the anodizing process of up to 3h. TNT membranes were transferred to indium tin oxide substrates and attached with a B-TiO2 sol. TNT photoanode with the best photoelectrochemical performance was sensitized with CdS by SILAR method. On other hand, CdTe quantum dots prepared via colloidal synthesis were deposited on TNT photoanodes for 2h, 4h and 6h. In addition, TNT/CdS was loaded with CdTe quantum dots for 4 h. Morphology and chemical modification of TiO2 were characterized by FESEM and XPS, while their photoelectrochemical performance was measured by open-circuit photopotential and photovoltammetry under visible light. TiO2 nanotubes grown during 2.5h showed the highest photocurrent due to presence of Ti3+ donor states by N and F co-doping, increasing the number of photogenerated electrons transported to back collector. TNT/CdS/CdTe photoanode reach the highest conversion efficiency under AM 1.5G simulated solar illumination.

One-pot and ultrafast synthesis of nitrogen and phosphorus co-doped carbon dots possessing bright dual wavelength fluorescence emission

NASA Astrophysics Data System (ADS)

Sun, Xiangcheng; Brückner, Christian; Lei, Yu

2015-10-01

Very brief microwave heating of aniline, ethylene diamine, and phosphoric acid in water at ambient pressure generated nitrogen and phosphorus co-doped carbon dots (N,P-CDs) that exhibit bright dual blue (centred at 450 nm; 51% quantum yield) and green (centred at 510 nm, 38% quantum yield) fluorescence emission bands. The N,P-CDs were characterized using TEM, XRD, XPS, IR, UV-vis, and fluorescence spectroscopy, demonstrating their partially crystalline carbon, partially amorphous structures, and the incorporation of O, N, and P into the carbogenic scaffold. The N,P-CDs demonstrated excitation-dependent and nearly pH-independent emission properties. The unique dual emission properties lay the foundation for the use of N,P-CDs in ratiometric sensing applications.Very brief microwave heating of aniline, ethylene diamine, and phosphoric acid in water at ambient pressure generated nitrogen and phosphorus co-doped carbon dots (N,P-CDs) that exhibit bright dual blue (centred at 450 nm; 51% quantum yield) and green (centred at 510 nm, 38% quantum yield) fluorescence emission bands. The N,P-CDs were characterized using TEM, XRD, XPS, IR, UV-vis, and fluorescence spectroscopy, demonstrating their partially crystalline carbon, partially amorphous structures, and the incorporation of O, N, and P into the carbogenic scaffold. The N,P-CDs demonstrated excitation-dependent and nearly pH-independent emission properties. The unique dual emission properties lay the foundation for the use of N,P-CDs in ratiometric sensing applications. Electronic supplementary information (ESI) available: Detailed experimental section, XRD, FTIR, explosive sensing and the applications results. See DOI: 10.1039/c5nr05549k

Enhanced photovoltaic performance of quantum dot-sensitized solar cells with a progressive reduction of recombination using Cu-doped CdS quantum dots

NASA Astrophysics Data System (ADS)

Muthalif, Mohammed Panthakkal Abdul; Lee, Young-Seok; Sunesh, Chozhidakath Damodharan; Kim, Hee-Je; Choe, Youngson

2017-02-01

In this article, we have systematically probed the effect of Cu-doping in CdS quantum dots (QDs) to enhance the photovoltaic performance of the quantum dot-sensitized solar cells (QDSSCs). The Cu-doped CdS photoanodes were prepared by successive ionic layer adsorption and reaction (SILAR) method and the corresponding cell devices were fabricated using CuS counter electrodes with a polysulfide electrolyte. The photovoltaic performance results demonstrate that 3 mM Cu-doped CdS QDs based QDSSCs exhibit the efficiency (η) of 3% including JSC = 9.40 mA cm-2, VOC = 0.637 V, FF = 0.501, which are higher than those with bare CdS (η = 2.05%, JSC = 7.12 mA cm-2, VOC = 0.588 V, FF = 0.489). The structural, topographical and optical properties of the thin films have been studied with the help of X-ray diffraction pattern (XRD), atomic force microscopy (AFM) and UV-vis spectrophotometer. Electrochemical impedance spectroscopy (EIS) and open circuit voltage decay (OCVD) measurements indicate that Cu-dopant can inhibit the charge recombination at the photoanode/electrolyte interface and extend the lifetime of electrons. These results reveal that incorporation of copper metal in CdS QDs is a simple and effective method to improve the photovoltaic properties of QDSSCs.

Cultivating Fluorescent Flowers with Highly Luminescent Carbon Dots Fabricated by a Double Passivation Method.

PubMed

Han, Shuai; Chang, Tao; Zhao, Haiping; Du, Huanhuan; Liu, Shan; Wu, Baoshuang; Qin, Shenjun

2017-07-07

In this work, we present the fabrication of highly luminescent carbon dots (CDs) by a double passivation method with the assistance of Ca(OH)₂. In the reaction process, Ca 2+ protects the active functional groups from overconsumption during dehydration and carbonization, and the electron-withdrawing groups on the CD surface are converted to electron-donating groups by the hydroxyl ions. As a result, the fluorescence quantum yield of the CDs was found to increase with increasing Ca(OH)₂ content in the reaction process. A blue-shift optical spectrum of the CDs was also found with increasing Ca(OH)₂ content, which could be attributed to the increasing of the energy gaps for the CDs. The highly photoluminescent CDs obtained (quantum yield: 86%) were used to cultivate fluorescent carnations by a water culture method, while the results of fluorescence microscopy analysis indicated that the CDs had entered the plant tissue structure.

Chemical synthesis of CdS onto TiO2 nanorods for quantum dot sensitized solar cells

NASA Astrophysics Data System (ADS)

Pawar, Sachin A.; Patil, Dipali S.; Lokhande, Abhishek C.; Gang, Myeng Gil; Shin, Jae Cheol; Patil, Pramod S.; Kim, Jin Hyeok

2016-08-01

A quantum dot sensitized solar cell (QDSSC) is fabricated using hydrothermally grown TiO2 nanorods and successive ionic layer adsorption and reaction (SILAR) deposited CdS. Surface morphology of the TiO2 films coated with different SILAR cycles of CdS is examined by Scanning Electron Microscopy which revealed aggregated CdS QDs coverage grow on increasing onto the TiO2 nanorods with respect to cycle number. Under AM 1.5G illumination, we found the TiO2/CdS QDSSC photoelectrode shows a power conversion efficiency of 1.75%, in an aqueous polysulfide electrolyte with short-circuit photocurrent density of 4.04 mA/cm2 which is higher than that of a bare TiO2 nanorods array.

Preparation and photovoltaic properties of CdS quantum dot-sensitized solar cell based on zinc tin mixed metal oxides.

PubMed

Cao, Jiupeng; Zhao, Yifan; Zhu, Yatong; Yang, Xiaoyu; Shi, Peng; Xiao, Hongdi; Du, Na; Hou, Wanguo; Qi, Genggeng; Liu, Jianqiang

2017-07-15

The present study reports a new type of quantum dot sensitized solar cells (QDSSCs) using the zinc tin mixed metal oxides (MMO) as the anode materials, which were obtained from the layered double hydroxide (LDH) precursor. The successive ionic layer adsorption and reaction (SILAR) method is applied to deposit CdS quantum dots. The effects of sensitizing cycles on the performance of CdS QDSSC are studied. Scanning electron microscopy (SEM), Transmission electron microscope (TEM) and X-ray diffraction (XRD) are used to identify the surface profile and crystal structure of the mixed metal oxides anode. The photovoltaic performance of the QDSSC is studied by the electrochemical method. The new CdS QDSSC exhibits power conversion efficiency (PCE) up to 0.48% when the anode was sensitized for eight cycles. Copyright © 2017 Elsevier Inc. All rights reserved.

Optimal nitrogen and phosphorus codoping carbon dots towards white light-emitting device

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Feng; Wang, Yaling; Miao, Yanqin

Through a one-step fast microwave-assisted approach, nitrogen and phosphorus co-doped carbon dots (N,P-CDs) were synthesized using ammonium citrate (AC) as a carbon source and phosphates as additive reagent. Under the condition of an optimal reaction time of 140 s, the influence of additive with different N and P content on fluorescent performance of N,P-CDs was further explored. It was concluded that high nitrogen content and moderate phosphorus content are necessary for obtaining high quantum yield (QY) N,P-CDs, among which the TAP-CDs (CDs synthesized using ammonium phosphate as additive reagent) show high quantum yield (QY) of 62% and red-green-blue (RGB) spectral compositionmore » of 51.67%. Besides, the TAP-CDs exhibit satisfying thermal stability within 180 °C. By virtue of good optical and thermal properties of TAP-CDs, a white light-emitting device (LED) was fabricated by combining ultraviolet chip with TAP-CDs as phosphor. The white LED emits bright warm-white light with the CIE chromaticity coordinate of (0.38, 0.35) and the corresponding color temperature (CCT) of 4450 K, indicating the potential of TAP-CDs phosphor in white LED.« less

Highly Efficient Carbon Dots with Reversibly Switchable Green-Red Emissions for Trichromatic White Light-Emitting Diodes.

PubMed

Yuan, Biao; Guan, Shanyue; Sun, Xingming; Li, Xiaoming; Zeng, Haibo; Xie, Zheng; Chen, Ping; Zhou, Shuyun

2018-05-09

Carbon dots (CDs) have potentials to be utilized in optoelectronic devices, bioimaging, and photocatalysis. The majority of the current CDs with high quantum yield to date were limited in the blue light emission region. Herein, on the basis of surface electron-state engineering, we report a kind of CDs with reversible switching ability between green and red photoluminescence with a quantum yield (QY) of both up to 80%. Highly efficient green and red solid-state luminescence is realized by doping CDs into a highly transparent matrix of methyltriethoxysilane and 3-triethoxysilylpropylamine to form CDs/gel glasses composites with QYs of 80 and 78%. The CDs/gel glasses show better transmittance in visible light bands and excellent thermal stability. A blue-pumped CDs/gel glasses phosphor-based trichromatic white light-emitting diode (WLED) is realized, whose color rendering index is 92.9. The WLED gets the highest luminous efficiency of 71.75 lm W -1 in CDs-based trichromatic WLEDs. This work opens a door for developing highly efficient green- and red-emissive switching CDs which were used as phosphors for WLEDs and have the tendency for applications in other fields, such as sensing, bioimaging, and photocatalysis.

Solvent-Controlled Synthesis of Highly Luminescent Carbon Dots with a Wide Color Gamut and Narrowed Emission Peak Widths.

PubMed

Ding, Hui; Wei, Ji-Shi; Zhang, Peng; Zhou, Zi-Yuan; Gao, Qing-Yu; Xiong, Huan-Ming

2018-05-01

Carbon dots (CDs) have tremendous potential applications in bioimaging, biomedicine, and optoelectronics. By far, it is still difficult to produce photoluminescence (PL) tunable CDs with high quantum yield (QY) across the entire visible spectrum and narrow the emission peak widths of CDs close to those of typical quantum dots. In this work, a series of CDs with tunable emission from 443 to 745 nm, quantum yield within 13-54%, and narrowed full width at half maximum (FWHM) from 108 to 55 nm, are obtained by only adjusting the reaction solvents in a one-pot solvothermal route. The distinct optical features of these CDs are based on their differences in the particle size, and the content of graphitic nitrogen and oxygen-containing functional groups, which can be modulated by controlling the dehydration and carbonization processes during solvothermal reactions. Blue, green, yellow, red, and even pure white light emitting films (Commission Internationale de L'Eclairage (CIE)= 0.33, 0.33, QY = 39%) are prepared by dispersing one or three kinds of CDs into polyvinyl alcohol with appropriate ratios. The near-infrared emissive CDs are excellent fluorescent probes for both in vitro and in vivo bioimaging because of their high QY in water, long-term stability, and low cytotoxicity. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Comparative photoluminescence study of close-packed and colloidal InP/ZnS quantum dots

NASA Astrophysics Data System (ADS)

Thuy, Ung Thi Dieu; Thuy, Pham Thi; Liem, Nguyen Quang; Li, Liang; Reiss, Peter

2010-02-01

This letter reports on the comparative photoluminescence study of InP/ZnS quantum dots in the close-packed solid state and in colloidal solution. The steady-state photoluminescence spectrum of the close-packed InP/ZnS quantum dots peaks at a longer wavelength than that of the colloidal ones. Time-resolved photoluminescence shows that the close-packed quantum dots possess a shorter luminescence decay time and strongly increased spectral shift with the time delayed from the excitation moment in comparison with the colloidal ones. The observed behavior is discussed on the basis of energy transfer enabled by the short interparticle distance between the close-packed quantum dots.

Cultivating Fluorescent Flowers with Highly Luminescent Carbon Dots Fabricated by a Double Passivation Method

PubMed Central

Chang, Tao; Zhao, Haiping; Du, Huanhuan; Liu, Shan; Wu, Baoshuang; Qin, Shenjun

2017-01-01

In this work, we present the fabrication of highly luminescent carbon dots (CDs) by a double passivation method with the assistance of Ca(OH)2. In the reaction process, Ca2+ protects the active functional groups from overconsumption during dehydration and carbonization, and the electron-withdrawing groups on the CD surface are converted to electron-donating groups by the hydroxyl ions. As a result, the fluorescence quantum yield of the CDs was found to increase with increasing Ca(OH)2 content in the reaction process. A blue-shift optical spectrum of the CDs was also found with increasing Ca(OH)2 content, which could be attributed to the increasing of the energy gaps for the CDs. The highly photoluminescent CDs obtained (quantum yield: 86%) were used to cultivate fluorescent carnations by a water culture method, while the results of fluorescence microscopy analysis indicated that the CDs had entered the plant tissue structure. PMID:28686178

Cadmium sulfide quantum dots/poly(acrylic acid-co-acrylic amide) composite hydrogel synthesized by gamma irradiation

NASA Astrophysics Data System (ADS)

Yang, Tao; Li, Qing; Wen, Wanxin; Hu, Liang; He, Weiwei; Liu, Hanzhou

2018-04-01

To improve the durability and stability of quantum dots (QDs) in the composite hydrogel, an irradiation induced reduction and polymerization-crosslinking method was reported herein where CdS QDs could be synthesized in situ and fastened to polymer chains due to the coordination forces between amino groups and CdS nanoparticles. The morphology and photoluminescence (PL) property of the composite hydrogel were studied. The result indicated that the CdS QDs with uniform size were dispersed evenly in the composite hydrogel, and the introduced CdS QDs had no obvious effect on the hydrogel structure. With the increases of reagent concentrations, PL intensity of the composite hydrogel was enhanced; however, the emission wavelength had no change.

Platelike WO3 sensitized with CdS quantum dots heterostructures for photoelectrochemical dynamic sensing of H2O2 based on enzymatic etching.

PubMed

Wang, Yanhu; Gao, Chaomin; Ge, Shenguang; Yu, Jinghua; Yan, Mei

2016-11-15

A platelike tungsten trioxide (WO3) sensitized with CdS quantum dots (QDs) heterojunction is developed for solar-driven, real-time, and selective photoelectrochemical (PEC) sensing of H2O2 in the living cells. The structure is synthesized by hydrothermally growing platelike WO3 on fluorine doped tin oxide (FTO) and subsequently sensitized with CdS QDs. The as-prepared WO3-CdS QDs heterojunction achieve significant photocurrent enhancement, which is remarkably beneficial for light absorption and charge carrier separation. Based on the enzymatic etching of CdS QDs enables the activation of quenching the charge transfer efficiency, thus leading to sensitive PEC recording of H2O2 level in buffer and cellular environments. The results indicated that the proposed method will pave the way for the development of excellent PEC sensing platform with the quantum dot sensitization. This study could also provide a new train of thought on designing of self-operating photoanode in PEC sensing, promoting the application of semiconductor nanomaterials in photoelectrochemistry. Copyright © 2016 Elsevier B.V. All rights reserved.

Core–Shell to Doped Quantum Dots: Evolution of the Local Environment Using XAFS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Saha, Avijit; Chattopadhyay, Soma; Shibata, Tomohiro

2016-09-30

Internal structure study at an atomic level is a challenging task with far reaching consequences to its material properties, specifically in the field of transition metal doping in quantum dots. Diffusion of transition metal ions in and out of quantum dots forming magnetic clusters has been a major bottleneck in this class of materials. Diffusion of the magnetic ions from the core into the nonmagnetic shell in a core/shell heterostructure architecture to attain uniform doping has been recently introduced and yet to be understood. In this work, we have studied the local structure variation of Fe as a function ofmore » CdS matrix thickness and annealing time during the overcoating of Fe 3O 4 core with CdS using X-ray absorption spectroscopy. The data reveals that Fe 3O 4 core initially forms a core/shell structure with CdS followed by alloying at the interface eventually completely diffusing all the way through the CdS matrix to form homogeneously Fe-doped CdS QDs with excellent control over size and size distribution. Study of Fe K-edge shows a complete change of Fe local environment from Fe–O to FeS.« less

Synthesis and formation mechanistic investigation of nitrogen-doped carbon dots with high quantum yields and yellowish-green fluorescence

NASA Astrophysics Data System (ADS)

Hou, Juan; Wang, Wei; Zhou, Tianyu; Wang, Bo; Li, Huiyu; Ding, Lan

2016-05-01

Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively.Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr02701f

Electronic structure of CdSe-ZnS 2D nanoplatelets

NASA Astrophysics Data System (ADS)

Cruguel, Hervé; Livache, Clément; Martinez, Bertille; Pedetti, Silvia; Pierucci, Debora; Izquierdo, Eva; Dufour, Marion; Ithurria, Sandrine; Aubin, Hervé; Ouerghi, Abdelkarim; Lacaze, Emmanuelle; Silly, Mathieu G.; Dubertret, Benoit; Lhuillier, Emmanuel

2017-04-01

Among colloidal nanocrystals, 2D nanoplatelets (NPLs) made of cadmium chalcogenides have led to especially well controlled optical features. However, the growth of core shell heterostructures has so far been mostly focused on CdS shells, while more confined materials will be more promising to decouple the emitting quantum states of the core from their external environment. Using k.p simulation, we demonstrate that a ZnS shell reduces by a factor 10 the leakage of the wavefunction into the surrounding medium. Using X-ray photoemission (XPS), we confirm that the CdSe active layer is indeed unoxidized. Finally, we build an effective electronic spectrum for these CdSe/ZnS NPLs on an absolute energy scale which is a critical set of parameters for the future integration of this material into optoelectronic devices. We determine the work function (WF) to be 4.47 eV while the material is behaving as an n-type semiconductor.

Preparation of CdS Nanoparticles by First-Year Undergraduates

ERIC Educational Resources Information Center

Winkelmann, Kurt; Noviello, Thomas; Brooks, Stephen

2007-01-01

The first year undergraduates use a simple method to synthesize 5-nm CdS nanoparticles in a water-in-oil microemulsion. The quantum size effect, the relationship between colors, optical absorbance, band-gap energy and the CdS particles affected by the formation of micelles are observed.

A strategy to improve the energy conversion efficiency and stability of quantum dot-sensitized solar cells using manganese-doped cadmium sulfide quantum dots.

PubMed

Gopi, Chandu V V M; Venkata-Haritha, M; Kim, Soo-Kyoung; Kim, Hee-Je

2015-01-14

This article describes the effect of manganese (Mn) doping in CdS to improve the photovoltaic performance of quantum dot sensitized solar cells (QDSSCs). The performances of the QDSSCs are examined in detail using a polysulfide electrolyte with a copper sulfide (CuS) counter electrode. Under the illumination of one sun (AM 1.5 G, 100 mW cm(-2)), 10 molar% Mn-doped CdS QDSSCs exhibit a power conversion efficiency (η) of 2.85%, which is higher than the value of 2.11% obtained with bare CdS. The improved photovoltaic performance is due to the impurities from Mn(2+) doping of CdS, which have an impact on the structure of the host material and decrease the surface roughness. The surface roughness and morphology of Mn-doped CdS nanoparticles can be characterised from atomic force microscopy images. Furthermore, the cell device based on the Mn-CdS electrode shows superior stability in the sulfide/polysulfide electrolyte in a working state for over 10 h, resulting in a highly reproducible performance, which is a serious challenge for the Mn-doped solar cell. Our finding provides an effective method for the fabrication of Mn-doped CdS QDs, which can pave the way to further improve the efficiency of future QDSSCs.

Visible Light Photocatalysis via CdS/ TiO 2 Nanocomposite Materials

DOE PAGES

Srinivasan, Sesha S.; Wade, Jeremy; Stefanakos, Elias K.

2006-01-01

Nmore » anostructured colloidal semiconductors with heterogeneous photocatalytic behavior have drawn considerable attention over the past few years. This is due to their large surface area, high redox potential of the photogenerated charge carriers, and selective reduction/oxidation of different classes of organic compounds. In the present paper, we have carried out a systematic synthesis of nanostructured CdS- TiO 2 via reverse micelle process. The structural and microstructural characterizations of the as-prepared CdS- TiO 2 nanocomposites are determined using XRD and SEM-EDS techniques. The visible light assisted photocatalytic performance is monitored by means of degradation of phenol in water suspension.« less

Crystalline phase transformation of colloidal cadmium sulfide nanocrystals

NASA Astrophysics Data System (ADS)

Ghali, M.; Eissa, A. M.; Mosaad, M. M.

2017-03-01

In this paper, we give a microscopic view concerning influence of the growth conditions on the physical properties of nanocrystals (NCs) thin films made of CdS, prepared using chemical bath deposition CBD technique. We show a crystalline phase transformation of CdS NCs from hexagonal wurtzite (W) structure to cubic zincblende (ZB) when the growth conditions change, particularly the solution pH values. This effect was confirmed using X-ray diffraction (XRD), transmission electron microscopy (TEM), optical absorption and photoluminescence (PL) measurements. The optical absorption spectra allow calculation of the bandgap value, Eg, where significant increase ˜200 meV in the CdS bandgap when transforming from Hexagonal to Cubic phase was found.

Ultrasensitive detection of amifostine and alkaline phosphatase based on the growth of CdS quantum dots.

PubMed

Na, Weidan; Liu, Siyu; Liu, Xiaotong; Su, Xingguang

2015-11-01

In this study, we reported a simple and sensitive fluorescence nanosensor for rapid detection of amifostine and alkaline phosphatase (ALP). The novel nanosensor was based on the fluorescence "turn on-off" of CdS quantum dots (QDs). Firstly, Cd(2+) cation could react with S(2-) anion to generate fluorescent CdS QDs in the presence of amifostine. The fluorescence (FL) intensity of amifostine-capped CdS QDs (Amifostine-CdS QDs) was increased with the increasing amounts of amifostine, and could be used for amifostine detection. However, amifostine could be converted to 2-(3-aminopropylamino) ethanethiol (WR1065) in the presence of ALP based on the dephosphorylation of ALP. Under the optimum conditions, the affinity of WR1065 to CdS QDs was weaker than that of amifostine. Therefore the new generation of WR1065-CdS QDs would reduce the FL intensity with the increase of ALP concentration, and the fluorescence of CdS QDs was turn off. The metabolic process of amifostine in the presence of alkaline phosphatase could be also studied via the change of FL intensity of CdS QDs. The present method was cost-effective, convenient, and does not require any complicated synthetic procedures. Copyright © 2015 Elsevier B.V. All rights reserved.

Emitting color tunable carbon dots by adjusting solvent towards light-emitting devices

NASA Astrophysics Data System (ADS)

Zhu, Jinyang; Bai, Xue; Bai, Jialin; Pan, Gencai; Zhu, Yongsheng; Zhai, Yue; Shao, He; Chen, Xu; Dong, Biao; Zhang, Hanzhuang; Song, Hongwei

2018-02-01

Carbon dots (CDs), one of the most significant classes of carbon-based nanophosphors, have attracted extensive attention in recent years. However, few attempts have been reported for realizing CDs with tunable emissions, especially for obtaining the red-light emissions with high photoluminescence quantum yields. Herein, we synthesized CDs with different chromatic blue, green and red emissions by facilely changing the reaction solvent during hydrothermal conditions. The photoluminescence quantum yields of 34%, 19% and 47% for the blue, green and red emissions, respectively, were achieved. Furthermore, the solid-state CD/PVA composite films were constructed through mixing the CDs with PVA polymer, in which the self-quenching of photoluminescence of CDs had been successfully avoided benefiting from the formation of hydrogen bonds between the CDs and PVA molecules. Finally, the warm white light emitting diode (WLED) was fabricated by integrating CD/PVA film on a UV-LED chip. The WLED exhibited the Commission International de l’Eclairage coordinates (CIE) of (0.38, 0.34), correlated color temperature of 3913 K and color rendering index of 91, respectively, which were comparable with the commercial WLEDs.

Rapid microwave-assisted synthesis of highly luminescent nitrogen-doped carbon dots for white light-emitting diodes

NASA Astrophysics Data System (ADS)

Wang, Yaling; Zheng, Jingxia; Wang, Junli; Yang, Yongzhen; Liu, Xuguang

2017-11-01

Highly luminescent nitrogen-doped carbon dots (N-CDs) were synthesized rapidly by one-step microwave-assisted hydrothermal method using citric acid as carbon source and ethylenediamine as dopant. The influences of reaction temperature, reaction time and raw material ratio on the fluorescence performance of N-CDs were investigated. Then N-CDs with the highest quantum yield were selected as fluorescent materials for fabricating white light-emitting diodes (LEDs). Highly luminescent N-CDs with the quantum yield of 75.96% and blue-to-red spectral composition of 51.48% were obtained at the conditions of 180 °C, 8 min and the molar ratio of citric acid to ethylenediamine 2:1. As-prepared highly luminescent N-CDs have an average size of 6.06 nm, possess extensive oxygen- and nitrogen-containing functional groups on their surface, and exhibit strong absorption in ultraviolet region. White LEDs based on the highly luminescent N-CDs emit warm white light with color coordinates of (0.42, 0.40) and correlated color temperature of 3416 K.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mthethwa, T.P.; Moloto, M.J., E-mail: mmoloto@uj.ac.za; De Vries, A.

Graphical abstract: SEM images of CdS/PMMA showing coiling as loading of CdS nanoparticles is increased. Thermal stability is increased with increase in %loading of both CdS and CdSe nanoparticles. Research highlights: {yields} TOPO-capped CdS and HDA-capped CdSe nanoparticles were synthesized and fully characterized. {yields} The nanoparticles were mixed with the polymer, PMMA using electrospinning technique using 2, 5 and 10% weight loadings. {yields} The mixture was spun to produce fibres with optical and thermal properties showing significant change and also the increase in loading causing bending or spiraling. {yields} Both TEM images for nanoparticles and SEM for fibres shows themore » morphology and sizes of the particles. -- Abstract: Electrospinning technique was used to fabricate poly(methyl methacrylate) (PMMA) fibres incorporating CdS and CdSe quantum dots (nanoparticles). Different nanoparticle loadings (2, 5 and 10 wt% with respect to PMMA) were used and the effect of the quantum dots on the properties of the fibres was studied. The optical properties of the hybrid composite fibres were investigated by photoluminescence and UV-vis spectrophotometry. Scanning electron microscopy (SEM), X-ray diffraction and FTIR spectrophotometry were also used to investigate the morphology and structure of the fibres. The optical studies showed that the size-tunable optical properties can be achieved in the polymer fibres by addition of quantum dots. SEM images showed that the morphologies of the fibres were dependent on the added amounts of quantum dots. A spiral type of morphology was observed with an increase in the concentration of CdS and CdSe nanoparticles. Less beaded structures and bigger diameter fibres were obtained at higher quantum dot concentrations. X-ray diffractometry detected the amorphous peaks of the polymer and even after the quantum dots were added and the FTIR analysis shows that there was no considerable interaction between the quantum dots and the polymer fibres at low concentration of quantum dots however at higher concentrations some interactions were observed which shows that QDs were present on the surfaces of the fibres.« less

Self-organized colloidal quantum dots and metal nanoparticles for plasmon-enhanced intermediate-band solar cells.

PubMed

Mendes, Manuel J; Hernández, Estela; López, Esther; García-Linares, Pablo; Ramiro, Iñigo; Artacho, Irene; Antolín, Elisa; Tobías, Ignacio; Martí, Antonio; Luque, Antonio

2013-08-30

A colloidal deposition technique is presented to construct long-range ordered hybrid arrays of self-assembled quantum dots and metal nanoparticles. Quantum dots are promising for novel opto-electronic devices but, in most cases, their optical transitions of interest lack sufficient light absorption to provide a significant impact in their implementation. A potential solution is to couple the dots with localized plasmons in metal nanoparticles. The extreme confinement of light in the near-field produced by the nanoparticles can potentially boost the absorption in the quantum dots by up to two orders of magnitude.In this work, light extinction measurements are employed to probe the plasmon resonance of spherical gold nanoparticles in lead sulfide colloidal quantum dots and amorphous silicon thin-films. Mie theory computations are used to analyze the experimental results and determine the absorption enhancement that can be generated by the highly intense near-field produced in the vicinity of the gold nanoparticles at their surface plasmon resonance.The results presented here are of interest for the development of plasmon-enhanced colloidal nanostructured photovoltaic materials, such as colloidal quantum dot intermediate-band solar cells.

Record Charge Carrier Diffusion Length in Colloidal Quantum Dot Solids via Mutual Dot-To-Dot Surface Passivation.

PubMed

Carey, Graham H; Levina, Larissa; Comin, Riccardo; Voznyy, Oleksandr; Sargent, Edward H

2015-06-03

Through a combination of chemical and mutual dot-to-dot surface passivation, high-quality colloidal quantum dot solids are fabricated. The joint passivation techniques lead to a record diffusion length for colloidal quantum dots of 230 ± 20 nm. The technique is applied to create thick photovoltaic devices that exhibit high current density without losing fill factor. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Supersensitization of CdS quantum dots with a near-infrared organic dye: toward the design of panchromatic hybrid-sensitized solar cells.

PubMed

Choi, Hyunbong; Nicolaescu, Roxana; Paek, Sanghyun; Ko, Jaejung; Kamat, Prashant V

2011-11-22

The photoresponse of quantum dot solar cells (QDSCs) has been successfully extended to the near-IR (NIR) region by sensitizing nanostructured TiO(2)-CdS films with a squaraine dye (JK-216). CdS nanoparticles anchored on mesoscopic TiO(2) films obtained by successive ionic layer adsorption and reaction (SILAR) exhibit limited absorption below 500 nm with a net power conversion efficiency of ~1% when employed as a photoanode in QDSC. By depositing a thin barrier layer of Al(2)O(3), the TiO(2)-CdS films were further modified with a NIR absorbing squaraine dye. Quantum dot sensitized solar cells supersensitized with a squariand dye (JK-216) showed good stability during illumination with standard global AM 1.5 solar conditions, delivering a maximum overall power conversion efficiency (η) of 3.14%. Transient absorption and pulse radiolysis measurements provide further insight into the excited state interactions of squaraine dye with SiO(2), TiO(2), and TiO(2)/CdS/Al(2)O(3) films and interfacial electron transfer processes. The synergy of combining semiconductor quantum dots and NIR absorbing dye provides new opportunities to harvest photons from different regions of the solar spectrum. © 2011 American Chemical Society

Bright colloidal quantum dot light-emitting diodes enabled by efficient chlorination

NASA Astrophysics Data System (ADS)

Li, Xiyan; Zhao, Yong-Biao; Fan, Fengjia; Levina, Larissa; Liu, Min; Quintero-Bermudez, Rafael; Gong, Xiwen; Quan, Li Na; Fan, James; Yang, Zhenyu; Hoogland, Sjoerd; Voznyy, Oleksandr; Lu, Zheng-Hong; Sargent, Edward H.

2018-03-01

The external quantum efficiencies of state-of-the-art colloidal quantum dot light-emitting diodes (QLEDs) are now approaching the limit set by the out-coupling efficiency. However, the brightness of these devices is constrained by the use of poorly conducting emitting layers, a consequence of the present-day reliance on long-chain organic capping ligands. Here, we report how conductive and passivating halides can be implemented in Zn chalcogenide-shelled colloidal quantum dots to enable high-brightness green QLEDs. We use a surface management reagent, thionyl chloride (SOCl2), to chlorinate the carboxylic group of oleic acid and graft the surfaces of the colloidal quantum dots with passivating chloride anions. This results in devices with an improved mobility that retain high external quantum efficiencies in the high-injection-current region and also feature a reduced turn-on voltage of 2.5 V. The treated QLEDs operate with a brightness of 460,000 cd m-2, significantly exceeding that of all previously reported solution-processed LEDs.

Selective contacts drive charge extraction in quantum dot solids via asymmetry in carrier transfer kinetics.

PubMed

Mora-Sero, Ivan; Bertoluzzi, Luca; Gonzalez-Pedro, Victoria; Gimenez, Sixto; Fabregat-Santiago, Francisco; Kemp, Kyle W; Sargent, Edward H; Bisquert, Juan

2013-01-01

Colloidal quantum dot solar cells achieve spectrally selective optical absorption in a thin layer of solution-processed, size-effect tuned, nanoparticles. The best devices built to date have relied heavily on drift-based transport due to the action of an electric field in a depletion region that extends throughout the thickness of the quantum dot layer. Here we study for the first time the behaviour of the best-performing class of colloidal quantum dot films in the absence of an electric field, by screening using an electrolyte. We find that the action of selective contacts on photovoltage sign and amplitude can be retained, implying that the contacts operate by kinetic preferences of charge transfer for either electrons or holes. We develop a theoretical model to explain these experimental findings. The work is the first to present a switch in the photovoltage in colloidal quantum dot solar cells by purposefully formed selective contacts, opening the way to new strategies in the engineering of colloidal quantum dot solar cells.

Biosynthesis of fluorescent CdS nanocrystals with semiconductor properties: Comparison of microbial and plant production systems.

PubMed

Al-Shalabi, Zahwa; Doran, Pauline M

2016-04-10

This study investigated fission yeast (Schizosaccharomyces pombe) and hairy roots of tomato (Solanum lycopersicum) as in vitro production vehicles for biological synthesis of CdS quantum dots. Cd added during the mid-growth phase of the cultures was detoxified within the biomass into inorganic sulphide-containing complexes with the quantum confinement properties of semiconductor nanocrystals. Significant differences were found between the two host systems in terms of nanoparticle production kinetics, yield and quality. The much slower growth rate of hairy roots compared with yeast is a disadvantage for commercial scaled-up production. Nanoparticle extraction from the biomass was less effective for the roots: 19% of the Cd present in the hairy roots was recovered after extraction compared with 34% for the yeast. The overall yield of CdS quantum dots was also lower for the roots: relative to the amount of Cd taken up into the biomass, 8.5% was recovered in yeast gel filtration fractions exhibiting quantum dot properties whereas the result for hairy roots was only 0.99%. Yeast-produced CdS crystallites were somewhat smaller with diameters of approximately 2-6 nm compared with those of 4-10nm obtained from the roots. The average ratio of inorganic sulphide to Cd for the purified and size-fractionated particles was 0.44 for the yeast and 1.6 for the hairy roots. Despite the limitations associated with hairy roots in terms of culture kinetics and product yield, this system produced CdS nanoparticles with enhanced photostability and 3.7-13-fold higher fluorescence quantum efficiency compared with those generated by yeast. This work demonstrates that the choice of cellular host can have a significant effect on nanoparticle functional properties as well as on the bioprocessing aspects of biological quantum dot synthesis. Copyright © 2016 Elsevier B.V. All rights reserved.

Nanoscale patterning of colloidal quantum dots on transparent and metallic planar surfaces.

PubMed

Park, Yeonsang; Roh, Young-Geun; Kim, Un Jeong; Chung, Dae-Young; Suh, Hwansoo; Kim, Jineun; Cheon, Sangmo; Lee, Jaesoong; Kim, Tae-Ho; Cho, Kyung-Sang; Lee, Chang-Won

2012-09-07

The patterning of colloidal quantum dots with nanometer resolution is essential for their application in photonics and plasmonics. Several patterning approaches, such as the use of polymer composites, molecular lock-and-key methods, inkjet printing and microcontact printing of quantum dots have been recently developed. Herein, we present a simple method of patterning colloidal quantum dots for photonic nanostructures such as straight lines, rings and dot patterns either on transparent or metallic substrates. Sub-10 nm width of the patterned line could be achieved with a well-defined sidewall profile. Using this method, we demonstrate a surface plasmon launcher from a quantum dot cluster in the visible spectrum.

Co-sensitization of ZnO by CdS quantum dots in natural dye-sensitized solar cells with polymeric electrolytes to improve the cell stability

DOE Office of Scientific and Technical Information (OSTI.GOV)

Junhom, W.; Magaraphan, R.

2015-05-22

The CdS quantum dots (QDs) were deposited on ZnO layer by chemical bath deposition method to absorb light in the shorter wavelength region and used as photoanode in the dye sensitized solar cell (DSSCs) with natural dye extracted from Noni leaves. Microstructures of CdS-ZnO from various dipping time were characterized by XRD, FE-SEM and EDX. The results showed that the CdS is hexagonal structure and the amount of CdS increases when the dipping time increases. The maximal conversion efficiency of 0.292% was achieved by the DSSCs based on CdS QDs-sensitized ZnO film obtained from 9 min-dipping time. Furthermore, the stability ofmore » DSSCs was improved by using polymeric electrolyte. Poly (acrylic acid) (PAA) and Polyacrylamide (PAM) were introduced to CdS QDs-sensitized ZnO film from 9 min-dipping time. Each polymeric electrolyte was prepared by swelling from 0.1-2.0 %w in H2O. The maximal conversion efficiency of 0.207% was achieved for DSSCs based on CdS QDs-sensitized ZnO film with PAM 1.0% and the conversion efficiency was decreased 25% when it was left for1 hr.« less

Co-sensitization of ZnO by CdS quantum dots in natural dye-sensitized solar cells with polymeric electrolytes to improve the cell stability

NASA Astrophysics Data System (ADS)

Junhom, W.; Magaraphan, R.

2015-05-01

The CdS quantum dots (QDs) were deposited on ZnO layer by chemical bath deposition method to absorb light in the shorter wavelength region and used as photoanode in the dye sensitized solar cell (DSSCs) with natural dye extracted from Noni leaves. Microstructures of CdS-ZnO from various dipping time were characterized by XRD, FE-SEM and EDX. The results showed that the CdS is hexagonal structure and the amount of CdS increases when the dipping time increases. The maximal conversion efficiency of 0.292% was achieved by the DSSCs based on CdS QDs-sensitized ZnO film obtained from 9 min-dipping time. Furthermore, the stability of DSSCs was improved by using polymeric electrolyte. Poly (acrylic acid) (PAA) and Polyacrylamide (PAM) were introduced to CdS QDs-sensitized ZnO film from 9 min-dipping time. Each polymeric electrolyte was prepared by swelling from 0.1-2.0 %w in H2O. The maximal conversion efficiency of 0.207% was achieved for DSSCs based on CdS QDs-sensitized ZnO film with PAM 1.0% and the conversion efficiency was decreased 25% when it was left for1 hr.

TiO2 activity enhancement through synergistic effect of photons localization of photonic crystals and the sensitization of CdS quantum dots

NASA Astrophysics Data System (ADS)

Li, Ping; Wang, Yuan; Wang, Ai-Jun; Chen, Sheng-Li

2017-02-01

In this work, the enhancement of TiO2 photocatalytic activity was studied through synergistic effect of the photons localization of photonic crystals and the sensitization of CdS quantum dots (CdS QDs). CdS QDs sensitized TiO2 membrane (denoted as CdS QDs/TiO2) was synthesized through doping the TiO2 membrane with CdS QDs by chemical bath deposition method (CBD). After TiO2 was sensitized with CdS QDs, the edge of light absorption of TiO2 was red-shifted to 470 nm and the light absorption in the range of 400 600 nm was higher than that of plain TiO2 membrane. Another type of composite membrane, CdS QDs/TiO2/SiO2 opal composite membrane was prepared by coupling SiO2 opal (a kind of photonic crystal) layer onto the CdS QDs/TiO2 membrane, and the photonic band gap of the SiO2 opal photonic crystal layer was deliberately planned at the electronic band gap of the CdS QDs. The photodegradation of gaseous CH3CHO (acetaldehyde) was used as probe reaction to test the photocatalytic activity of the as-prepared membranes, and the results showed that the CdS QDs sensitization can significantly improve the photocatalytic activity of TiO2 membrane under visible light irradiation, with the acetaldehyde degradation rate constant (k) on CdS QDs/TiO2 membranes being 1.59 times of that on plain TiO2 membranes. The acetaldehyde degradation rate constant on CdS QDs/TiO2/SiO2 opal composite membrane reached 4 times of that on plain TiO2 membrane. The photocatalytic activity of TiO2 membrane can be improved through synergistic effect of the photons localization of photonic crystals and the sensitization of CdS QDs.

Single colloidal quantum dots as sources of single photons for quantum cryptography

NASA Astrophysics Data System (ADS)

Pisanello, Ferruccio; Qualtieri, Antonio; Leménager, Godefroy; Martiradonna, Luigi; Stomeo, Tiziana; Cingolani, Roberto; Bramati, Alberto; De Vittorio, Massimo

2011-02-01

Colloidal nanocrystals, i.e. quantum dots synthesized trough wet-chemistry approaches, are promising nanoparticles for photonic applications and, remarkably, their quantum nature makes them very promising for single photon emission at room temperature. In this work we describe two approaches to engineer the emission properties of these nanoemitters in terms of radiative lifetime and photon polarization, drawing a viable strategy for their exploitation as room-temperature single photon sources for quantum information and quantum telecommunications.

Transient bleaching of small PbS colloids. Influence of surface properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nenadovic, M.T.; Comor, M.I.; Vasic, V.

1990-08-09

Small PbS colloids with a particle diameter of 40 {angstrom} were prepared in aqueous solution, and their absorption spectra exhibit several maxima. Injection of electrons into these particles was achieved by using the pulse radiolysis technique. Excess electrons trapped on the surface lead to a blue shift in the absorption edge of colloids. The appearance of this shift depends critically on the method of colloid preparation. PbS and CdS colloids prepared at pH < 6 have long-lived bleaching, which disappears after several seconds. On the other hand, absorption bleaching does not appear after the addition of hydroxide ions to colloidalmore » solutions (pH > 8). The existence of a hydroxide ion on the particle surface most likely removes surface defects on which electrons are trapped. PbS colloids prepared in the presence of 3-mercapto-1,2-propanediol have an unstructured absorption spectrum, which is due to a wide particle size distribution (10-50 {angstrom}).« less

Exploring the effect of band alignment and surface states on photoinduced electron transfer from CuInS2/CdS core/shell quantum dots to TiO2 electrodes.

PubMed

Sun, Mingye; Zhu, Dehua; Ji, Wenyu; Jing, Pengtao; Wang, Xiuying; Xiang, Weidong; Zhao, Jialong

2013-12-11

Photoinduced electron transfer (ET) processes from CuInS2/CdS core/shell quantum dots (QDs) with different core sizes and shell thicknesses to TiO2 electrodes were investigated by time-resolved photoluminescence (PL) spectroscopy. The ET rates and efficiencies from CuInS2/CdS QDs to TiO2 were superior to those of CuInS2/ZnS QDs. An enhanced ET efficiency was surprisingly observed for 2.0 nm CuInS2 core QDs after growth of the CdS shell. On the basis of the experimental and theoretical analysis, the improved performances of CuInS2/CdS QDs were attributed to the passivation of nonradiative traps by overcoating shell and enhanced delocalization of electron wave function from core to CdS shell due to lower conduction band offset. These results indicated that the electron distribution regulated by the band alignment between core and shell of QDs and the passivation of surface defect states could improve ET performance between donor and acceptor.

Study of mesoporous CdS-quantum-dot-sensitized TiO2 films by using X-ray photoelectron spectroscopy and AFM

PubMed Central

Wojcieszak, Robert; Raj, Gijo

2014-01-01

Summary CdS quantum dots were grown on mesoporous TiO2 films by successive ionic layer adsorption and reaction processes in order to obtain CdS particles of various sizes. AFM analysis shows that the growth of the CdS particles is a two-step process. The first step is the formation of new crystallites at each deposition cycle. In the next step the pre-deposited crystallites grow to form larger aggregates. Special attention is paid to the estimation of the CdS particle size by X-ray photoelectron spectroscopy (XPS). Among the classical methods of characterization the XPS model is described in detail. In order to make an attempt to validate the XPS model, the results are compared to those obtained from AFM analysis and to the evolution of the band gap energy of the CdS nanoparticles as obtained by UV–vis spectroscopy. The results showed that XPS technique is a powerful tool in the estimation of the CdS particle size. In conjunction with these results, a very good correlation has been found between the number of deposition cycles and the particle size. PMID:24605274

Efficient color-tunable multiexcitonic dual wavelength emission from Type II semiconductor tetrapods.

PubMed

Wu, Wen-Ya; Li, Mingjie; Lian, Jie; Wu, Xiangyang; Yeow, Edwin K L; Jhon, Mark H; Chan, Yinthai

2014-09-23

We synthesized colloidal InP/ZnS seeded CdS tetrapods by harnessing the structural stability of the InP/ZnS seed nanocrystals at the high reaction temperatures needed to grow the CdS arms. Because of an unexpected Type II band alignment at the interface of the InP/ZnS core and CdS arms that enhanced the occurrence of radiative excitonic recombination in CdS, these tetrapods were found to be capable of exhibiting highly efficient multiexcitonic dual wavelength emission of equal intensity at spectrally distinct wavelengths of ∼485 and ∼675 nm. Additionally, the Type II InP/ZnS seeded CdS tetrapods displayed a wider range of pump-dependent emission color-tunability (from red to white to blue) within the context of a CIE 1931 chromaticity diagram and possessed higher photostability due to suppressed multiexcitonic Auger recombination when compared to conventional Type I CdSe seeded CdS tetrapods. By employing time-resolved spectroscopy measurements, we were able to attribute the wide emission color-tunability to the large valence band offset between InP and CdS. This work highlights the importance of band alignment in the synthetic design of semiconductor nanoheterostructures, which can exhibit color-tunable multiwavelength emission with high efficiency and photostability.

Pulsed laser induced optical nonlinearities in undoped, copper doped and chromium doped CdS quantum dots

NASA Astrophysics Data System (ADS)

Sharma, Dimple; Malik, B. P.; Gaur, Arun

2015-04-01

Quantum dots (QDs) of CdS, Cu doped and Cr doped CdS were synthesized through chemical co- precipitation method. The synthesized QDs have been characterized by x-ray diffraction, ultraviolet visible absorption spectroscopy. The diameters of QDs were calculated using Debye-Scherrer’s formula and Brus equation. They are found to be in 3.5-3.8 nm range. The nonlinear properties has been studied by the open and closed aperture Z-scan technique using frequency double Nd:YAG laser. The nonlinear refractive index (n2), nonlinear absorption coefficient (β), third order nonlinear susceptibilities (χ3) of QDs has been calculated. It has been found that the values of nonlinear parameters are higher for doped QDs than undoped CdS QDs. Hence they can be regarded as potential material for the development of optoelectronics and photonics devices.

Green Synthesis of Bifunctional Fluorescent Carbon Dots from Garlic for Cellular Imaging and Free Radical Scavenging.

PubMed

Zhao, Shaojing; Lan, Minhuan; Zhu, Xiaoyue; Xue, Hongtao; Ng, Tsz-Wai; Meng, Xiangmin; Lee, Chun-Sing; Wang, Pengfei; Zhang, Wenjun

2015-08-12

Nitrogen and sulfur codoped carbon dots (CDs) were prepared from garlic by a hydrothermal method. The as-prepared CDs possess good water dispersibility, strong blue fluorescence emission with a fluorescent quantum yield of 17.5%, and excellent photo and pH stabilities. It is also demonstrated that the fluorescence of CDs are resistant to the interference of metal ions, biomolecules, and high ionic strength environments. Combining with low cytotoxicity properties, CDs could be used as an excellent fluorescent probe for cellular multicolor imaging. Moreover, the CDs were also demonstrated to exhibit favorable radical scavenging activity.

Chiral quantum dot based materials

NASA Astrophysics Data System (ADS)

Govan, Joseph; Loudon, Alexander; Baranov, Alexander V.; Fedorov, Anatoly V.; Gun'ko, Yurii

2014-05-01

Recently, the use of stereospecific chiral stabilising molecules has also opened another avenue of interest in the area of quantum dot (QD) research. The main goal of our research is to develop new types of technologically important quantum dot materials containing chiral defects, study their properties and explore their applications. The utilisation of chiral penicillamine stabilisers allowed the preparation of new water soluble white emitting CdS quantum nanostructures which demonstrated circular dichroism in the band-edge region of the spectrum. It was also demonstrated that all three types of QDs (D-, L-, and Rac penicillamine stabilised) show very broad emission bands between 400 and 700 nm due to defects or trap states on the surfaces of the nanocrystals. In this work the chiral CdS based quantum nanostructures have also been doped by copper metal ions and new chiral penicilamine stabilized CuS nanoparticles have been prepared and investigated. It was found that copper doping had a strong effect at low levels in the synthesis of chiral CdS nanostructures. We expect that this research will open new horizons in the chemistry of chiral nanomaterials and their application in biotechnology, sensing and asymmetric synthesis.

Slow Auger Relaxation in HgTe Colloidal Quantum Dots.

PubMed

Melnychuk, Christopher; Guyot-Sionnest, Philippe

2018-05-03

The biexciton lifetimes in HgTe colloidal quantum dots are measured as a function of particle size. Samples produced by two synthetic methods, leading to partially aggregated or well-dispersed particles, exhibit markedly different dynamics. The relaxation characteristics of partially aggregated HgTe inhibit reliable determinations of the Auger lifetime. In well-dispersed HgTe quantum dots, the biexciton lifetime increases approximately linearly with particle volume, confirming trends observed in other systems. The extracted Auger coefficient is three orders of magnitude smaller than that for bulk HgCdTe materials with similar energy gaps. We discuss these findings in the context of understanding Auger relaxation in quantum-confined systems and their relevance to mid-infrared optoelectronic devices based on HgTe colloidal quantum dots.

INTERACTIONS OF METHYL ORANGE WITH CYCLODEXTRIN/SODIUM-MONTMORILLONITE SYSTEMS PROBED BY UV-VISIBLE SPECTROSCOPY

EPA Science Inventory

Clay mineral colloids play important roles in the adsorption of polar organic contaminants in the environment. Similarly, cyclodextrins (CD) can entrap poorly water-soluble organic compounds. A combination of CDs and clay minerals affords great opportunities to investigate simult...

Light-emitting diodes based on colloidal silicon quantum dots

NASA Astrophysics Data System (ADS)

Zhao, Shuangyi; Liu, Xiangkai; Pi, Xiaodong; Yang, Deren

2018-06-01

Colloidal silicon quantum dots (Si QDs) hold great promise for the development of printed Si electronics. Given their novel electronic and optical properties, colloidal Si QDs have been intensively investigated for optoelectronic applications. Among all kinds of optoelectronic devices based on colloidal Si QDs, QD light-emitting diodes (LEDs) play an important role. It is encouraging that the performance of LEDs based on colloidal Si QDs has been significantly increasing in the past decade. In this review, we discuss the effects of the QD size, QD surface and device structure on the performance of colloidal Si-QD LEDs. The outlook on the further optimization of the device performance is presented at the end.

Nitrogen and sulfur co-doped carbon dots with strong blue luminescence

NASA Astrophysics Data System (ADS)

Ding, Hui; Wei, Ji-Shi; Xiong, Huan-Ming

2014-10-01

Sulfur-doped carbon dots (S-CDs) with a quantum yield (QY) of 5.5% and nitrogen, sulfur co-doped carbon dots (N,S-CDs) with a QY of 54.4% were synthesized, respectively, via the same hydrothermal route using α-lipoic acid as the carbon source. The obtained S-CDs and N,S-CDs had similar sizes but different optical features. The QY of N,S-CDs was gradually enhanced when extending the reaction time to increase the nitrogen content. After careful characterization of these CDs, the doped nitrogen element was believed to be in the form of C&z.dbd;N and C-N bonds which enhanced the fluorescence efficiency significantly. Meanwhile, the co-doped sulfur element was found to be synergistic for nitrogen doping in N,S-CDs. The optimal N,S-CDs were successfully employed as good multicolor cell imaging probes due to their fine dispersion in water, excitation-dependent emission, excellent fluorescence stability and low toxicity. Besides, such N,S-CDs showed a wide detection range and excellent accuracy as fluorescent sensors for Fe3+ ions.Sulfur-doped carbon dots (S-CDs) with a quantum yield (QY) of 5.5% and nitrogen, sulfur co-doped carbon dots (N,S-CDs) with a QY of 54.4% were synthesized, respectively, via the same hydrothermal route using α-lipoic acid as the carbon source. The obtained S-CDs and N,S-CDs had similar sizes but different optical features. The QY of N,S-CDs was gradually enhanced when extending the reaction time to increase the nitrogen content. After careful characterization of these CDs, the doped nitrogen element was believed to be in the form of C&z.dbd;N and C-N bonds which enhanced the fluorescence efficiency significantly. Meanwhile, the co-doped sulfur element was found to be synergistic for nitrogen doping in N,S-CDs. The optimal N,S-CDs were successfully employed as good multicolor cell imaging probes due to their fine dispersion in water, excitation-dependent emission, excellent fluorescence stability and low toxicity. Besides, such N,S-CDs showed a wide detection range and excellent accuracy as fluorescent sensors for Fe3+ ions. Electronic supplementary information (ESI) available: Experimental details and comparable characterization of three kinds of CDs. See DOI: 10.1039/c4nr04267k

One pot synthesis of highly luminescent polyethylene glycol anchored carbon dots functionalized with a nuclear localization signal peptide for cell nucleus imaging.

PubMed

Yang, Lei; Jiang, Weihua; Qiu, Lipeng; Jiang, Xuewei; Zuo, Daiying; Wang, Dongkai; Yang, Li

2015-04-14

Strong blue fluorescent polyethylene glycol (PEG) anchored carbon nitride dots (CDs@PEG) with a high quantum yield (QY) of 75.8% have been synthesized by a one step hydrothermal treatment. CDs with a diameter of ca. 6 nm are well dispersed in water and present a graphite-like structure. Photoluminescence (PL) studies reveal that CDs display excitation-dependent behavior and are stable under various test conditions. Based on the as-prepared CDs, we designed novel cell nucleus targeting imaging carbon dots functionalized with a nuclear localization signal (NLS) peptide. The favourable biocompatibilities of CDs and NLS modified CDs (NLS-CDs) are confirmed by in vitro cytotoxicity assays. Importantly, intracellular localization experiments in MCF7 and A549 cells demonstrate that NLS-CDs could be internalized in the nucleus and show blue light, which indicates that CDs may serve as cell nucleus imaging probes.

On the origin of stretched exponential (Kohlrausch) relaxation kinetics in the room temperature luminescence decay of colloidal quantum dots.

PubMed

Bodunov, E N; Antonov, Yu A; Simões Gamboa, A L

2017-03-21

The non-exponential room temperature luminescence decay of colloidal quantum dots is often well described by a stretched exponential function. However, the physical meaning of the parameters of the function is not clear in the majority of cases reported in the literature. In this work, the room temperature stretched exponential luminescence decay of colloidal quantum dots is investigated theoretically in an attempt to identify the underlying physical mechanisms associated with the parameters of the function. Three classes of non-radiative transition processes between the excited and ground states of colloidal quantum dots are discussed: long-range resonance energy transfer, multiphonon relaxation, and contact quenching without diffusion. It is shown that multiphonon relaxation cannot explain a stretched exponential functional form of the luminescence decay while such dynamics of relaxation can be understood in terms of long-range resonance energy transfer to acceptors (molecules, quantum dots, or anharmonic molecular vibrations) in the environment of the quantum dots acting as energy-donors or by contact quenching by acceptors (surface traps or molecules) distributed statistically on the surface of the quantum dots. These non-radiative transition processes are assigned to different ranges of the stretching parameter β.

[Properties of synthesized CdS nanoparticles by reverse micelle method].

PubMed

Li, Heng-Da; Wang, Qing-Wei; Zhai, Hong-Ju; Li, Wen-Lian

2008-07-01

Micelle system with reverse phase (water/CTAB/n-hexyl alcohol/n-heptane) is a weenie liquid-globelet of surface active agent molecule which can be stably and uniformly dispersed in continuous oil medium. The micelle system with reverse phase can work as a "micro-reactor" to synthesize CdS nano-particle with excellent performance. In the present article considering the effects of W value (W= [water]/[surface agent]) of the micelle system with reverse phase, we observed that the ratio of [Cd2+] and [S2-] ions to the original concentrations of the Cd2+ and S2- ions can affect the luminescent properties of CdS nano-particle. Using regurgitant treatment process the surface of CdS nano-particle can be modified, and as a result the defect emission was reduced and even disappeared, but exciton emissions markedly increased. On the other hand, a red-shift of the exciton emission peak with the increase in the particle size was observed, indicating considerable quantum confinement effect. A maximum quantum efficiency of 11% for the synthesized CdS nano-material was achieved.

Emulsion Synthesis of Size-Tunable CH3NH3PbBr3 Quantum Dots: An Alternative Route toward Efficient Light-Emitting Diodes.

PubMed

Huang, Hailong; Zhao, Fangchao; Liu, Lige; Zhang, Feng; Wu, Xian-gang; Shi, Lijie; Zou, Bingsuo; Pei, Qibing; Zhong, Haizheng

2015-12-30

We report a facile nonaqueous emulsion synthesis of colloidal halide perovskite quantum dots by controlled addition of a demulsifier into an emulsion of precursors. The size of resulting CH3NH3PbBr3 quantum dots can be tuned from 2 to 8 nm by varying the amount of demulsifier. Moreover, this emulsion synthesis also allows the purification of these quantum dots by precipitation from the colloidal solution and obtains solid-state powder which can be redissolved for thin film coating and device fabrication. The photoluminescence quantum yields of the quantum dots is generally in the range of 80-92%, and can be well-preserved after purification (∼80%). Green light-emitting diodes fabricated comprising a spin-cast layer of the colloidal CH3NH3PbBr3 quantum dots exhibited maximum current efficiency of 4.5 cd/A, power efficiency of 3.5 lm/W, and external quantum efficiency of 1.1%. This provides an alternative route toward high efficient solution-processed perovskite-based light-emitting diodes. In addition, the emulsion synthesis is versatile and can be extended for the fabrication of inorganic halide perovskite colloidal CsPbBr3 nanocrystals.

Supramolecular Gel-Templated In Situ Synthesis and Assembly of CdS Quantum Dots Gels

NASA Astrophysics Data System (ADS)

Zhu, Lili; He, Jie; Wang, Xiaoliang; Li, Dawei; He, Haibing; Ren, Lianbing; Jiang, Biwang; Wang, Yong; Teng, Chao; Xue, Gi; Tao, Huchun

2017-01-01

Although many studies have attempted to develop strategies for spontaneously organizing nanoparticles (NPs) into three-dimensional (3D) geometries, it remains a fascinating challenge. In this study, a method for in situ synthesis and self-assembly of a CdS quantum dots (QDs) gel using a Cd supramolecular gel as a scaffold was demonstrated. During the QDs formation process, the Cd ions that constituted the Cd gels served as the precursors of the CdS QDs, and the oleic acid (OA) that ligated with the Cd in the supramolecular gels was capped on the surface of the CdS QDs in the form of carboxylate. The OA-stabilized CdS QDs were in situ synthesized in the entangled self-assembled fibrillar networks (SAFIN) of the Cd gels through reactions between the gelator and H2S. As a result, the QDs exactly replicated the framework of the SAFIN in the CdS QD gels instead of simply assembling along the SAFIN of the supramolecular gels. Moreover, the CdS QDs showed extraordinary sensitivity in the fluorescence detection of IO4 - anions. The facile one-step method developed here is a new approach to assembling nanostructured materials into 3D architectures and has general implications for the design of low molecular mass gelators to bring desired functionality to the developed supramolecular gels.

Size dependence in tunneling spectra of PbSe quantum-dot arrays.

PubMed

Ou, Y C; Cheng, S F; Jian, W B

2009-07-15

Interdot Coulomb interactions and collective Coulomb blockade were theoretically argued to be a newly important topic, and experimentally identified in semiconductor quantum dots, formed in the gate confined two-dimensional electron gas system. Developments of cluster science and colloidal synthesis accelerated the studies of electron transport in colloidal nanocrystal or quantum-dot solids. To study the interdot coupling, various sizes of two-dimensional arrays of colloidal PbSe quantum dots are self-assembled on flat gold surfaces for scanning tunneling microscopy and scanning tunneling spectroscopy measurements at both room and liquid-nitrogen temperatures. The tip-to-array, array-to-substrate, and interdot capacitances are evaluated and the tunneling spectra of quantum-dot arrays are analyzed by the theory of collective Coulomb blockade. The current-voltage of PbSe quantum-dot arrays conforms properly to a scaling power law function. In this study, the dependence of tunneling spectra on the sizes (numbers of quantum dots) of arrays is reported and the capacitive coupling between quantum dots in the arrays is explored.

Colloidal CdSe Quantum Rings.

PubMed

Fedin, Igor; Talapin, Dmitri V

2016-08-10

Semiconductor quantum rings are of great fundamental interest because their non-trivial topology creates novel physical properties. At the same time, toroidal topology is difficult to achieve for colloidal nanocrystals and epitaxially grown semiconductor nanostructures. In this work, we introduce the synthesis of luminescent colloidal CdSe nanorings and nanostructures with double and triple toroidal topology. The nanorings form during controlled etching and rearrangement of two-dimensional nanoplatelets. We discuss a possible mechanism of the transformation of nanoplatelets into nanorings and potential utility of colloidal nanorings for magneto-optical (e.g., Aharonov-Bohm effect) and other applications.

Redox shuttle mechanism enhances photocatalytic H2 generation on Ni-decorated CdS nanorods

NASA Astrophysics Data System (ADS)

Simon, Thomas; Bouchonville, Nicolas; Berr, Maximilian J.; Vaneski, Aleksandar; Adrović, Asmir; Volbers, David; Wyrwich, Regina; Döblinger, Markus; Susha, Andrei S.; Rogach, Andrey L.; Jäckel, Frank; Stolarczyk, Jacek K.; Feldmann, Jochen

2014-11-01

Photocatalytic conversion of solar energy to fuels, such as hydrogen, is attracting enormous interest, driven by the promise of addressing both energy supply and storage. Colloidal semiconductor nanocrystals have been at the forefront of these efforts owing to their favourable and tunable optical and electronic properties as well as advances in their synthesis. The efficiency of the photocatalysts is often limited by the slow transfer and subsequent reactions of the photoexcited holes and the ensuing high charge recombination rates. Here we propose that employing a hydroxyl anion/radical redox couple to efficiently relay the hole from the semiconductor to the scavenger leads to a marked increase in the H2 generation rate without using expensive noble metal co-catalysts. The apparent quantum yield and the formation rate under 447 nm laser illumination exceeded 53% and 63 mmol g-1 h-1, respectively. The fast hole transfer confers long-term photostability on the system and opens new pathways to improve the oxidation side of full water splitting.

One pot synthesis of intriguing fluorescent carbon dots for sensing and live cell imaging.

PubMed

Jana, Jayasmita; Ganguly, Mainak; Das, Bodhisatwa; Dhara, Santanu; Negishi, Yuichi; Pal, Tarasankar

2016-04-01

We report a simple one-pot synthesis of highly fluorescent carbon dots (CDs) via modified hydrothermal (MHT) treatment of alkaline solution of dopamine and cysteine. These CDs (λex=320 nm, λem=390 nm, and quantum yield ∼ 5.1%) are of ∼ 2-3 nm in diameter. Further attempt of synthesizing CDs in some common water-miscible solvents ends up the fact that the MHT product from acetone medium is nonfluorescent. However, CDs, produced in aqueous medium, are so stable that they can be dried as a deliverable solid (WCD) without any alteration of fluorescing property if reversibly dispersed in water. Fluorescence of WCD is quenched selectively in acetone. Quenching occurs presumably due to the disruption of radiative recombination along with the hindrance in quantum confinement of the emissive energy traps to the particle surface. Successive quenching of fluorescence of WCD in different acetone concentration admixed in water paves the way to selective acetone sensing (LOD=8.75 × 10(-7) M). The synthesized CDs (in aqueous medium) are cytocompatible and are efficient fluorescent probe for cell imaging. Only living cells are recognized exclusively from fluorescence imaging leaving aside dead cells, while cells are treated with CDs. Copyright © 2015 Elsevier B.V. All rights reserved.

Mn(II)-coordinated Fluorescent Carbon Dots: Preparation and Discrimination of Organic Solvents

NASA Astrophysics Data System (ADS)

Wang, Yuru; Wang, Tianren; Chen, Xi; Xu, Yang; Li, Huanrong

2018-04-01

Herein, we prepared a Mn(II)-coordinated carbon dots (CDs) with fluorescence and MRI (magnetic resonance imaging) bimodal properties by a one-pot solvothermal method and separated via silica column chromatography. The quantum yield of the CDs increased greatly from 2.27% to 6.75% with increase of Mn(II) doping, meanwhile the CDs exhibited a higher MR activity (7.28 mM-1s-1) than that of commercial Gd-DTPA (4.63 mM-1s-1). In addition, white light emitting CDs were obtained by mixing the different types of CDs. Notably, these CDs exhibited different fluorescence emissions in different organic solvents and could be used to discriminate organic solvents based on the polarity and protonation of the solvents.

Kelvin probe imaging of photo-injected electrons in metal oxide nanosheets from metal sulfide quantum dots under remote photochromic coloration

NASA Astrophysics Data System (ADS)

Kondo, A.; Yin, G.; Srinivasan, N.; Atarashi, D.; Sakai, E.; Miyauchi, M.

2015-07-01

Metal oxide and quantum dot (QD) heterostructures have attracted considerable recent attention as materials for developing efficient solar cells, photocatalysts, and display devices, thus nanoscale imaging of trapped electrons in these heterostructures provides important insight for developing efficient devices. In the present study, Kelvin probe force microscopy (KPFM) of CdS quantum dot (QD)-grafted Cs4W11O362- nanosheets was performed before and after visible-light irradiation. After visible-light excitation of the CdS QDs, the Cs4W11O362- nanosheet surface exhibited a decreased work function in the vicinity of the junction with CdS QDs, even though the Cs4W11O362- nanosheet did not absorb visible light. X-ray photoelectron spectroscopy revealed that W5+ species were formed in the nanosheet after visible-light irradiation. These results demonstrated that excited electrons in the CdS QDs were injected and trapped in the Cs4W11O362- nanosheet to form color centers. Further, the CdS QDs and Cs4W11O362- nanosheet composite films exhibited efficient remote photochromic coloration, which was attributed to the quantum nanostructure of the film. Notably, the responsive wavelength of the material is tunable by adjusting the size of QDs, and the decoloration rate is highly efficient, as the required length for trapped electrons to diffuse into the nanosheet surface is very short owing to its nanoscale thickness. The unique properties of this photochromic device make it suitable for display or memory applications. In addition, the methodology described in the present study for nanoscale imaging is expected to aid in the understanding of electron transport and trapping processes in metal oxide and metal chalcogenide heterostructure, which are crucial phenomena in QD-based solar cells and/or photocatalytic water-splitting systems.Metal oxide and quantum dot (QD) heterostructures have attracted considerable recent attention as materials for developing efficient solar cells, photocatalysts, and display devices, thus nanoscale imaging of trapped electrons in these heterostructures provides important insight for developing efficient devices. In the present study, Kelvin probe force microscopy (KPFM) of CdS quantum dot (QD)-grafted Cs4W11O362- nanosheets was performed before and after visible-light irradiation. After visible-light excitation of the CdS QDs, the Cs4W11O362- nanosheet surface exhibited a decreased work function in the vicinity of the junction with CdS QDs, even though the Cs4W11O362- nanosheet did not absorb visible light. X-ray photoelectron spectroscopy revealed that W5+ species were formed in the nanosheet after visible-light irradiation. These results demonstrated that excited electrons in the CdS QDs were injected and trapped in the Cs4W11O362- nanosheet to form color centers. Further, the CdS QDs and Cs4W11O362- nanosheet composite films exhibited efficient remote photochromic coloration, which was attributed to the quantum nanostructure of the film. Notably, the responsive wavelength of the material is tunable by adjusting the size of QDs, and the decoloration rate is highly efficient, as the required length for trapped electrons to diffuse into the nanosheet surface is very short owing to its nanoscale thickness. The unique properties of this photochromic device make it suitable for display or memory applications. In addition, the methodology described in the present study for nanoscale imaging is expected to aid in the understanding of electron transport and trapping processes in metal oxide and metal chalcogenide heterostructure, which are crucial phenomena in QD-based solar cells and/or photocatalytic water-splitting systems. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr02405f

The Physics of Ultracold Sr2 Molecules: Optical Production and Precision Measurement

NASA Astrophysics Data System (ADS)

Osborn, Christopher Butler

Colloidal quantum dots have desirable optical properties which can be exploited to realize a variety of photonic devices and functionalities. However, colloidal dots have not had a pervasive utility in photonic devices because of the absence of patterning methods. The electronic chip industry is highly successful due to the well-established lithographic procedures. In this thesis we borrow ideas from the semiconductor industry to develop lithographic techniques that can be used to pattern colloidal quantum dots while ensuring that the optical properties of the quantum dots are not affected by the process. In this thesis we have developed colloidal quantum dot based waveguide structures for amplification and switching applications for all-optical signal processing. We have also developed colloidal quantum dot based light emitting diodes. We successfully introduced CdSe/ZnS quantum dots into a UV curable photo-resist, which was then patterned to realize active devices. In addition, "passive" devices (devices without quantum dots) were integrated to "active" devices via waveguide couplers. Use of photo-resist devices offers two distinct advantages. First, they have low scattering loss and secondly, they allow good fiber to waveguide coupling efficiency due to the low refractive index which allows for large waveguide cross-sections while supporting single mode operation. Practical planar photonic devices and circuits incorporating both active and passive structures can now be realized, now that we have patterning capabilities of quantum dots while maintaining the original optical attributes of the system. In addition to the photo-resist host, we also explored the incorporation of colloidal quantum dots into a dielectric silicon dioxide and silicon nitride one-dimensional microcavity structures using low temperature plasma enhanced chemical vapor deposition. This material system can be used to realize microcavity light emitting diodes that can be realized on any substrate. As a proof of concept demonstration we show a 1550 nm emitting all-dielectric vertical cavity structure embedded with PbS quantum dots. Enhancement in spontaneous emission from the dots embedded in the microcavity is also demonstrated.

A CCD-based reader combined with CdS quantum dot-labeled lateral flow strips for ultrasensitive quantitative detection of CagA

NASA Astrophysics Data System (ADS)

Gui, Chen; Wang, Kan; Li, Chao; Dai, Xuan; Cui, Daxiang

2014-02-01

Immunochromatographic assays are widely used to detect many analytes. CagA is proved to be associated closely with initiation of gastric carcinoma. Here, we reported that a charge-coupled device (CCD)-based test strip reader combined with CdS quantum dot-labeled lateral flow strips for quantitative detection of CagA was developed, which used 365-nm ultraviolet LED as the excitation light source, and captured the test strip images through an acquisition module. Then, the captured image was transferred to the computer and was processed by a software system. A revised weighted threshold histogram equalization (WTHE) image processing algorithm was applied to analyze the result. CdS quantum dot-labeled lateral flow strips for detection of CagA were prepared. One hundred sera samples from clinical patients with gastric cancer and healthy people were prepared for detection, which demonstrated that the device could realize rapid, stable, and point-of-care detection, with a sensitivity of 20 pg/mL.

Exciton-Plasmon Interaction between AuNPs/Graphene Nanohybrids and CdS Quantum Dots/TiO2 for Photoelectrochemical Aptasensing of Prostate-Specific Antigen.

PubMed

Cai, Guoneng; Yu, Zhengzhong; Ren, Rongrong; Tang, Dianping

2018-03-23

A competitive-displacement reaction strategy based on target-induced dissociation of gold nanoparticle coated graphene nanosheet (AuNPs/GN) from CdS quantum dot functionalized mesoporous titanium dioxide (CdS QDs/TiO 2 ) was designed for the sensitive photoelectrochemical (PEC) aptasensing of prostate-specific antigen (PSA) through the exciton-plasmon interaction (EPI) between CdS QDs and AuNPs. To construct such an aptasensing system, capture DNA was initially conjugated covalently onto CdS QDs/TiO 2 -modified electrode, and then AuNPs/GN-labeled PSA aptamer was bound onto biofunctionalized CdS QDs/TiO 2 via hybridization chain reaction of partial bases with capture DNA. Introduction of AuNPs/GN efficiently quenched the photocurrent of CdS QDs/TiO 2 thanks to energy transfer. Upon addition of target PSA, the sandwiched aptamer between CdS QDs/TiO 2 and AuNPs/GN reacted with the analyte analyte, thus resulting in the dissociation of AuNPs/GN from the CdS QDs/TiO 2 to increase the photocurrent. Under optimum conditions, the aptasensing platform exhibited a high sensitivity for PSA detection within a dynamic linear range of 1.0 pg/mL to 8.0 ng/mL at a low limitat of detection of 0.52 pg/mL. The interparticle distance of exciton-plasmon interaction and contents of AuNPs corresponding to EPI effect in this system were also studied. Good selectivity and high reproducibility were obtained for the analysis of target PSA. Importantly, the accuracy and matrix effect of PEC aptasensor was evaluated for the determination of human serum specimens and newborn calf serum-diluted PSA standards, giving a well-matched result with the referenced PSA ELISA kit.

Photocatalyst based on TiO2 nanotube arrays co-decorated with CdS quantum dots and reduced graphene oxide irradiated by γ rays for effective degradation of ethylene

NASA Astrophysics Data System (ADS)

Zhang, Quan; Ye, Shengying; Song, Xianliang; Luo, Shucan

2018-06-01

We report herein a means of transforming TiO2 nanotube arrays (TNAs) from an amorphous state to an anatase crystal state (denoted as ∗TNAs), and present a single-step synthetic route for preparing CdS quantum dots (CdS QDs) as well as reduced graphene oxide (rGO) through gamma-ray irradiation. The as-prepared ∗TNAs, CdS QDs, and rGO, which had all been subjected to gamma-ray irradiation, were then assembled together to produce the desired heterojunction (denoted as CdS QDs/rGO-∗TNAs). X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), ultraviolet/visible diffuse-reflectance spectroscopy (UV/Vis DRS), Fourier-transform infrared spectroscopy (FTIR), micro-Raman spectrometry (RS), atomic force microscopy (AFM), and X-ray photoelectron spectroscopy (XPS) have been applied to characterize the appearance and performance of this photocatalyst. The photocatalytic activity of CdS QDs/rGO-∗TNAs towards ethylene degradation has been measured by placing it in a simulated cold-storage environment, the temperature and humidity of which were set at about 3 ± 1 °C and 75-90%, respectively. The results showed that the rate constant (K) of ethylene degradation could reach up to 1.07 × 10-3 min-1 with CdS QDs/rGO-∗TNAs, as compared to 2.30 × 10-4 min-1 with ∗TNAs and 6.25 × 10-4 min-1 with CdS QDs-∗TNAs, indicating that the constructed CdS QDs/rGO-∗TNAs constitutes a promising photocatalyst for ethylene removal in a cold storage environment.

Transition Metal Nanomaterials by Bacterial Precipitation: Synthesis and Characterization of Cadmium Sulfide Quantum Dots

NASA Astrophysics Data System (ADS)

Marusak, Katherine Elizabeth

We present a new method to fabricate semiconducting, transition metal nanoparticles (NPs) with tunable bandgap energies using engineered Escherichia coli. These bacteria overexpress the Treponema denticola cysteine desulfhydrase gene to facilitate precipitation of cadmium sulfide (CdS) NPs. Multiple characterization techniques reveal that the bacterially precipitated NPs are agglomerates of mostly quantum dots, with diameters that can range from 3 to 15 nm, embedded in a carbon-rich matrix. Notably, the measured photoelectrochemical current generated by these NPs is comparable to values reported in the literature and higher than that of synthesized chemical bath deposited CdS NPs. We showed that we can manipulate the bandgap energy of the NPs by controlling their size through varying the precursor concentrations. Our calculated bandgap energies ranged between 2.67 eV (i.e., quantum confined CdS) to 2.36 eV ( i.e., bulk CdS). By adding the CdCl2 precursor at a specific stage of the bacterial growth cycle, we were able to induce extracellular CdS NP precipitation. Additionally, we adapted extracellular precipitation strategies to form CdS NPs on surfaces as bacterial/PC membrane composites and characterized them by spectroscopic and imaging methods, including energy dispersive spectroscopy, and scanning and transmission electron microscopy. This method allowed us to control the localization of NP precipitation throughout the layered bacterial/membrane composite, by varying the timing of the cadmium precursor addition. Additionally, we demonstrated the photodegradation of methyl orange using the CdS functionalized porous membranes, thus confirming the photocatalytic properties of our composites for eventual translation to device development. We finally also explored the precipitation of other metallic NPs using our bacterial system, using enzyme extracted from our bacterial system, and using commercially available, his-tagged enzyme. We hope to extend this research to tethering enzymes on surfaces to direct NP precipitation. Taken all together, our results show the great promise bacteria have for the fabrication of tunable, transition metal NPs with useful electronic properties.

Blocking the Formation of Zn2+/Dye Complexes in Dye-Sensitized Solar Cells by Inserting CdS Quantum Dots into Sandwich Layer

NASA Astrophysics Data System (ADS)

Sun, Yunfei; Liu, Chunling; Yang, Lili; Wei, Maobin; Lv, Shiquan; Sui, Yingrui; Cao, Jian; Chen, Gang; Yang, Jinghai

2018-06-01

ZnO NRAs are grown on ITO substrates by a simple chemical method. CdS QDs were deposited on ZnO NRAs by SILAR. N719 was synthesized by dipping method. J-V analysis indicates that by inserting a layer of CdS QDs, the conversion efficiency of DSSCs was improved obviously. The device with CdS QDs shows the higher conversion efficiency due to the three reasons: (1) CdS QDs enhanced adsorption spectra of DSSCs in the visible region; (2) CdS QDs block the formation of Zn2+/dye complex, it is beneficial for electros transport from dye to ZnO photoanode. It is the key to obtain higher conversion efficiency; (3) FRET dynamics exists by the introduction of CdS QDs.

Quantum junction solar cells.

PubMed

Tang, Jiang; Liu, Huan; Zhitomirsky, David; Hoogland, Sjoerd; Wang, Xihua; Furukawa, Melissa; Levina, Larissa; Sargent, Edward H

2012-09-12

Colloidal quantum dot solids combine convenient solution-processing with quantum size effect tuning, offering avenues to high-efficiency multijunction cells based on a single materials synthesis and processing platform. The highest-performing colloidal quantum dot rectifying devices reported to date have relied on a junction between a quantum-tuned absorber and a bulk material (e.g., TiO(2)); however, quantum tuning of the absorber then requires complete redesign of the bulk acceptor, compromising the benefits of facile quantum tuning. Here we report rectifying junctions constructed entirely using inherently band-aligned quantum-tuned materials. Realizing these quantum junction diodes relied upon the creation of an n-type quantum dot solid having a clean bandgap. We combine stable, chemically compatible, high-performance n-type and p-type materials to create the first quantum junction solar cells. We present a family of photovoltaic devices having widely tuned bandgaps of 0.6-1.6 eV that excel where conventional quantum-to-bulk devices fail to perform. Devices having optimal single-junction bandgaps exhibit certified AM1.5 solar power conversion efficiencies of 5.4%. Control over doping in quantum solids, and the successful integration of these materials to form stable quantum junctions, offers a powerful new degree of freedom to colloidal quantum dot optoelectronics.

Studies on the interaction between 7-(dimethyl amino)-4-(trifluoromethyl)-2H-1-benzopyran-2-one and cadmium sulfide quantum dots

NASA Astrophysics Data System (ADS)

Kuriakose, Alina C.; Pradeep, C.; Nampoori, V. P. N.; Thomas, Sheenu

2018-04-01

Quantum dots (QDs) are well known for their optical properties which differ from those of bulk semiconductors. Herein, we have created an energy transfer platform that combines CdS QDs with a coumarin based dye C485 [7-(dimethyl amino)-4-(trifluoromethyl)-2H-1-benzopyran-2-one]. Spectroscopic studies of energy transfer between the dye donor and CdS QDs as acceptors reveal the occurrence of dynamic quenching. Analysis of the steady-state and time resolved fluorescence measurements of C485 in the presence of CdS QDs infers fluorescence resonance (Förster type) energy transfer (FRET) as responsible for the quenching phenomena. The energy transfer efficiency as well as energy transfer distance for the donor-acceptor pair is calculated using steady-state fluorescence method. Luminescence enhancement of CdS QDs play a critical role in device performance for solar applications and also in the field of biological applications.

Fabrication of nanocrystal ink based superstrate-type CuInS₂ thin film solar cells.

PubMed

Cho, Jin Woo; Park, Se Jin; Kim, Woong; Min, Byoung Koun

2012-07-05

A CuInS₂ (CIS) nanocrystal ink was applied to thin film solar cell devices with superstrate-type configuration. Monodispersed CIS nanocrystals were synthesized by a colloidal synthetic route and re-dispersed in toluene to form an ink. A spray method was used to coat CIS films onto conducting glass substrates. Prior to CIS film deposition, TiO₂ and CdS thin films were also prepared as a blocking layer and a buffer layer, respectively. We found that both a TiO₂ blocking layer and a CdS buffer layer are necessary to generate photoresponses in superstrate-type devices. The best power conversion efficiency (∼1.45%) was achieved by the CIS superstrate-type thin film solar cell device with 200 and 100 nm thick TiO₂ and CdS films, respectively.

CdS quantum dots as fluorescence probes for the sensitive and selective detection of highly reactive HSe- ions in aqueous solution.

PubMed

Wu, Chuan-Liu; Zhao, Yi-Bing

2007-06-01

Water-soluble cadmium sulfide (CdS) quantum dots (QDs) capped by mercaptoacetic acid were synthesized by aqueous-phase arrested precipitation, and characterized by transmission electron microscopy, spectrofluorometry, and UV-Vis spectrophotometry. The prepared luminescent water-soluble CdS QDs were evaluated as fluorescence probes for the detection of highly reactive hydrogen selenide ions (HSe(-) ions). The quenching of the fluorescence emission of CdS QDs with the addition of HSe(-) ions is due to the elimination of the S(2-) vacancies which are luminescence centers. Quantitative analysis based on chemical interaction between HSe(-) ions and the surface of CdS QDs is very simple, easy to develop, and has demonstrated very high sensitivity and selectivity features. The effect of foreign ions (common anions and biologically relevant cations) on the fluorescence of the CdS QDs was examined to evaluate the selectivity. Only Cu(2+) and S(2-) ions exhibit significant effects on the fluorescence of CdS QDs. With the developed method, we are able to determine the concentration of HSe(-) ions in the range from 0.10 to 4.80 micromol L(-1), and the limit of detection is 0.087 micromol L(-1). The proposed method was successfully applied to monitor the obtained HSe(-) ions from the reaction of glutathione with selenite. To the best of our knowledge, this is the first report on fluorescence analysis of HSe(-) ions in aqueous solution.

Single-Source Molecular Precursor for Synthesis of CdS Nanoparticles and Nanoflowers

NASA Astrophysics Data System (ADS)

Salavati-Niasari, Masoud; Sobhani, Azam

2012-04-01

CdS Semiconductor nanostructures were synthesized by using two different methods. Using triphenylphosphine (C18H15P) and oleylamine (C18H37N) as surfactant, CdS semiconductor nanocrystals with a size ranging from 30 to 90 nm can be synthesized by thermal decomposition of precursor [bis(thiosemicarbazide)cadmium(II)]. CdS nanoflowers were synthesized via hydrothermal decomposition of [bis(thiosemicarbazide) cadmium(II)] without any surfactant. X-ray diffraction (XRD) patterns confirm that the resulting samples were a pure hexagonal phase of CdS. The optical property test indicates that the absorption peak of the samples shifts towards short wavelength, and the blue shift phenomenon might be ascribed to the quantum effect.

Single-step fabrication of quantum funnels via centrifugal colloidal casting of nanoparticle films

PubMed Central

Kim, Jin Young; Adinolfi, Valerio; Sutherland, Brandon R.; Voznyy, Oleksandr; Kwon, S. Joon; Kim, Tae Wu; Kim, Jeongho; Ihee, Hyotcherl; Kemp, Kyle; Adachi, Michael; Yuan, Mingjian; Kramer, Illan; Zhitomirsky, David; Hoogland, Sjoerd; Sargent, Edward H.

2015-01-01

Centrifugal casting of composites and ceramics has been widely employed to improve the mechanical and thermal properties of functional materials. This powerful method has yet to be deployed in the context of nanoparticles—yet size–effect tuning of quantum dots is among their most distinctive and application-relevant features. Here we report the first gradient nanoparticle films to be constructed in a single step. By creating a stable colloid of nanoparticles that are capped with electronic-conduction-compatible ligands we were able to leverage centrifugal casting for thin-films devices. This new method, termed centrifugal colloidal casting, is demonstrated to form films in a bandgap-ordered manner with efficient carrier funnelling towards the lowest energy layer. We constructed the first quantum-gradient photodiode to be formed in a single deposition step and, as a result of the gradient-enhanced electric field, experimentally measured the highest normalized detectivity of any colloidal quantum dot photodetector. PMID:26165185

Reversed oxygen sensing using colloidal quantum wells towards highly emissive photoresponsive varnishes

PubMed Central

Lorenzon, Monica; Christodoulou, Sotirios; Vaccaro, Gianfranco; Pedrini, Jacopo; Meinardi, Francesco; Moreels, Iwan; Brovelli, Sergio

2015-01-01

Colloidal quantum wells combine the advantages of size-tunable electronic properties with vast reactive surfaces that could allow one to realize highly emissive luminescent-sensing varnishes capable of detecting chemical agents through their reversible emission response, with great potential impact on life sciences, environmental monitoring, defence and aerospace engineering. Here we combine spectroelectrochemical measurements and spectroscopic studies in a controlled atmosphere to demonstrate the ‘reversed oxygen-sensing’ capability of CdSe colloidal quantum wells, that is, the exposure to oxygen reversibly increases their luminescence efficiency. Spectroelectrochemical experiments allow us to directly relate the sensing response to the occupancy of surface states. Magneto-optical measurements demonstrate that, under vacuum, heterostructured CdSe/CdS colloidal quantum wells stabilize in their negative trion state. The high starting emission efficiency provides a possible means to enhance the oxygen sensitivity by partially de-passivating the particle surfaces, thereby enhancing the density of unsaturated sites with a minimal cost in term of luminescence losses. PMID:25910499

Thiol surface complexation on growing CdS clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Swayambunathan, V.; Hayes, D.; Schmidt, K.H.

1990-05-09

The growth of small CdS colloidal particles has been initiated by pulse radiolytic release of sulfide from thiol (3-mercapto-1,2-propanediol, RSH) in the presence of Cd{sup 2+} ions. The kinetics and stoichiometry of the ensuring reactions were followed by conductivity, absorption spectroscopy, and light-scattering techniques. The final CdS product has been identified by electron diffraction. The formation of Cd-thiolate complexes at the surface of the particles is indicated by conductivity and by energy dispersive analysis of X-ray (EDAX) results. The rate of formation of CdS clusters is strongly pH dependent due to the pH effect on the stability of Dd{sup 2+}/HS{supmore » {minus}} complexes. At low pHs (4.0-5.3) the growth mechanism is proposed to be primarily a cluster-molecule process. At this pH range Cd{sup 2+} ions at the CdS particle surface complex with thiolate ions stronger than in the bulk of the solution. The size control of the particles by thiols is proposed to result from a competition of thiolate ions with HS{sup {minus}} ions for cadmium ions at the surface of the growing particles.« less

Enhance the performance of liquid crystal as an optical switch by doping CdS quantum dots

NASA Astrophysics Data System (ADS)

Ahmed, Sudad S.; Ibrahim, Rawa K.; Al-Naimee, Kais; Naje, Asama N.; Ibrahim, Omar A.; Majeed, K. A.

2018-05-01

The electrical and optical properties results were studied for Cadmium Sulphide (CdS) Nanoparticles / Nematic liquid crystal (5CB) mixtures. Doping of CdS nanoparticles increases the spontaneous polarization and response time, the increase is due to large dipole-dipole interaction between the liquid crystal (LC) molecules and CdS nanoparticles, which increase the anchoring energy. The electro-optic measurements revealed a decrease (∼40%) in threshold voltage, and faster response time in doped sample cells than Pure 4'-n-pentyl-4-cyanobiphenyl (5CB) nematic liquid crystal.

Facile synthesis of fluorescence carbon dots from sweet potato for Fe3+ sensing and cell imaging.

PubMed

Shen, Jie; Shang, Shaoming; Chen, Xiuying; Wang, Dan; Cai, Yan

2017-07-01

In this study, a facile synthesis of fluorescence carbon dots (CDs) from sweet potato was performed through hydrothermal treatment. The obtained CDs with quantum yield of 8.64% have good dispersibility due to the soluble functional groups on their surfaces. The characterization of CDs was carried out and their possible formation mechanism was also discussed. In addition, the cytotoxicity results showed that the CDs exhibit non toxicity within 100μg/mL. At this concentration, the CDs were applied in cell imaging, indicating that they are promising fluorescent probes for biological imaging. In addition, the fluorescence of CDs was quenched by Fe 3+ with a linear concentration of 1 to 100μM, associated with the limit of detection of 0.32μM. Subsequently, the CDs were successfully applied for Fe 3+ probing in living cells. Copyright © 2017 Elsevier B.V. All rights reserved.

Quantum dot sensitized solar cell based on TiO2/CdS/Ag2S heterostructure

NASA Astrophysics Data System (ADS)

Pawar, Sachin A.; Patil, Dipali S.; Kim, Jin Hyeok; Patil, Pramod S.; Shin, Jae Cheol

2017-04-01

Quantum dot sensitized solar cell (QDSSC) is fabricated based on a stepwise band structure of TiO2/CdS/Ag2S to improve the photoconversion efficiency of TiO2/CdS system by incorporating a low band gap Ag2S QDs. Vertically aligned TiO2 nanorods assembly is prepared by a simple hydrothermal technique. The formation of CdS and Ag2S QDs over TiO2 nanorods assembly as a photoanode is carried out by successive ionic layer adsorption and reaction (SILAR) technique. The synthesized electrode materials are characterized by XRD, XPS, field emission scanning electron microscopy (FE-SEM), Optical, solar cell and electrochemical performances. The results designate that the QDs of CdS and Ag2S have efficiently covered exterior surfaces of TiO2 nanorods assembly. A cautious evaluation between TiO2/CdS and TiO2/CdS/Ag2S sensitized cells tells that CdS and Ag2S synergetically helps to enhance the light harvesting ability. Under AM 1.5G illumination, the photoanodes show an improved power conversion efficiency of 1.87%, in an aqueous polysulfide electrolyte with short-circuit photocurrent density of 7.03 mA cm-2 which is four fold higher than that of a TiO2/CdS system.

Near-infrared light-mediated photodynamic/photothermal therapy nanoplatform by the assembly of Fe3O4 carbon dots with graphitic black phosphorus quantum dots

PubMed Central

Zhang, Ming; Wang, Wentao; Cui, Yingjun; Zhou, Ninglin; Shen, Jian

2018-01-01

Background Recently, combined photodynamic therapy (PDT) and photothermal therapy (PTT) has become a desired treatment for cancer. However, the development of economic, high-efficiency, and safe photosensitizers/photothermal agents remains a significant challenge. Methods A novel nanocomposite has been developed via the assembly of iron oxide carbon dot (Fe3O4-CDs) nanoparticles and black phosphorus quantum dots (genipin [GP]-polyglutamic acid [PGA]-Fe3O4-CDs@BPQDs), and this nanocomposite shows a broad light-absorption band and a photodegradable character. Results In vitro and in vivo assays indicated that GP-PGA-Fe3O4-CDs@BPQDs were highly biocompatible and exhibited excellent tumor-inhibition efficacy, due to the synergistic PTT and PDT via a near-infrared laser. Importantly, in vivo tumor magnetic resonance imaging (MRI) results illustrated that GP-PGA-Fe3O4-CDs@BPQDs can be specifically applied for enhanced T2 MRI of tumors. This work presents the first combined application of a PDT and PTT effect deriving from BPQDs and MRI from Fe3O4-CDs, which may promote utilization of black BPQDs in biomedicine. Conclusion As expected, GP-PGA-Fe3O4-CDs@BPQDs displayed a dramatically enhanced ability to destroy tumor cells, due to the synergistic combination of PTT and PDT. PMID:29785107

Unity quantum yield of photogenerated charges and band-like transport in quantum-dot solids.

PubMed

Talgorn, Elise; Gao, Yunan; Aerts, Michiel; Kunneman, Lucas T; Schins, Juleon M; Savenije, T J; van Huis, Marijn A; van der Zant, Herre S J; Houtepen, Arjan J; Siebbeles, Laurens D A

2011-09-25

Solid films of colloidal quantum dots show promise in the manufacture of photodetectors and solar cells. These devices require high yields of photogenerated charges and high carrier mobilities, which are difficult to achieve in quantum-dot films owing to a strong electron-hole interaction and quantum confinement. Here, we show that the quantum yield of photogenerated charges in strongly coupled PbSe quantum-dot films is unity over a large temperature range. At high photoexcitation density, a transition takes place from hopping between localized states to band-like transport. These strongly coupled quantum-dot films have electrical properties that approach those of crystalline bulk semiconductors, while retaining the size tunability and cheap processing properties of colloidal quantum dots.

CdS/CdSe co-sensitized SnO2 photoelectrodes for quantum dots sensitized solar cells

NASA Astrophysics Data System (ADS)

Lin, Yibing; Lin, Yu; Meng, Yongming; Tu, Yongguang; Zhang, Xiaolong

2015-07-01

SnO2 nanoparticles were synthesized by hydrothermal method and applied to photo-electrodes of quantum dots-sensitized solar cells (QDSSCs). After sensitizing SnO2 films via CdS quantum dots, CdSe quantum dots was decorated on the surface of CdS/SnO2 photo-electrodes to further improve the power conversion efficiency. CdS and CdSe quantum dots were deposited by successive ionic layer absorption and reaction method (SILAR) and chemical bath deposition method (CBD) respectively. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD) were used to identify the surface profile and crystal structure of SnO2 photo-electrodes before and after deposited quantum dots. After CdSe co-sensitized process, an overall power conversion efficiency of 1.78% was obtained in CdSe/CdS/SnO2 QDSSC, which showed 66.4% improvement than that of CdS/SnO2 QDSSC.

Fabrication of CDs/CdS-TiO2 ternary nano-composites for photocatalytic degradation of benzene and toluene under visible light irradiation

NASA Astrophysics Data System (ADS)

Wang, Meng; Hua, Jianhao; Yang, Yaling

2018-06-01

An efficient cadmium sulfide quantum-dots (CdS QDs) and carbon dots (CDs) modified TiO2 photocatalyst (CdS/CDs-TiO2) was successfully fabricated. The as-prepared ternary nano-composites simultaneously improved the photo-corrosion of CdS and amplified its photocatalytic activity. The introduction of CdS QDs and CDs could enhance more absorbance of light, prevent the undesirable electron/hole recombination, and promote charge separation, which was important for the continuous formation of rad OH and rad O2- radicals. When the optimal mass ratio of CdS QDs to CDs was 3:1, above 90% degradation efficiencies were achieved for benzene within 1 h and toluene in 2 h, while that of pure TiO2 (P25), CdS QDs-TiO2, CDs-TiO2 nano-composites was around 15%. Owing to the symmetric structure and conjugation of methyl with benzene ring, the degradation of toluene was more difficult than benzene to carry on. The new fabricated nano-composites showed good prospective application of cleaning up refractory pollutants and the resource utilization.

Green preparation of carbon dots with papaya as carbon source for effective fluorescent sensing of Iron (III) and Escherichia coli.

PubMed

Wang, Ning; Wang, Yiting; Guo, Tingting; Yang, Ting; Chen, Mingli; Wang, Jianhua

2016-11-15

A simple one-step hydrothermal green approach was reported for the preparation of carbon dots (CDs) without any further decoration or modification with papaya powder as natural carbon source. In this economical and eco-friendly system, deionized water or 90% ethanol was used as solvent to produce water-soluble or ethanol-soluble CDs, respectively, termed as W-CDs and E-CDs. The quantum yield (QY) for W-CDs was 18.98%, while that for E-CDs was 18.39%. The potentials of the prepared carbon dots toward diverse applications were thoroughly investigated. W-CDs and E-CDs provide promising probes for fluorescence detection of Fe(3+), offering limits of detection of 0.48μmolL(-1) and 0.29μmolL(-1), respectively. W-CDs was further demonstrated to be a promising probe for fluorescence sensing of Escherichia coli O157: H7, along with a limit of detection of 9.5×10(4)cfumL(-1). Meanwhile, both W-CDs and E-CDs exhibit favorable biocompatibility, and demonstrated to be efficient for Hela cell imaging. Copyright © 2016 Elsevier B.V. All rights reserved.

One-step, low-temperature fabrication of CdS quantum dots by watermelon rind: a green approach

PubMed Central

Lakshmipathy, Rajasekhar; Sarada, Nallani Chakravarthula; Chidambaram, K; Pasha, Sk Khadeer

2015-01-01

We investigated the one-step synthesis of CdS nanoparticles via green synthesis that used aqueous extract of watermelon rind as a capping and stabilizing agent. Preliminary phytochemical analysis depicted the presence of carbohydrates which can act as capping and stabilizing agents. Synthesized CdS nanoparticles were characterized using UV-visible, Fourier transform infrared spectroscopy, X-ray diffraction, EDX, dynamic light scattering, transmission electron microscopy, and atomic force microscopy techniques. The CdS nanoparticles were found to be size- and shape-controlled and were stable even after 3 months of synthesis. The results suggest that watermelon rind, an agro-waste, can be used for synthesis of CdS nanoparticles without any addition of stabilizing and capping agents. PMID:26491319

Synthesis of Nitrogen and Sulfur Co-doped Carbon Dots from Garlic for Selective Detection of Fe3+

NASA Astrophysics Data System (ADS)

Sun, Chun; Zhang, Yu; Wang, Peng; Yang, Yue; Wang, Yu; Xu, Jian; Wang, Yiding; Yu, William W.

2016-02-01

Garlic was used as a green source to synthesize carbon dots (CDs) with a systematic study of the optical and structure properties. Ethylenediamine was added into the synthesis to improve the photoluminescence quantum yield (PL QY) of the CDs. Detailed structural and composition studies demonstrated that the content of N and the formation of C-N and C=N were critical to improve the PL QY. The as-synthesized CDs exhibited excellent stability in a wide pH range and high NaCl concentrations, rendering them applicable in complicated and harsh conditions. Quenching the fluorescence of the CDs in the presence of Fe3+ ion made these CDs a luminescent probe for selective detection of Fe3+ ion.

Synthesis of Nitrogen and Sulfur Co-doped Carbon Dots from Garlic for Selective Detection of Fe(3.).

PubMed

Sun, Chun; Zhang, Yu; Wang, Peng; Yang, Yue; Wang, Yu; Xu, Jian; Wang, Yiding; Yu, William W

2016-12-01

Garlic was used as a green source to synthesize carbon dots (CDs) with a systematic study of the optical and structure properties. Ethylenediamine was added into the synthesis to improve the photoluminescence quantum yield (PL QY) of the CDs. Detailed structural and composition studies demonstrated that the content of N and the formation of C-N and C=N were critical to improve the PL QY. The as-synthesized CDs exhibited excellent stability in a wide pH range and high NaCl concentrations, rendering them applicable in complicated and harsh conditions. Quenching the fluorescence of the CDs in the presence of Fe(3+) ion made these CDs a luminescent probe for selective detection of Fe(3+) ion.

Highly luminescent silica-coated CdS/CdSe/CdS nanoparticles with strong chemical robustness and excellent thermal stability

NASA Astrophysics Data System (ADS)

Wang, Nianfang; Koh, Sungjun; Jeong, Byeong Guk; Lee, Dongkyu; Kim, Whi Dong; Park, Kyoungwon; Nam, Min Ki; Lee, Kangha; Kim, Yewon; Lee, Baek-Hee; Lee, Kangtaek; Bae, Wan Ki; Lee, Doh C.

2017-05-01

We present facile synthesis of bright CdS/CdSe/CdS@SiO2 nanoparticles with 72% of quantum yields (QYs) retaining ca 80% of the original QYs. The main innovative point is the utilization of the highly luminescent CdS/CdSe/CdS seed/spherical quantum well/shell (SQW) as silica coating seeds. The significance of inorganic semiconductor shell passivation and structure design of quantum dots (QDs) for obtaining bright QD@SiO2 is demonstrated by applying silica encapsulation via reverse microemulsion method to three kinds of QDs with different structure: CdSe core and 2 nm CdS shell (CdSe/CdS-thin); CdSe core and 6 nm CdS shell (CdSe/CdS-thick); and CdS core, CdSe intermediate shell and 5 nm CdS outer shell (CdS/CdSe/CdS-SQW). Silica encapsulation inevitably results in lower photoluminescence quantum yield (PL QY) than pristine QDs due to formation of surface defects. However, the retaining ratio of pristine QY is different in the three silica coated samples; for example, CdSe/CdS-thin/SiO2 shows the lowest retaining ratio (36%) while the retaining ratio of pristine PL QY in CdSe/CdS-thick/SiO2 and SQW/SiO2 is over 80% and SQW/SiO2 shows the highest resulting PL QY. Thick outermost CdS shell isolates the excitons from the defects at surface, making PL QY relatively insensitive to silica encapsulation. The bright SiO2-coated SQW sample shows robustness against harsh conditions, such as acid etching and thermal annealing. The high luminescence and long-term stability highlights the potential of using the SQW/SiO2 nanoparticles in bio-labeling or display applications.

Erbium-implanted silica colloids with 80% luminescence quantum efficiency

NASA Astrophysics Data System (ADS)

Slooff, L. H.; de Dood, M. J. A.; van Blaaderen, A.; Polman, A.

2000-06-01

Silica colloids with a diameter of 240-360 nm, grown by wet chemical synthesis using ethanol, ammonia, water, and tetraethoxysilane, were implanted with 350 keV Er ions, to peak concentrations of 0.2-1.1 at. % and put onto a silicon or glass substrate. After annealing at 700-900 °C the colloids show clear room-temperature photoluminescence at 1.53 μm, with lifetimes as high as 17 ms. By comparing data of different Er concentrations, the purely radiative lifetime is estimated to be 20-22 ms, indicating a high quantum efficiency of about 80%. This high quantum efficiency indicates that, after annealing, the silica colloids are almost free of OH impurities. Spinning a layer of polymethylmethacrylate over the silica spheres results in an optically transparent nanocomposite layer, that can be used as a planar optical waveguide amplifier at 1.5 μm that is fully compatible with polymer technology.

Nitrogen and sulfur co-doped carbon dots with strong blue luminescence.

PubMed

Ding, Hui; Wei, Ji-Shi; Xiong, Huan-Ming

2014-11-21

Sulfur-doped carbon dots (S-CDs) with a quantum yield (QY) of 5.5% and nitrogen, sulfur co-doped carbon dots (N,S-CDs) with a QY of 54.4% were synthesized, respectively, via the same hydrothermal route using α-lipoic acid as the carbon source. The obtained S-CDs and N,S-CDs had similar sizes but different optical features. The QY of N,S-CDs was gradually enhanced when extending the reaction time to increase the nitrogen content. After careful characterization of these CDs, the doped nitrogen element was believed to be in the form of C=N and C-N bonds which enhanced the fluorescence efficiency significantly. Meanwhile, the co-doped sulfur element was found to be synergistic for nitrogen doping in N,S-CDs. The optimal N,S-CDs were successfully employed as good multicolor cell imaging probes due to their fine dispersion in water, excitation-dependent emission, excellent fluorescence stability and low toxicity. Besides, such N,S-CDs showed a wide detection range and excellent accuracy as fluorescent sensors for Fe(3+) ions.

Modified transverse phonon-helicon interaction in colloids laden semiconductor plasmas due to Bohm potential and Fermi degenerate pressure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sharma, Aartee, E-mail: aartee.sharma08@gmail.com; Yadav, N.; Ghosh, S.

2015-07-31

A detailed study of the quantum modification of acousto-helicon wave spectra due to Bohm potential and Fermi degenerate pressure in colloids laden semiconductor plasma has been presented. We have used quantum hydrodynamic model of plasmas to arrive at most general dispersion relation in presence of magnetic field. This dispersion relation has been analyzed in three different velocity regimes and the expressions for gain constants have been obtained. From the present study it has been concluded that the quantum effect and the magnetic field significantly modify the wave characteristics particularly in high doping regime in semiconductor plasma medium in presence ofmore » colloids in it.« less

Defect-mediated photoluminescence up-conversion in cadmium sulfide nanobelts (Conference Presentation)

NASA Astrophysics Data System (ADS)

Morozov, Yurii; Kuno, Masaru K.

2017-02-01

The concept of optical cooling of solids has existed for nearly 90 years ever since Pringsheim proposed a way to cool solids through the annihilation of phonons via phonon-assisted photoluminescence (PL) up-conversion. In this process, energy is removed from the solid by the emission of photons with energies larger than those of incident photons. However, actually realizing optical cooling requires exacting parameters from the condensed phase medium such as near unity external quantum efficiencies as well as existence of a low background absorption. Until recently, laser cooling has only been successfully realized in rare earth doped solids. In semiconductors, optical cooling has very recently been demonstrated in cadmium sulfide (CdS) nanobelts as well as in hybrid lead halide perovskites. For the former, large internal quantum efficiencies, sub-wavelength thicknesses, which decrease light trapping, and low background absorption, all make near unity external quantum yields possible. Net cooling by as much as 40 K has therefore been possible with CdS nanobelts. In this study, we describe a detailed investigation of the nature of efficient anti-Stokes photoluminescence (ASPL) in CdS nanobelts. Temperature-dependent PL up-conversion and optical absorption studies on individual NBs together with frequency-dependent up-converted PL intensity spectroscopies suggest that ASPL in CdS nanobelts is defect-mediated through involvement of defect levels below the band gap.

Surface Traps in Colloidal Quantum Dots: A Combined Experimental and Theoretical Perspective.

PubMed

Giansante, Carlo; Infante, Ivan

2017-10-19

Surface traps are ubiquitous to nanoscopic semiconductor materials. Understanding their atomistic origin and manipulating them chemically have capital importance to design defect-free colloidal quantum dots and make a leap forward in the development of efficient optoelectronic devices. Recent advances in computing power established computational chemistry as a powerful tool to describe accurately complex chemical species and nowadays it became conceivable to model colloidal quantum dots with realistic sizes and shapes. In this Perspective, we combine the knowledge gathered in recent experimental findings with the computation of quantum dot electronic structures. We analyze three different systems: namely, CdSe, PbS, and CsPbI 3 as benchmark semiconductor nanocrystals showing how different types of trap states can form at their surface. In addition, we suggest experimental healing of such traps according to their chemical origin and nanocrystal composition.

Nanotwinning and structural phase transition in CdS quantum dots

NASA Astrophysics Data System (ADS)

Kumar, Pragati; Saxena, Nupur; Chandra, Ramesh; Gupta, Vinay; Agarwal, Avinash; Kanjilal, Dinakar

2012-10-01

Nanotwin structures are observed in high-resolution transmission electron microscopy studies of cubic phase CdS quantum dots in powder form by chemical co-precipitation method. The deposition of thin films of nanocrystalline CdS is carried out on silicon, glass, and TEM grids keeping the substrates at room temperature (RT) and 200°C by pulsed laser ablation. These films are then subjected to thermal annealing at different temperatures. Glancing angle X-ray diffraction results confirm structural phase transitions after thermal annealing of films deposited at RT and 200°C. The variation of average particle size and ratio of intensities in Raman peaks I 2LO/ I 1LO with annealing temperature are studied. It is found that electron-phonon interaction is a function of temperature and particle size and is independent of the structure. Besides Raman modes LO, 2LO and 3LO of CdS at approximately 302, 603, and 903 cm-1 respectively, two extra Raman modes at approximately 390 and 690 cm-1 are studied for the first time. The green and orange emissions observed in photoluminescence are correlated with phase transition.

Nanotwinning and structural phase transition in CdS quantum dots.

PubMed

Kumar, Pragati; Saxena, Nupur; Chandra, Ramesh; Gupta, Vinay; Agarwal, Avinash; Kanjilal, Dinakar

2012-10-23

Nanotwin structures are observed in high-resolution transmission electron microscopy studies of cubic phase CdS quantum dots in powder form by chemical co-precipitation method. The deposition of thin films of nanocrystalline CdS is carried out on silicon, glass, and TEM grids keeping the substrates at room temperature (RT) and 200°C by pulsed laser ablation. These films are then subjected to thermal annealing at different temperatures. Glancing angle X-ray diffraction results confirm structural phase transitions after thermal annealing of films deposited at RT and 200°C. The variation of average particle size and ratio of intensities in Raman peaks I2LO/I1LO with annealing temperature are studied. It is found that electron-phonon interaction is a function of temperature and particle size and is independent of the structure. Besides Raman modes LO, 2LO and 3LO of CdS at approximately 302, 603, and 903 cm-1 respectively, two extra Raman modes at approximately 390 and 690 cm-1 are studied for the first time. The green and orange emissions observed in photoluminescence are correlated with phase transition.

Photocatalytic activity of CdS and Ag2S quantum dots deposited on poly(amidoamine) functionalized carbon nanotubes

PubMed Central

Neelgund, Gururaj M.; Oki, Aderemi

2011-01-01

Two novel ternary nanocatalysts, f-MWCNTs-CdS and f-MWCNTs-Ag2S were successfully constructed by covalent grafting of fourth generation (G4) hyperbranched, crosslinked poly(amidoamine) (PAMAM) to carboxylated multi-walled carbon nanotubes (MWCNTs-COOH) and subsequent deposition of CdS or Ag2S quantum dots (QDs). The structural transformation, surface potential, and morphology of functionalized MWCNTs (f-MWCNTs) and nanocatalysts were characterized by UV-vis spectrophotometer, Fourier transform infrared spectroscopy, powder X-ray diffraction, Raman spectroscopy, thermogravimetric analysis, scanning electron microscopy and energy dispersive spectroscopy. Transmission electron microscopy reveals the effective anchoring of QDs on f-MWCNTs. The catalytic activity of nanocatalysts was evaluated by photodegradation of methyl orange under illumination of UV light. The coupling of MWCNTs, PAMAM and CdS or Ag2S QDs significantly enhanced the catalytic efficiency of nanocatalysts. The rate constants for degradation of methyl orange in presence of nanocatalysts were calculated using the Langmuir-Hinshelwood model. Overall, the excellence in photodegradation was accomplished by hybridizing f-MWCNTs with CdS or Ag2S PMID:22267895

Influence of heat treatment on hole transfer dynamics in core-shell quantum dot/organic hole conductor hybrid films

NASA Astrophysics Data System (ADS)

Sun, Mingye; Zheng, Youjin; Zhang, Lei; Zhao, Liping; Zhang, Bing

2017-08-01

The influence of heat treatment on hole transfer (HT) processes from the CdSe/ZnS and CdSe/CdS/ZnS quantum dots (QDs) to 4,4‧,4″-Tris(carbazol-9-yl)-triphenylamine (TCTA) in QD/TCTA hybrid films has been researched with time-resolved photoluminescence (PL) spectroscopy. The PL dynamic results demonstrated a heat-treatment-temperature-dependent HT process from the core-shell CdSe QDs to TCTA. The HT rates and efficiencies can be effectively increased due to reduced distance between core-shell CdSe QDs and TCTA after heat treatment. The CdS shell exhibited a more obvious effect on HT from the core-shell CdSe QDs to TCTA than on electron transfer to TiO2, due to higher barrier for holes to tunnel through CdS shell and larger effective mass of holes in CdS than electrons. These results indicate that heat treatment would be an effective means to further optimize solid-state QD sensitized solar cells and rational design of CdS shell is significant.

Detection of trace tetracycline in fish via synchronous fluorescence quenching with carbon quantum dots coated with molecularly imprinted silica

NASA Astrophysics Data System (ADS)

Yang, Ji; Lin, Zheng-Zhong; Nur, A.-Zha; Lu, Yan; Wu, Ming-Hui; Zeng, Jun; Chen, Xiao-Mei; Huang, Zhi-Yong

2018-02-01

A novel fluorescence-based sensor combining synchronous fluorescence spectroscopy (SFS) with molecularly imprinted polymers (MIPs) was fabricated with reverse microemulsion method. Tetracycline (TC), (3-aminopropyl) triethoxysilane (APTES), tetraethyl orthosilicate (TEOS) and carbon quantum dots (CDs) were used as template, functional monomer, cross-linker and signal sources respectively in the probe preparation. A synchronous fluorescence emission (λem) at 355 nm was observed for the prepared MIP-coated CDs (MIP@CDs) particles when the wavelength interval (Δλ) was set as 70 nm, and the synchronous fluorescence intensity could be rapidly and efficiently quenched by TC based on inner filter effect (IFE). The quenching efficiencies of synchronous fluorescence intensity was linearly fitted with tetracycline (TC) concentrations ranging from 0.1 to 50 μmol L- 1 with a detection limit (DL) of 9 nmol L- 1 (3σ, n = 9). The MIP@CDs was used as a probe to detect TC in fish samples with the recoveries ranging from 98.4% to 103.1% and the relative standard deviation less than 6.0%. The results illustrated that the as-prepared MIP@CDs could be applied to the detection of trace TC in fish samples with rapidity, high sensitivity and accuracy.

CdS quantum dots modified CuO inverse opal electrodes for ultrasensitive electrochemical and photoelectrochemical biosensor

PubMed Central

Xia, Lei; Xu, Lin; Song, Jian; Xu, Ru; Liu, Dali; Dong, Biao; Song, Hongwei

2015-01-01

The CuO inverse opal photonic crystals (IOPCs) were synthesized by the sol-gel method and modified with CdS quantum dots by successive ionic layer adsorption and reaction (SILAR). CdS QDs modified CuO IOPCs FTO electrodes of different SILAR cycles were fabricated and their electrochemical properties were studied by cyclic voltammetry (CV) and chronoamperometry (I–t). Structure and morphology of the samples were characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), high-resolution TEM (HRTEM), Energy-dispersive X-ray analysis (EDX) and X-ray diffraction pattern (XRD). The result indicated that the structure of IOPCs and loading of CdS QDs could greatly improve the electrochemical properties. Three SILAR cycles of CdS QDs sensitization was the optimum condition for preparing electrodes, it exhibited a sensitivity of 4345 μA mM-1 cm-2 to glucose with a 0.15 μM detection limit (S/N= 3) and a linear range from 0.15 μM to 0.5 mM under a working potential of +0.7 V. It also showed strong stability, good reproducibility, excellent selectivity and fast amperometric response. This work provides a promising approach for realizing excellent photoelectrochemical nonenzymatic glucose biosensor of similar composite structure. PMID:26042520

White light emitting device based on single-phase CdS quantum dots.

PubMed

Li, Feng; Nie, Chao; You, Lai; Jin, Xiao; Zhang, Qin; Qin, Yuancheng; Zhao, Feng; Song, Yinglin; Chen, Zhongping; Li, Qinghua

2018-05-18

White light emitting diodes (WLEDs) based on quantum dots (QDs) are emerging as robust candidates for white light sources, however they are suffering from the problem of energy loss resulting from the re-absorption and self-absorption among the employed QDs of different peak wavelengths. It still remains a challenging task to construct WLEDs based on single-phase QD emitters. Here, CdS QDs with short synthesis times are introduced to the fabrication of WLEDs. With a short synthesis time, on one hand, CdS QDs with a small diameter with blue emission can be obtained. On the other hand, surface reconstruction barely has time to occur, and the surface is likely defect-ridden, which enables the existence of a broad emission covering the range of green, yellow and red regions. This is essential for the white light emission of CdS QDs, and is very important for WLED applications. The temporal evolution of the PL spectra for CdS QDs was obtained to investigate the influence of growth time on the luminescent properties. The CdS QDs with a growth time of 0.5 min exhibited a colour rendering index (CRI) of 79.5 and a correlated colour temperature (CCT) of 6238 K. With increasing reaction time, the colour coordinates of the CdS QDs will move away from the white light region in the CIE 1931 chromaticity diagram. By integrating the as prepared white light emission CdS QDs with a violet GaN chip, WLEDs were fabricated. The fabricated WLEDs exhibited a CRI of 87.9 and a CCT of 4619 K, which satisfy the demand of general illumination. The luminous flux and the luminous efficiency of the fabricated WLEDs, being less advanced than current commercial white light sources, can be further improved, meaning there is a need for much more in-depth studies on white light emission CdS QDs.

White light emitting device based on single-phase CdS quantum dots

NASA Astrophysics Data System (ADS)

Li, Feng; Nie, Chao; You, Lai; Jin, Xiao; Zhang, Qin; Qin, Yuancheng; Zhao, Feng; Song, Yinglin; Chen, Zhongping; Li, Qinghua

2018-05-01

White light emitting diodes (WLEDs) based on quantum dots (QDs) are emerging as robust candidates for white light sources, however they are suffering from the problem of energy loss resulting from the re-absorption and self-absorption among the employed QDs of different peak wavelengths. It still remains a challenging task to construct WLEDs based on single-phase QD emitters. Here, CdS QDs with short synthesis times are introduced to the fabrication of WLEDs. With a short synthesis time, on one hand, CdS QDs with a small diameter with blue emission can be obtained. On the other hand, surface reconstruction barely has time to occur, and the surface is likely defect-ridden, which enables the existence of a broad emission covering the range of green, yellow and red regions. This is essential for the white light emission of CdS QDs, and is very important for WLED applications. The temporal evolution of the PL spectra for CdS QDs was obtained to investigate the influence of growth time on the luminescent properties. The CdS QDs with a growth time of 0.5 min exhibited a colour rendering index (CRI) of 79.5 and a correlated colour temperature (CCT) of 6238 K. With increasing reaction time, the colour coordinates of the CdS QDs will move away from the white light region in the CIE 1931 chromaticity diagram. By integrating the as prepared white light emission CdS QDs with a violet GaN chip, WLEDs were fabricated. The fabricated WLEDs exhibited a CRI of 87.9 and a CCT of 4619 K, which satisfy the demand of general illumination. The luminous flux and the luminous efficiency of the fabricated WLEDs, being less advanced than current commercial white light sources, can be further improved, meaning there is a need for much more in-depth studies on white light emission CdS QDs.

Preparation of highly luminescent and biocompatible carbon dots using a new extraction method

NASA Astrophysics Data System (ADS)

Zhang, Rui; Liu, Ying-Bo; Sun, Shu-Qing

2013-10-01

C dots (CDs) are among the most promising emerging fluorescent labels for biological imaging and sensing. A facile new synthesis method was developed using common organic solvents for fabricating CDs from candle soot. The common organic solvents were used as extractants and the obtained CDs have a narrow size distribution with average diameters of about 3.4 nm for ethylene glycol, 3.5 nm for ethanol, and 3.4 nm for n-butanol. This approach is simpler, easier, and more effective than other methods currently used for CD fabrication. The obtained CDs had a high quantum yield (38 %), tunable emission and are water-soluble. The mechanism for the luminescence of the CDs was investigated and the results indicate that the ability of the solvent to disperse the CDs plays a very important role in the photoluminescence of these CDs. The type of organic solvent and the surface groups on the CDs also influenced the optical properties of the CDs. Different emissive traps are shown to play the major role in the luminescence of the carbon materials. An in vitro hemolysis assay was performed and showed that the CDs are biocompatible.

Enhanced photoluminescence of corrugated Al2O3 film assisted by colloidal CdSe quantum dots.

PubMed

Bai, Zhongchen; Hao, Licai; Zhang, Zhengping; Huang, Zhaoling; Qin, Shuijie

2017-05-19

We present the enhanced photoluminescence (PL) of a corrugated Al 2 O 3 film enabled by colloidal CdSe quantum dots. The colloidal CdSe quantum dots are fabricated directly on a corrugated Al 2 O 3 substrate using an electrochemical deposition (ECD) method in a microfluidic system. The photoluminescence is excited by using a 150 nm diameter ultraviolet laser spot of a scanning near-field optical microscope. Owing to the electron transfer from the conduction band of the CdSe quantum dots to that of Al 2 O 3 , the enhanced photoluminescence effect is observed, which results from the increase in the recombination rate of electrons and holes on the Al 2 O 3 surface and the reduction in the fluorescence of the CdSe quantum dots. A periodically-fluctuating fluorescent spectrum was exhibited because of the periodical wire-like corrugated Al 2 O 3 surface serving as an optical grating. The spectral topographic map around the fluorescence peak from the Al 2 O 3 areas covered with CdSe quantum dots was unique and attributed to the uniform deposition of CdSe QDs on the corrugated Al 2 O 3 surface. We believe that the microfluidic ECD system and the surface enhanced fluorescence method described in this paper have potential applications in forming uniform optoelectronic films of colloidal quantum dots with controllable QD spacing and in boosting the fluorescent efficiency of weak PL devices.

Hydrothermal synthesis of nitrogen-doped carbon dots with real-time live-cell imaging and blood-brain barrier penetration capabilities.

PubMed

Lu, Shousi; Guo, Shanshan; Xu, Pingxiang; Li, Xiaorong; Zhao, Yuming; Gu, Wei; Xue, Ming

Nitrogen-doped carbon dots (N-CDs) were synthesized using a one-pot hydrothermal treatment with citric acid in the presence of polyethylenimine. Transmission electron microscopy analysis revealed that the N-CDs were monodispersed and quasi-spherical with an average size of ~2.6 nm. Under ultraviolet irradiation the N-CDs emitted a strong blue luminescence with a quantum yield as high as 51%. Moreover, the N-CDs exhibited a negligible cytotoxicity and could be applied as efficient nanoprobes for real-time imaging of live cells. In addition, the ability of the N-CDs to cross the blood-brain barrier (BBB) in a concentration-dependent manner was demonstrated using an in vitro BBB model. Therefore, these PEI-passivated N-CDs with real-time live-cell imaging and BBB-penetration capabilities hold promise for traceable drug delivery to the brain.

Highly fluorescent carbon dots for visible sensing of doxorubicin release based on efficient nanosurface energy transfer.

PubMed

Wang, Beibei; Wang, Shujun; Wang, Yanfang; Lv, Yan; Wu, Hao; Ma, Xiaojun; Tan, Mingqian

2016-01-01

To prepare fluorescent carbon dots for loading cationic anticancer drug through donor-quenched nanosurface energy transfer in visible sensing of drug release. Highly fluorescent carbon dots (CDs) were prepared by a facile hydrothermal approach from citric acid and o-phenylenediamine. The obtained CDs showed a high quantum yield of 46 % and exhibited good cytocompatibility even at 1 mg/ml. The cationic anticancer drug doxorubicin (DOX) can be loaded onto the negatively charged CDs through electrostatic interactions. Additionally, the fluorescent CDs feature reversible donor-quenched mode nanosurface energy transfer. When loading the energy receptor DOX, the donor CDs' fluorescence was switched "off", while it turned "on" again after DOX release from the surface through endocytic uptake. Most DOX molecules were released from the CDs after 6 h incubation and entered cell nuclear region after 8 h, suggesting the drug delivery system may have potential for visible sensing in drug release.

One-pot synthesis of fluorescent nitrogen-doped carbon dots with good biocompatibility for cell labeling.

PubMed

Zhang, Zhengwei; Yan, Kun; Yang, Qiulian; Liu, Yanhua; Yan, Zhengyu; Chen, Jianqiu

2017-12-01

Here we report an easy and economical hydrothermal carbonization approach to synthesize the fluorescent nitrogen-doped carbon dots (N-CDs) that was developed using citric acid and triethanolamine as the precursors. The synthesis conditions were optimized to obtain the N-CDs with superior fluorescence performances. The as-prepared N-CDs are monodispersed sphere nanoparticles with good water solubility, and exhibited strong fluorescence, favourable photostability and excitation wavelength-dependent behavior. Furthermore, the in vitro cytotoxicity and cellular labeling of N-CDs were investigated using the rat glomerular mesangial cells. The results showed the N-CDs have more inconspicuous cytotoxicity and better biosafety in comparison with ZnSe quantum dots, although both targeted the cells successfully. Considering their admirable photostability, low toxicity and good compatibility, the as-obtained N-CDs could have potential applications in biosensors, cellular imaging, and other fields. Copyright © 2017 John Wiley & Sons, Ltd.

Hydrothermal synthesis of nitrogen-doped carbon dots with real-time live-cell imaging and blood–brain barrier penetration capabilities

PubMed Central

Lu, Shousi; Guo, Shanshan; Xu, Pingxiang; Li, Xiaorong; Zhao, Yuming; Gu, Wei; Xue, Ming

2016-01-01

Nitrogen-doped carbon dots (N-CDs) were synthesized using a one-pot hydrothermal treatment with citric acid in the presence of polyethylenimine. Transmission electron microscopy analysis revealed that the N-CDs were monodispersed and quasi-spherical with an average size of ~2.6 nm. Under ultraviolet irradiation the N-CDs emitted a strong blue luminescence with a quantum yield as high as 51%. Moreover, the N-CDs exhibited a negligible cytotoxicity and could be applied as efficient nanoprobes for real-time imaging of live cells. In addition, the ability of the N-CDs to cross the blood–brain barrier (BBB) in a concentration-dependent manner was demonstrated using an in vitro BBB model. Therefore, these PEI-passivated N-CDs with real-time live-cell imaging and BBB-penetration capabilities hold promise for traceable drug delivery to the brain. PMID:27932880

Flow-injection chemiluminescence analysis for sensitive determination of atenolol using cadmium sulfide quantum dots.

PubMed

Khataee, Alireza; Lotfi, Roya; Hasanzadeh, Aliyeh; Iranifam, Mortaza; Joo, Sang Woo

2016-03-15

A sensitive, rapid and simple flow-injection chemiluminescence (CL) system based on the light emitted from KMnO4-cadmium sulfide quantum dots (CdS QDs) reaction in the presence of cetyltrimethylammonium bromide (CTAB) in acidic medium was developed as a CL probe for the sensitive determination of atenolol. Optical and structural features of CdS QDs capped with l-cysteine, which synthesized via hydrothermal approach, were investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM), photoluminescence (PL), and UV-Vis spectroscopy. The CL intensity of KMnO4-CdS QDs-CTAB was remarkably enhanced in the presence of trace level of atenolol. Under optimum experimental conditions, there is a linear relationship between the increase in CL intensity of KMnO4-CdS QDs-CTAB system and atenolol concentration in a range of 0.001 to 4.0 mg L(-1) and 4.0 to 18.0 mg L(-1), with a detection limit (3σ) of 0.0010 mg L(-1). A possible mechanism for KMnO4-CdS QDs-CTAB-atenolol CL reaction is proposed. To prove the practical application of the KMnO4-CdS QDs-CTAB CL method, the method was applied for the determination of atenolol in spiked environmental water samples and commercial pharmaceutical formulation. Furthermore, corona discharge ionization ion mobility spectrometry (CD-IMS) technique was utilized for determination of atenolol. Copyright © 2015 Elsevier B.V. All rights reserved.

Novel cookie-with-chocolate carbon dots displaying extremely acidophilic high luminescence

NASA Astrophysics Data System (ADS)

Lu, Siyu; Zhao, Xiaohuan; Zhu, Shoujun; Song, Yubin; Yang, Bai

2014-10-01

A fluorescent carbon dot with a cookie-with-chocolate film structure (about 5 × 5 μm2) showed a high fluorescence quantum yield (61.12%) at low pH. It was hydrothermally synthesized from l-serine and l-tryptophan. The formation mechanism of the film with carbon dots (CDs) was investigated. The film structure was formed by hydrogen bonding and π-π stacking interactions between aromatic rings. The strong blue fluorescence of the CDs increased under strong acidic conditions owing to the changes in the N-groups. These cookie-like CDs are attractive for their potential use as effective fluorescent probes for the sensitive detection of aqueous H+ and Fe3+.A fluorescent carbon dot with a cookie-with-chocolate film structure (about 5 × 5 μm2) showed a high fluorescence quantum yield (61.12%) at low pH. It was hydrothermally synthesized from l-serine and l-tryptophan. The formation mechanism of the film with carbon dots (CDs) was investigated. The film structure was formed by hydrogen bonding and π-π stacking interactions between aromatic rings. The strong blue fluorescence of the CDs increased under strong acidic conditions owing to the changes in the N-groups. These cookie-like CDs are attractive for their potential use as effective fluorescent probes for the sensitive detection of aqueous H+ and Fe3+. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr03965c

Hydrothermal growth of TiO2 nanowire membranes sensitized with CdS quantum dots for the enhancement of photocatalytic performance

PubMed Central

2014-01-01

In this paper, TiO2 nanowires (NWs) on Ti foils were prepared using a simple hydrothermal approach and annealing treatment. CdS quantum dots (QDs) were assembled onto the crystallized TiO2 NWs by sequential chemical bath deposition. Ultraviolet-visible absorption spectra showed that CdS adds bands in the visible to the TiO2 absorption and exhibited a broad absorption band in the visible region, which extended the scope of absorption spectrum and helped improve the photocatalytic degradation efficiency. The results of photocatalytic experiment revealed that CdS-TiO2 NWs possessed higher photocatalytic activities toward methyl orange than pure TiO2 nanowires. The degradation efficiency of 96.32% after ten cycles indicated that the as-prepared CdS-TiO2 composite exhibited excellent long-time recyclable ability and can be reused for the degradation of contaminants. PMID:24936164

[Determination of protein by CdS quantum dot fluorometry].

PubMed

Hu, Wei-Ping; Jiao, Man; Dong, Xue-Zhi; Wang, Xin

2011-02-01

Determination of protein content by fluorometry was carried out. In this experiment, CdS quantum dots (QDs) that have special spectral properties were prepared with sodium hexametaphosphate as stabilizer and mercapto acetic acid as modifier by hydrothermal synthesis method. Based on the increase in fluorescence intensity after CdS reacted with bovine serum albumin (BSA), a new method for the determination of protein was established. Results show that the fluorescence intensity of system has a good linear relationship with the concentration of BSA in the range of 0.001 43-0.250 mg x mL(-1), and the linear equation was F = 5 444.301 03 + 43.327 39c, relation coefficient (r) was 0.996 6, the limit of detection was 0.001 4 mg x mL(-1). The method has been used for the determination of protein in milk and egg, and compared with the standard method (biuret method), and the results were satisfactory.

Enhanced photocatalytic hydrogen evolution from in situ formation of few-layered MoS2/CdS nanosheet-based van der Waals heterostructures.

PubMed

Iqbal, Shahid; Pan, Ziwei; Zhou, Kebin

2017-05-25

Here we report for the first time that the H 2 bubbles generated by photocatalytic water splitting are effective in the layer-by-layer exfoliation of MoS 2 nanocrystals (NCs) into few layers. The as-obtained few layers can be in situ assembled with CdS nanosheets (NSs) into van der Waals heterostructures (vdWHs) of few-layered MoS 2 /CdS NSs which, in turn, are effective in charge separation and transfer, leading to enhanced photocatalytic H 2 production activity. The few-layered MoS 2 /CdS vdWHs exhibited a H 2 evolution rate of 140 mmol g (CdS) -1 h -1 and achieved an apparent quantum yield of 66% at 420 nm.

Cadmium sulfide quantum dots supported on gallium and indium oxide for visible-light-driven hydrogen evolution from water.

PubMed

Pan, Yun-xiang; Zhuang, Huaqiang; Hong, Jindui; Fang, Zheng; Liu, Hai; Liu, Bin; Huang, Yizhong; Xu, Rong

2014-09-01

In this work, CdS quantum dots (QDs) supported on Ga2O3 and In2O3 are applied for visible-light-driven H2 evolution from aqueous solutions that contain lactic acid. With Pt as the cocatalyst, the H2 evolution rates on CdS/Pt/Ga2O3 and CdS/Pt/In2O3 are as high as 995.8 and 1032.2 μmol h(-1), respectively, under visible light (λ>420 nm) with apparent quantum efficiencies of 43.6 and 45.3% obtained at 460 nm, respectively. These are much higher than those on Pt/CdS (108.09 μmol h(-1)), Pt/Ga2O3 (0.12 μmol h(-1)), and Pt/In2O3 (0.05 μmol h(-1)). The photocatalysts have been characterized thoroughly and their band structures and photocurrent responses have been measured. The band alignment between the CdS QDs and In2O3 can lead to interfacial charge separation, which cannot occur between the CdS QDs and Ga2O3. Among the various possible factors that contribute to the high H2 evolution rates on CdS/Pt/oxide, the surface properties of the metal oxides play important roles, which include (i) the anchoring of CdS QDs and Pt nanoparticles for favorable interactions and (ii) the efficient trapping of photogenerated electrons from the CdS QDs because of surface defects (such as oxygen defects) based on photoluminescence and photocurrent studies. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fluorescent chemosensor for pyridine based on N-doped carbon dots.

PubMed

Campos, B B; Abellán, C; Zougagh, M; Jimenez-Jimenez, J; Rodríguez-Castellón, E; Esteves da Silva, J C G; Ríos, A; Algarra, M

2015-11-15

Fluorescent carbon dots (CDs) and its nitrogen doped (N-CDs) nanoparticles have been synthesized from lactose as precursor using a bottom-up hydrothermal methodology. The synthesized nanoparticles have been characterized by elemental analysis, FTIR, Raman, TEM, DLS, XPS, and steady-state and life-time fluorescence. The synthesized carbon nanoparticles, CDs and N-CDs, have a size at about 7.7±2.4 and 50±15nm, respectively, and quantum yields of 8% (CDs) and 11% (N-CDs). These techniques demonstrated the effectiveness of the synthesis procedure and the functionalization of the CDs surface with amine and amide groups in the presence of NH3 in aqueous media. The effect of excitation wavelength and pH on the luminescent properties was studied. Under the optimal conditions, the nitrogen doped nanoparticles can be used as pyridine sensor in aqueous media because they show an enhancement of its fluorescence with a good linear relationship. The analytical method is simple, reproducible and very sensitive for pyridine determination. Copyright © 2015 Elsevier Inc. All rights reserved.

Surface Traps in Colloidal Quantum Dots: A Combined Experimental and Theoretical Perspective

PubMed Central

2017-01-01

Surface traps are ubiquitous to nanoscopic semiconductor materials. Understanding their atomistic origin and manipulating them chemically have capital importance to design defect-free colloidal quantum dots and make a leap forward in the development of efficient optoelectronic devices. Recent advances in computing power established computational chemistry as a powerful tool to describe accurately complex chemical species and nowadays it became conceivable to model colloidal quantum dots with realistic sizes and shapes. In this Perspective, we combine the knowledge gathered in recent experimental findings with the computation of quantum dot electronic structures. We analyze three different systems: namely, CdSe, PbS, and CsPbI3 as benchmark semiconductor nanocrystals showing how different types of trap states can form at their surface. In addition, we suggest experimental healing of such traps according to their chemical origin and nanocrystal composition. PMID:28972763

Size, surface, and compositional tuning of the electronic and photocatalytic properties of II-VI quantum-size semiconductor nanocrystals

NASA Astrophysics Data System (ADS)

Korgel, Brian Allan

1997-11-01

Phosphatidylcholine vesicles provide reaction compartments for synthesis of size-quantized CdS nanocrystals of dimension predicted to within ±2 A based on initial encapsulated CdClsb2 concentration and vesicle diameter. Vesicle formation by detergent dialysis of phosphatidylcholine/hexylglucoside mixed micelles yields highly monodisperse lipid capsules within which monodisperse CdS nanoparticles are precipitated with sulfide. Size-quantized CdS nanocrystals, with diameters ranging from 20 to 60 A, have been produced with typical standard deviations about the mean diameter of ±8% as measured by transmission electron microscopy. By including ZnClsb2 or HgClsb2 in the dialyzate prior to vesicle formation, quantum-sized Znsb{y}Cdsb{1-y}S or Hgsb{y}Cdsb{1-y}S nanocrystal alloys with controlled stoichiometry are generated. Spectrophotometric and spectrofluorimetric measurements are consistent with highly crystalline, monodisperse particles with few core or surface defects. The alloyed nanocrystal spectra shift consistently with composition indicating a high degree of compositional control. Measured exciton energies for CdS show excellent agreement with data in the literature. The empirical pseudopotential model presented by Ramakrishna and Friesner for a cubic CdS lattice, correcting for experimentally measured lattice contractions, best fits the data. Size-quantized CdS nanocrystals serve as photocatalysts for nitrate reduction at neutral pH under conditions that mimic illumination by sunlight with overall product quantum yields of up to 4% for {˜}20 A, amine-terminated particles. Due to the effects of quantum confinement on electron and hole redox potentials, photocatalyzed nitrate reduction rates depend strongly on the particle size, and the fastest reduction rates are observed with the smallest nanocrystals. Using a Tafel plot and the empirical pseudopotential model to estimate electron redox potentials, the apparent electron transfer coefficient and the apparent standard rate constant is estimated at 0.23 and 4.0× 10sp{-12} cm/sec, respectively, for amine-terminated particles. Nitrate adsorption is important in this system and the effect on photoreduction rates is described well by a Langmuir-Hinschelwood expression. Nitrate reduction rates are reduced two-fold or more on negatively charged, carboxy-terminated nanocrystals that electrostatically repel nitrate. Reaction rates are additionally influenced by competetive chloride adsorption and surface charge modification due to solution pH.

Erythorbic acid promoted formation of CdS QDs in a tube-in-tube micro-channel reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liang, Yan; Tan, Jiawei; Wang, Jiexin

2014-12-15

Erythorbic acid assistant synthesis of CdS quantum dots (QDs) was conducted by homogeneous mixing of two continuous liquids in a high-throughput microporous tube-in-tube micro-channel reactor (MTMCR) at room temperature. The effects of the micropore size of the MTMCR, liquid flow rate, mixing time and reactant concentration on the size and size distribution of CdS QDs were investigated. It was found that the size and size distribution of CdS QDs could be tuned in the MTMCR. A combination of erythorbic acid promoted formation technique with the MTMCR may be a promising pathway for controllable mass production of QDs.

Detection of Hg2+ ion using fluorescent carbon dots derived from elephant foot yum via green-chemistry

NASA Astrophysics Data System (ADS)

Choudhary, Raksha; Madhuri, Rashmi; Sharma, Prashant K.

2017-05-01

We have synthesized a fluorescent carbon dots (CDs) in an eco-friendly and cost effective manner through the combination of microwave plus hydrothermal process using elephant foot yam (Amorphophallus paeoniifolius) as carbon precursor. Combination of two processes was used to save time as well as energy with less use of harsh chemicals. The resultant CDs has good photostability, high quantum yield, excellent water dispersibility and high storage ability. Further, CDs was applied for the detection of Hg2+ ion from aqueous and real samples.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raja, Shilpa N.; Zherebetskyy, Danylo; Wu, Siva

Nanoscale stress-sensing can be used across fields ranging from detection of incipient cracks in structural mechanics to monitoring forces in biological tissues. We demonstrate how tetrapod quantum dots (tQDs) embedded in block copolymers act as sensors of tensile/compressive stress. Remarkably, tQDs can detect their own composite dispersion and mechanical properties with a switch in optomechanical response when tQDs are in direct contact. Using experimental characterizations, atomistic simulations and finite-element analyses, we show that under tensile stress, densely packed tQDs exhibit a photoluminescence peak shifted to higher energies ("blue-shift") due to volumetric compressive stress in their core; loosely packed tQDs exhibitmore » a peak shifted to lower energies ("red-shift") from tensile stress in the core. The stress shifts result from the tQD's unique branched morphology in which the CdS arms act as antennas that amplify the stress in the CdSe core. Our nanocomposites exhibit excellent cyclability and scalability with no degraded properties of the host polymer. Colloidal tQDs allow sensing in many materials to potentially enable autoresponsive, smart structural nanocomposites that self-predict upcoming fracture.« less

Luminescence in Sulfides: A Rich History and a Bright Future

PubMed Central

Smet, Philippe F.; Moreels, Iwan; Hens, Zeger; Poelman, Dirk

2010-01-01

Sulfide-based luminescent materials have attracted a lot of attention for a wide range of photo-, cathodo- and electroluminescent applications. Upon doping with Ce3+ and Eu2+, the luminescence can be varied over the entire visible region by appropriately choosing the composition of the sulfide host. Main application areas are flat panel displays based on thin film electroluminescence, field emission displays and ZnS-based powder electroluminescence for backlights. For these applications, special attention is given to BaAl2S4:Eu, ZnS:Mn and ZnS:Cu. Recently, sulfide materials have regained interest due to their ability (in contrast to oxide materials) to provide a broad band, Eu2+-based red emission for use as a color conversion material in white-light emitting diodes (LEDs). The potential application of rare-earth doped binary alkaline-earth sulfides, like CaS and SrS, thiogallates, thioaluminates and thiosilicates as conversion phosphors is discussed. Finally, this review concludes with the size-dependent luminescence in intrinsic colloidal quantum dots like PbS and CdS, and with the luminescence in doped nanoparticles.

Highly Efficient Light-Emitting Diodes of Colloidal Metal-Halide Perovskite Nanocrystals beyond Quantum Size.

PubMed

Kim, Young-Hoon; Wolf, Christoph; Kim, Young-Tae; Cho, Himchan; Kwon, Woosung; Do, Sungan; Sadhanala, Aditya; Park, Chan Gyung; Rhee, Shi-Woo; Im, Sang Hyuk; Friend, Richard H; Lee, Tae-Woo

2017-07-25

Colloidal metal-halide perovskite quantum dots (QDs) with a dimension less than the exciton Bohr diameter D B (quantum size regime) emerged as promising light emitters due to their spectrally narrow light, facile color tuning, and high photoluminescence quantum efficiency (PLQE). However, their size-sensitive emission wavelength and color purity and low electroluminescence efficiency are still challenging aspects. Here, we demonstrate highly efficient light-emitting diodes (LEDs) based on the colloidal perovskite nanocrystals (NCs) in a dimension > D B (regime beyond quantum size) by using a multifunctional buffer hole injection layer (Buf-HIL). The perovskite NCs with a dimension greater than D B show a size-irrespective high color purity and PLQE by managing the recombination of excitons occurring at surface traps and inside the NCs. The Buf-HIL composed of poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (PEDOT:PSS) and perfluorinated ionomer induces uniform perovskite particle films with complete film coverage and prevents exciton quenching at the PEDOT:PSS/perovskite particle film interface. With these strategies, we achieved a very high PLQE (∼60.5%) in compact perovskite particle films without any complex post-treatments and multilayers and a high current efficiency of 15.5 cd/A in the LEDs of colloidal perovskite NCs, even in a simplified structure, which is the highest efficiency to date in green LEDs that use colloidal organic-inorganic metal-halide perovskite nanoparticles including perovskite QDs and NCs. These results can help to guide development of various light-emitting optoelectronic applications based on perovskite NCs.

Double-Sided Transparent TiO2 Nanotube/ITO Electrodes for Efficient CdS/CuInS2 Quantum Dot-Sensitized Solar Cells

NASA Astrophysics Data System (ADS)

Chen, Chong; Ling, Lanyu; Li, Fumin

2017-01-01

In this paper, to improve the power conversion efficiencies (PCEs) of quantum dot-sensitized solar cells (QDSSCs) based on CdS-sensitized TiO2 nanotube (TNT) electrodes, two methods are employed on the basis of our previous work. First, by replacing the traditional single-sided working electrodes, double-sided transparent TNT/ITO (DTTO) electrodes are prepared to increase the loading amount of quantum dots (QDs) on the working electrodes. Second, to increase the light absorption of the CdS-sensitized DTTO electrodes and improve the efficiency of charge separation in CdS-sensitized QDSSCs, copper indium disulfide (CuInS2) is selected to cosensitize the DTTO electrodes with CdS, which has a complementary property of light absorption with CdS. The PCEs of QDSSCs based on these prepared QD-sensitized DTTO electrodes are measured. Our experimental results show that compared to those based on the CdS/DTTO electrodes without CuInS2, the PCEs of the QDSSCs based on CdS/CuInS2-sensitized DTTO electrode are significantly improved, which is mainly attributed to the increased light absorption and reduced charge recombination. Under simulated one-sun illumination, the best PCE of 1.42% is achieved for the QDSSCs based on CdS(10)/CuInS2/DTTO electrode, which is much higher than that (0.56%) of the QDSSCs based on CdS(10)/DTTO electrode.

Preparation and characterization of photocatalytic carbon dots-sensitized electrospun titania nanostructured fibers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Haopeng; Zhu, Yihua, E-mail: yhzhu@ecust.edu.cn; Cao, Huimin

2013-02-15

Graphical abstract: Display Omitted Highlights: ► The TiO{sub 2}-CDs nanostructured fibers are fabricated by using APS combining the electrospinning TiO{sub 2} nanostructured fibers and CDs. ► The CD can work as a photosensitizer in the degradation of rhodamine B under visible light irradiation. ► The TiO{sub 2}-CDs nanostructured fibers exhibit enhanced photocatalytic efficiency and can be easily handled and recycled. -- Abstract: The carbon dots (CDs) are new functional carbon-aceous materials. Compared to conventional dye molecules and semiconductor quantum dots, CDs are superior in chemical inertness and low toxicity. The TiO{sub 2}-CDs nanostructured fibers were fabricated by combining the electrospinningmore » technique and reflux method. Compared with the pure TiO{sub 2} nanostructured fibers and P25, the TiO{sub 2}-CDs nanostructured fibers exhibited enhanced photocatalytic efficiency of photodegradation of rhodamine B (RhB) under visible light irradiation. The enhanced photocatalytic activity of TiO{sub 2}-CDs nanostructured fibers could be attributed to the presence of CDs embedded in TiO{sub 2} nanostructured fibers. The CD can work as a photosensitizer in the degradation. Furthermore, the TiO{sub 2}-CDs nanostructured fibers could be easily handled and recycled due to their one-dimensional nanostructural property.« less

Effect of sodium acetate additive in successive ionic layer adsorption and reaction on the performance of CdS quantum-dot-sensitized solar cells

NASA Astrophysics Data System (ADS)

Liu, I.-Ping; Chen, Liang-Yih; Lee, Yuh-Lang

2016-09-01

Sodium acetate (NaAc) is utilized as an additive in cationic precursors of the successive ionic layer adsorption and reaction (SILAR) process to fabricate CdS quantum-dot (QD)-sensitized photoelectrodes. The effects of the NaAc concentration on the deposition rate and distribution of QDs in mesoporous TiO2 films, as well as on the performance of CdS-sensitized solar cells are studied. The experimental results show that the presence of NaAc can significantly accelerate the deposition of CdS, improve the QD distribution across photoelectrodes, and thereby, increase the performance of solar cells. These results are mainly attributed to the pH-elevation effect of NaAc to the cationic precursors which increases the electrostatic interaction of the TiO2 film to cadmium ions. The light-to-energy conversion efficiency of the CdS-sensitized solar cell increases with increasing concentration of the NaAc and approaches a maximum value (3.11%) at 0.05 M NaAc. Additionally, an ionic exchange is carried out on the photoelectrode to transform the deposited CdS into CdS1-xSex ternary QDs. The light-absorption range of the photoelectrode is extended and an exceptional power conversion efficiency of 4.51% is achieved due to this treatment.

Microwave formation and photoluminescence mechanisms of multi-states nitrogen doped carbon dots

NASA Astrophysics Data System (ADS)

He, Guili; Shu, Mengjun; Yang, Zhi; Ma, Yujie; Huang, Da; Xu, Shusheng; Wang, Yanfang; Hu, Nantao; Zhang, Yafei; Xu, Lin

2017-11-01

In recent years, carbon dots (CDs) have attracted much attention in the material field because of their remarkable performance in various aspects. Therefore, the exploration of complex and variable photoluminescence mechanisms shows great significance. Herein, we present a systematic study on the correlation between the formation process and photoluminescence mechanisms through the characterization and analysis of three states of nitrogen doped carbon dots (N-CDs) obtained by microwave irradiation. At low temperature of 160 °C, the small organic molecule polymer nanodots whose photoluminescence center is molecule state are obtained with superior quantum yield of about 51.61%. Increasing the reaction temperature up to 200 °C, the intermediate transition products named carbon nanodots begin to appear. Prolonging the holding time, the typical carbon quantum dots with a special stable optical properties are finally generated, and their most photoluminescence arises from the carbon cores which are gained through the polymerization, dehydration, carbonation of organic fluorescent molecules. Furthermore, N-CDs have been applied in metal ions detection as well as animal and plant cell fluorescence imaging owing to their excellent water solubility and low cytotoxicity. Our exploration provides the theoretical basis for synthesis of CDs with different properties and purposes. In the near future, more high-quality CDs will be developed in order to better benefit the various fields of mankind.

Ag nanoclusters could efficiently quench the photoresponse of CdS quantum dots for novel energy transfer-based photoelectrochemical bioanalysis.

PubMed

Zhang, Ling; Sun, Yue; Liang, Yan-Yu; He, Jian-Ping; Zhao, Wei-Wei; Xu, Jing-Juan; Chen, Hong-Yuan

2016-11-15

Herein the influence of ultrasmall Ag nanoclusters (Ag NCs) against CdS quantum dots (QDs) in a photoelectrochemical (PEC) nanosystem was exploited for the first time, based on which a novel PEC bioanalysis was successfully developed via the efficient quenching effect of Ag NCs against the CdS QDs. In a model system, DNA assay was achieved by using molecular beacon (MB) probes anchored on a CdS QDs modified electrode, and the MB probes contain two segments that can hybridize with both target DNA sequence and the label of DNA encapsulated Ag NCs. After the MB probe was unfolded by the target DNA sequence, the labels of oligonucleotide encapsulated Ag NCs would be brought in close proximity to the CdS QDs electrode surface, and efficient photocurrent quenching of QDs could be resulted from an energy transfer process that originated from NCs. Thus, by monitoring the attenuation in the photocurrent signal, an elegant and sensitive PEC DNA bioanalysis could be accomplished. The developed biosensor displayed a linear range from 1.0pM to 10nM and the detection limit was experimentally found to be of 0.3pM. This work presents a feasible signaling principle that could act as a common basis for general PEC bioanalysis development. Copyright © 2016 Elsevier B.V. All rights reserved.

Nanotwinning and structural phase transition in CdS quantum dots

PubMed Central

2012-01-01

Nanotwin structures are observed in high-resolution transmission electron microscopy studies of cubic phase CdS quantum dots in powder form by chemical co-precipitation method. The deposition of thin films of nanocrystalline CdS is carried out on silicon, glass, and TEM grids keeping the substrates at room temperature (RT) and 200°C by pulsed laser ablation. These films are then subjected to thermal annealing at different temperatures. Glancing angle X-ray diffraction results confirm structural phase transitions after thermal annealing of films deposited at RT and 200°C. The variation of average particle size and ratio of intensities in Raman peaks I2LO/I1LO with annealing temperature are studied. It is found that electron-phonon interaction is a function of temperature and particle size and is independent of the structure. Besides Raman modes LO, 2LO and 3LO of CdS at approximately 302, 603, and 903 cm−1 respectively, two extra Raman modes at approximately 390 and 690 cm−1 are studied for the first time. The green and orange emissions observed in photoluminescence are correlated with phase transition. PMID:23092351

Synthesis and Adsorption Study of BSA Surface Imprinted Polymer on CdS Quantum Dots

NASA Astrophysics Data System (ADS)

Tang, Ping-ping; Cai, Ji-bao; Su, Qing-de

2010-04-01

A new bovine serum albumin (BSA) surface imprinting method was developed by the incorporation of quantum dots (QDs) into molecularly imprinted polymers (MIP), which can offer shape selectivity. Preparation and adsorption conditions were optimized. Physical appearance of the QDs and QDs-MIP particles was illustrated by scanning electron microscope images. Photoluminescence emission of CdS was quenched when rebinding of the template. The quenching of photoluminescence emissions is presumably due to the fluorescence resonance energy transfer between quantum dots and BSA template molecules. The adsorption is compiled with Langmuir isotherm, and chemical adsorption is the rate-controlling step. The maximum adsorption capacity could reach 226.0 mg/g, which is 142.4 mg/g larger than that of undoped BSA MIP. This study demonstrates the validity of QDs coupled with MIP technology for analyzing BSA.

Integrated photonics using colloidal quantum dots

NASA Astrophysics Data System (ADS)

Menon, Vinod M.; Husaini, Saima; Okoye, Nicky; Valappil, Nikesh V.

2009-11-01

Integrated photonic devices were realized using colloidal quantum dot composites such as flexible microcavity laser, microdisk emitters and integrated active-passive waveguides. The microcavity laser structure was realized using spin coating and consisted of an all-polymer distributed Bragg reflector with a poly-vinyl carbazole cavity layer embedded with InGaP/ZnS colloidal quantum dots. These microcavities can be peeled off the substrate yielding a flexible structure that can conform to any shape and whose emission spectra can be mechanically tuned. Planar photonic devices consisting of vertically coupled microring resonators, microdisk emitters, active-passive integrated waveguide structures and coupled active microdisk resonators were realized using soft lithography, photo-lithography, and electron beam lithography, respectively. The gain medium in all these devices was a composite consisting of quantum dots embedded in SU8 matrix. Finally, the effect of the host matrix on the optical properties of the quantum dots using results of steady-state and time-resolved luminescence measurements was determined. In addition to their specific functionalities, these novel device demonstrations and their development present a low-cost alternative to the traditional photonic device fabrication techniques.

Photonic emitters and circuits based on colloidal quantum dot composites

NASA Astrophysics Data System (ADS)

Menon, Vinod M.; Husaini, Saima; Valappil, Nikesh; Luberto, Matthew

2009-02-01

We discuss our work on light emitters and photonic circuits realized using colloidal quantum dot composites. Specifically we will report our recent work on flexible microcavity laser, microdisk emitters and integrated active - passive waveguides. The entire microcavity laser structure was realized using spin coating and consisted of an all-polymer distributed Bragg reflector with a poly-vinyl carbazole cavity layer embedded with InGaP/ZnS colloidal quantum dots. These microcavities can be peeled off the substrate yielding a flexible structure that can conform to any shape and whose emission spectra can be mechanically tuned. The microdisk emitters and the integrated waveguide structures were realized using soft lithography and photo-lithography, respectively and were fabricated using a composite consisting of quantum dots embedded in SU8 matrix. Finally, we will discuss the effect of the host matrix on the optical properties of the quantum dots using results of steady-state and time-resolved luminescence measurements. In addition to their specific functionalities, these novel device demonstrations and their development present a low cost alternative to the traditional photonic device fabrication techniques.

Photosensitized electron transfer processes in SiO2 colloids and sodium lauryl sulfate micellar systems: Correlation of quantum yields with interfacial surface potentials

PubMed Central

Laane, Colja; Willner, Itamar; Otvos, John W.; Calvin, Melvin

1981-01-01

The effectiveness of negatively charged colloidal SiO2 particles in controlling photosensitized electron transfer reactions has been studied and compared with that of the negatively charged sodium lauryl sulfate (NaLauSO4) micellar system. In particular, the photosensitized reduction of the zwitterionic electron acceptor propylviologen sulfonate (PVS0) with tris(2,2′-bipyridinium)ruthenium(II) [Ru(bipy)32+] as the sensitizer and triethanolamine as the electron donor is found to have a quantum yield of 0.033 for formation of the radical anion (PVS[unk]) in the SiO2 colloid compared with 0.005 in the homogeneous system and 0.0086 in a NaLauSO4 micellar solution. The higher quantum yields obtained with the SiO2 colloidal system are attributed to substantial stabilization against back reaction of the intermediate photoproducts—i.e., Ru(bipy)33+ and PVS[unk]—by electrostatic repulsion of the reduced electron acceptor from the negatively charged particle surface. The binding properties of the SiO2 particles and NaLauSO4 micelles were investigated by flow dialysis. The results show that the sensitizer binds to both interfaces and that the SiO2 interface is characterized by a much higher surface potential than the micellar interface (≈-170 mV vs. -85 mV). The effect of ionic strength on the surface potential was estimated from the Gouy-Chapman theory, and the measured quantum yields of photosensitized electron transfer were correlated with surface potential at different ionic strengths. This correlation shows that the quantum yield is not affected by surface potentials smaller than ≈-40 mV. At larger potentials, the quantum yield increases rapidly. The quantum yield obtained in the micellar system at different strengths fits nicely on the correlation curve for the colloid SiO2 system. These results indicate that the surface potential is the dominant factor in the quantum yield improvement for PVS0 reduction. PMID:16593095

Red, green, and blue lasing enabled by single-exciton gain in colloidal quantum dot films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nurmikko, Arto V.; Dang, Cuong

The methods and materials described herein contemplate the use films of colloidal quantum dots as a gain medium in a vertical-cavity surface-emitting laser. The present disclosure demonstrates a laser with single-exciton gain in the red, green, and blue wavelengths. Leveraging this nanocomposite gain, the results realize a significant step toward full-color single-material lasers.

Red carbon dots-based phosphors for white light-emitting diodes with color rendering index of 92.

PubMed

Zhai, Yuechen; Wang, Yi; Li, Di; Zhou, Ding; Jing, Pengtao; Shen, Dezhen; Qu, Songnan

2018-05-29

Exploration of solid-state efficient red emissive carbon dots (CDs) phosphors is strongly desired for the development of high performance CDs-based white light-emitting diodes (WLEDs). In this work, enhanced red emissive CDs-based phosphors with photoluminescence quantum yields (PLQYs) of 25% were prepared by embedding red emissive CDs (PLQYs of 23%) into polyvinyl pyrrolidone (PVP). Because of the protection of PVP, the phosphors could preserve strong luminescence under long-term UV excitation or being mixed with conventional packaging materials. By applying the red emissive phosphors as the color conversion layer, WLEDs with high color rendering index of 92 and color coordinate of (0.33, 0.33) are fabricated. Copyright © 2018 Elsevier Inc. All rights reserved.

One-Step Hydrothermal Approach to Synthesis Carbon Dots from D-Sorbitol for Detection of Iron(III) and Cell Imaging.

PubMed

Zhang, Junqiu; Yan, Juping; Wang, Yingte; Zhang, Yong

2018-07-01

A facile and economic approach to synthesis highly fluorescence carbon dots (CDs) via one-step hydrothermal treatment of D-sorbitol was presented. The as-synthesized CDs were characterized by good water solubility, well monodispersion, and excellent biocompatibility. Spherical CDs had a particle size about 5 nm and exhibited a quantum yield of 8.85% at excitation wavelength of 360 nm. In addition, the CDs can serve as fluorescent probe for sensitive and selective detection of Fe3+ ions with the detection limit of 1.16 μM. Moreover, the potential of the as-prepared carbon dots for biological application was confirmed by employing it for fluorescence imaging in MCF-7 cells.

New Meta Nanomaterials Extension II of Optical Enhancement and Photorefractive Two-Beam Coupling - Synthesis and Fabrication of Quantum Dot NLO Polymer Composites

DTIC Science & Technology

2015-07-09

peaks at -65, which is assigned to Si(- OSi )3. All of these signals are consistent with the functionalization of CdS with MPS. However, another intense...OR CdS S RO 5 Si S OR SiO OR OR CdS S OR Si RO Si O ORRO S CdS S Si S S Si O O O O O O 6 Si Si Si SiSi O Si = OSi n Figure 3. Possible alternative...on this assumption, we attribute the peak in the 29Si SSNMR spectrum at-57 ppm to Si(- OSi )2O(R/H) groups, respectively, where R = CH3 and the weak

Tuning band alignment by CdS layers using a SILAR method to enhance TiO2/CdS/CdSe quantum-dot solar-cell performance.

PubMed

Zhang, Bingkai; Zheng, Jiaxin; Li, Xiaoning; Fang, Yanyan; Wang, Lin-Wang; Lin, Yuan; Pan, Feng

2016-04-28

We report tuning band alignment by optimized CdS layers using a SILAR method to achieve the recorded best performance with about 6% PCE in TiO2/CdS/CdSe QDSSCs. Combining experimental and theoretical studies, we find that a better lattices match between CdS and TiO2 assists the growth of CdSe, and the combined effect of charge transfer and surface dipole moment at the TiO2/CdS/CdSe interface shifts the energy levels of TiO2 upward and increases Voc of the solar cells. More importantly, the band gap of CdS buffer layers is sensitive to the distortion induced by lattice mismatch and numbers of CdS layers. For example, the barrier for charge transfer disappears when there are more than 4 layers of CdS, facilitating the charge injection from CdSe to TiO2.

Prominence of fusion temperature and engineering heteroatoms on multifarious emissive shifts in carbon dots.

PubMed

Velusamy, Jayaramakrishnan; Ramos-Ortiz, Gabriel; Rodríguez, Mario; Hernández-Cruz, Olivia; Ponce, Arturo

2018-05-16

We present a simple but robust strategy to engineering heteroatoms (N, S) on carbon dots (CDs) surface that results in a collection of enhanced photoluminescence (PL) emissions. The use of citric acid (CA) and 2-Imidazolidinethione (2-IZT) as precursors was envisioned to study the impact of thermolysis process on the PL properties. The proposed strategy, implemented at two different temperatures (180 °C and 200 °C), is suitable to produce CDs with tunable PL and quantum yield (QY) up to ∼32%. Similar to earlier reports of CA-based CDs, the self-assembling of fluorophores integrated into the CDs edge is hypothesized, however, in our CDs a double intriguing effect of blue- and red-shifting can be observed for PL as the wavelength of excitation is increased in the range 280-480 nm. Through a comprehensive characterization and evaluation of these CDs in water suspensions, the mechanisms that lead to PL multifarious emissions are proposed. Copyright © 2018 Elsevier Inc. All rights reserved.

Highly Efficient Red-Emitting Carbon Dots with Gram-Scale Yield for Bioimaging.

PubMed

Ding, Hui; Wei, Ji-Shi; Zhong, Ning; Gao, Qing-Yu; Xiong, Huan-Ming

2017-11-07

Carbon dots (CDs) are a new class of photoluminescent (PL), biocompatible, environment-friendly, and low-cost carbon nanomaterials. Synthesis of highly efficient red-emitting carbon dots (R-CDs) on a gram scale is a great challenge at present, which heavily restricts the wide applications of CDs in the bioimaging field. Herein, R-CDs with a high quantum yield (QY) of 53% are produced on a gram scale by heating a formamide solution of citric acid and ethylenediamine. The as-prepared R-CDs have an average size of 4.1 nm and a nitrogen content of about 30%, with an excitation-independent emission at 627 nm. After detailed characterizations, such strong red fluorescence is ascribed to the contribution from the nitrogen- and oxygen-related surface states and the nitrogen-derived structures in the R-CD cores. Our R-CDs show good photostability and low cytotoxicity, and thus they are excellent red fluorescence probes for bioimaging both in vitro and in vivo.

Facile synthesis of S, N co-doped carbon dots and investigation of their photoluminescence properties.

PubMed

Zhang, Yue; He, Junhui

2015-08-21

A facile one-pot approach to prepare photoluminescent carbon dots (CDs) was developed through hydrothermal treatment of cysteine and citric acid. The obtained CDs show stable and bright blue emission with a quantum yield of 54% and an average lifetime of 11.61 ns. Moreover, the two-photon induced upconversion fluorescence of the CDs was observed and demonstrated. Interestingly, both down and up conversion fluorescence of the CDs show excitation-independent emission, which is quite different from most of the previously reported CDs. Ultrafast spectroscopy was also employed here to study the photoluminescence (PL) properties of the CDs. After characterization using various spectroscopic techniques, a unique PL mechanism for the as-prepared CDs' fluorescence was proposed accordingly. In addition, the influence of various metal ions on the CD fluorescence was examined and no quenching phenomena were observed. Meanwhile, gold nanoparticles (Au NPs) were found to be good quenchers of CD fluorescence and their quenching behavior was fitted to the Stern-Volmer equation. This provides new opportunities for fluorescence sensor designs and light energy conversion applications. Finally, the as-prepared CDs were inkjet-printed to form a desirable pattern, which is useful for fluorescent patterns, and anti-counterfeiting labeling.

A new photoelectric ink based on nanocellulose/CdS quantum dots for screen-printing.

PubMed

Tang, Aimin; Liu, Yuan; Wang, Qinwen; Chen, Ruisong; Liu, Wangyu; Fang, Zhiqiang; Wang, Lishi

2016-09-05

CdS quantum dots with excellent photoelectrical properties embedded in nanocellulose could be exploited for use in photoelectrical ink. In this work, nanocellulose/CdS quantum dot composites were fabricated by controlling the carboxylate content of the nanocellulose and the molar ratio of Cd(2+)/-COOH. New photoelectric inks were prepared based on the composites, in which the CdS quantum dots acted as the pigment and the nanocellulose as the binder. The results of the photocurrent of the composites showed that the photocurrent could be tailored by the carboxylate content and the molar ratio of Cd(2+)/-COOH. And the photocurrent could be as high as 2μA. The surface tension of the photoelectric ink was 27.80±0.03mN/m and its viscosity was 30.3mPas. The photoelectric ink was stable with excellent fluidity and rheology, it could therefore be applied to screen-printing and three-dimensional (3D) printing. Copyright © 2016 Elsevier Ltd. All rights reserved.

CdS quantum dots in a novel glass with a very low activation energy and its variation of diffusivity with temperature

NASA Astrophysics Data System (ADS)

Nagpal, Swati

2011-07-01

CdS quantum dots of different average sizes in the range 2 to 3.8 nm were grown by diffusion-limited growth process in indigenously made silicate glass. The absorption spectra showed a strong quantum confinement effect with a blue shift of the order of 500 meV depending on the average size. Critical radius of quantum dots was found to be 1.8 nm. The size dispersion decreased from 15.2 to 12.5% with a 20% increase in the particle size. The activation energy for diffusion was found to be very low i.e. 193 kJ mol-1 and the diffusion coefficient increased by 60% for 10 K rise in temperature. The PL emission spectra showed the presence of only deep traps around 600 nm with a red shift of 200 nm. No shallow traps or band edge emission was observed. The PL peak position changed from 560 to 640 nm with a 35 K increase in annealing temperature.

Design of a High-Power White Light Source with Colloidal Quantum Dots and Non-Rare-Earth Phosphors

NASA Astrophysics Data System (ADS)

Bicanic, Kristopher T.

This thesis describes the design process of a high-power white light source, using novel phosphor and colloidal quantum dot materials. To incorporate multiple light emitters, we generalized and extended a down-converting layer model. We employed a phosphor mixture comprising of YAG:Ce and K2TiF 6:Mn4+ powders to illustrate the effectiveness of the model. By incorporating experimental photophysical results from the phosphors and colloidal quantum dots, we modeled our system and chose the design suitable for high-power applications. We report a reduction in the correlated color temperature by 600K for phosphor and quantum dot systems, enabling the creation of a warm white light emission at power densities up to 5 kW/cm 2. Furthermore, at this high-power, their emission achieves the digital cinema initiative (DCI) requirements with a luminescence efficacy improvement up to 32% over the stand-alone ceramic YAG:Ce phosphor.

Economical and green synthesis of bagasse-derived fluorescent carbon dots for biomedical applications.

PubMed

Du, Fengyi; Zhang, Miaomiao; Li, Xiaofeng; Li, Jianan; Jiang, Xinyi; Li, Zhang; Hua, Ye; Shao, Genbao; Jin, Jie; Shao, Qixiang; Zhou, Ming; Gong, Aihua

2014-08-08

Carbon quantum dots (CDs) are promising nanomaterials in biomedical, photocatalytical and photoelectronic applications. However, determining how to explore an ideal precursor for a renewable carbon resource is still an interesting challenge. Here, for the first time, we report that renewable wastes of bagasse as a new precursor were prepared for fluorescent CDs by a hydrothermal carbonization (HTC) process. The characterization results show that such bagasse-derived CDs are monodispersed, contain quasi spherical particles with a diameter of about 1.8 nm and exhibit favorable photoluminescence properties, super-high photostability and good dispersibility in water. Most importantly, bagasse-derived CDs have good biocompatibility and can be easily and quickly internalized by living cancer cells; they can also be used for multicolour biolabeling and bioimaging in cancer cells. It is suggested that bagasse-derived CDs might have potential applications in biomedical and photoelectronic fields.

Facile synthesis of blue-emitting carbon dots@mesoporous silica composite spheres

NASA Astrophysics Data System (ADS)

Guo, Ziying; Zhu, Zhenpeng; Zhang, Xinguo; Chen, Yibo

2018-02-01

This paper reported a facile and effective approach towards high-efficient composite luminophores by embedding blue-emitting N-doped carbon dots into spherical SiO2 matrix (CDs@SiO2). Mesoporous silica microspheres (r-CDs@MSN) with strong luminescence were synthesized by removing CTAB templates in CDs@SiO2 using reflux with acetone. The r-CDs@MSN possess a spherical morphology with smooth surface and a diameter of 130 nm, while it exhibits an excitation-independent blue emission peak at 440 nm with an internal quantum yield of 21.5%. BET result shows that the corresponding surface area and adsorption total pore volume are 156.27 m2/g and 0.682 cm3/g, which is suitable for the drugs loading and release. The results indicate that r-CDs@MSN might act as a potential fluorescent drug carrier.

Colloidal 3-Mercaptopropionic Acid Capped Lead Sulfide Quantum Dots in a Low Boiling Point Solvent.

PubMed

Reinhart, Chase C; Johansson, Erik

2017-04-26

Colloidal 3-mercaptopropionic acid (3-MPA) capped lead sulfide quantum dots were prepared in a variety of organic solvents stabilized with a quaternary ammonium halide salt. The stabilized colloids' optical properties were studied through optical absorption and emission spectroscopy and found to be dependent on both the concentration of a new ligand and stabilizer, and sample age. Nanocrystal ligand chemistry was studied through a combination of 1 H NMR and two-dimensional Nuclear Overhauser Effect Spectroscopy (NOESY) which revealed full displacement of the original oleate ligand to form a dynamically exchanging ligand shell. The colloids were studied optically and via NMR as they aged and revealed a quantitative conversion of monomeric 3-mercaptopropionic acid to its dimer, dithiodipropionic acid (dTdPA).

Performances of some low-cost counter electrode materials in CdS and CdSe quantum dot-sensitized solar cells.

PubMed

Jun, Hieng Kiat; Careem, Mohamed Abdul; Arof, Abdul Kariem

2014-02-10

Different counter electrode (CE) materials based on carbon and Cu2S were prepared for the application in CdS and CdSe quantum dot-sensitized solar cells (QDSSCs). The CEs were prepared using low-cost and facile methods. Platinum was used as the reference CE material to compare the performances of the other materials. While carbon-based materials produced the best solar cell performance in CdS QDSSCs, platinum and Cu2S were superior in CdSe QDSSCs. Different CE materials have different performance in the two types of QDSSCs employed due to the different type of sensitizers and composition of polysulfide electrolytes used. The poor performance of QDSSCs with some CE materials is largely due to the lower photocurrent density and open-circuit voltage. The electrochemical impedance spectroscopy performed on the cells showed that the poor-performing QDSSCs had higher charge-transfer resistances and CPE values at their CE/electrolyte interfaces.

Controlled Growth of CdS Quantum Dot in an Amphiphilic Diblock Copolymer Poly(2-Vinyl Pyridine)-b-Poly(n-Hexyl Isocyanate) Reversed Micelle Nanoreactor.

PubMed

Samal, Monica; Mohapatra, Priya Ranjan; Yun, Kyu Sik

2015-09-01

A diblock copolymer poly(2-vinyl pyridine)-b-poly(n-hexyl isocyanate) (P2VP-b-PHIC) is used for the present study. It has two blocks; a rod-shaped PHIC block that adopts a helical conformation, and a coil shaped P2VP block. In a polar solvent such as THF both PHIC and P2VP blocks are soluble. In mixtures of two solvents, such as THF and methanol, while the solubility of P2VP component is augmented that of PHIC is decreased leading to formation of reversed micelles. The pyridine nitrogen in P2VP block is a reactive site. It forms complexes with a suitable metal ion, such as Cd2+. The micelle is employed as a nanoreactor for synthesis of CdS quantum dot (QD). In this paper, the micellization behaviour of the copolymer and the use of the micelles for synthesis and controlled growth of CdS nanocrystals are demonstrated.

Spin manipulation and spin-lattice interaction in magnetic colloidal quantum dots

NASA Astrophysics Data System (ADS)

Moro, Fabrizio; Turyanska, Lyudmila; Granwehr, Josef; Patanè, Amalia

2014-11-01

We report on the spin-lattice interaction and coherent manipulation of electron spins in Mn-doped colloidal PbS quantum dots (QDs) by electron spin resonance. We show that the phase memory time,TM , is limited by Mn-Mn dipolar interactions, hyperfine interactions of the protons (1H) on the QD capping ligands with Mn ions in their proximity (<1 nm), and surface phonons originating from thermal fluctuations of the capping ligands. In the low Mn concentration limit and at low temperature, we achieve a long phase memory time constant TM˜0.9 μ s , thus enabling the observation of Rabi oscillations. Our findings suggest routes to the rational design of magnetic colloidal QDs with phase memory times exceeding the current limits of relevance for the implementation of QDs as qubits in quantum information processing.

Brightly Luminescent and Color-Tunable Colloidal CH3NH3PbX3 (X = Br, I, Cl) Quantum Dots: Potential Alternatives for Display Technology.

PubMed

Zhang, Feng; Zhong, Haizheng; Chen, Cheng; Wu, Xian-gang; Hu, Xiangmin; Huang, Hailong; Han, Junbo; Zou, Bingsuo; Dong, Yuping

2015-04-28

Organometal halide perovskites are inexpensive materials with desirable characteristics of color-tunable and narrow-band emissions for lighting and display technology, but they suffer from low photoluminescence quantum yields at low excitation fluencies. Here we developed a ligand-assisted reprecipitation strategy to fabricate brightly luminescent and color-tunable colloidal CH3NH3PbX3 (X = Br, I, Cl) quantum dots with absolute quantum yield up to 70% at room temperature and low excitation fluencies. To illustrate the photoluminescence enhancements in these quantum dots, we conducted comprehensive composition and surface characterizations and determined the time- and temperature-dependent photoluminescence spectra. Comparisons between small-sized CH3NH3PbBr3 quantum dots (average diameter 3.3 nm) and corresponding micrometer-sized bulk particles (2-8 μm) suggest that the intense increased photoluminescence quantum yield originates from the increase of exciton binding energy due to size reduction as well as proper chemical passivations of the Br-rich surface. We further demonstrated wide-color gamut white-light-emitting diodes using green emissive CH3NH3PbBr3 quantum dots and red emissive K2SiF6:Mn(4+) as color converters, providing enhanced color quality for display technology. Moreover, colloidal CH3NH3PbX3 quantum dots are expected to exhibit interesting nanoscale excitonic properties and also have other potential applications in lasers, electroluminescence devices, and optical sensors.

Green synthesis of carbon dots originated from Lycii Fructus for effective fluorescent sensing of ferric ion and multicolor cell imaging.

PubMed

Sun, Xiaohan; He, Jiang; Yang, Shenghong; Zheng, Mingda; Wang, Yingying; Ma, Shuang; Zheng, Haipeng

2017-10-01

Green, economical and effective method was developed for synthesis of fluorescent carbon dots (CDs), using one-pot hydrothermal treatment of Lycii Fructus. Optical and structural properties of the CDs have been extensively studied by UV-visible and fluorescence spectroscopic, x-ray diffraction (XRD) techniques, transmission electron microscopy (TEM) and high resolution TEM (HRTEM). Surface functionality and composition of CDs has been illustrated by Fourier transform infrared spectroscopy (FTIR), x-ray photoelectron spectroscopy (XPS) spectra and elemental analysis. The fabricated CDs possess stable fluorescent properties. The fluorescent quantum yield of the CDs can reach 17.2%. The prepared CDs emitted a broad fluorescence between 415 and 545nm and their fluorescence was tuned by changing excitation wavelength. Meanwhile, the fluorescence intensity of the CDs could be significantly quenched by Fe 3+ (turn-off). The CDs exhibit captivating sensitivity and selectivity toward Fe 3+ with a linear range from 0 to 30μM and a detection limit of 21nM. The prepared CDs were successfully applied to the determination of Fe 3+ in the urine samples, the water samples from the from the Yellow River and living HeLa (Henrietta Lacks) cells. Moreover, the low-toxicity and excellent biocompatibility of the CDs were evaluated through MTT assay on HeLa cells. The CDs were also employed as fluorescent probes for multicolor imaging of HeLa cells successfully. Copyright © 2017 Elsevier B.V. All rights reserved.

Biphasic photoelectrochemical sensing strategy based on in situ formation of CdS quantum dots for highly sensitive detection of acetylcholinesterase activity and inhibition.

PubMed

Hou, Ting; Zhang, Lianfang; Sun, Xinzhi; Li, Feng

2016-01-15

Herein, we reported a facile and highly sensitive biphasic photoelectrochemical (PEC) sensing strategy based on enzymatic product-mediated in situ formation of CdS quantum dots (QDs), and assayed the activity and inhibition of acetylcholinesterase (AChE) in its optimal state. Upon the hydrolysis of acetylthiocholine catalyzed by AChE, the product thiocholine stabilizes the in situ formation of CdS QDs in homogenous solution. Due to the electrostatic attraction, the resulting tertiary amino group-functionalized CdS QDs are attached to the surface of the negatively charged indium tin oxide (ITO) electrode, generating significant PEC response upon illumination in the presence of electron donors. By taking full advantage of the in situ formation of CdS QDs in homogenous solution, this strategy is capable of detecting AChE activity and inhibition in its optimal state. A directly measured detection limit of 0.01mU/mL for AChE activity is obtained, which is superior to those obtained by some fluorescence methods. The inhibition of AChE activity by aldicarb is successfully detected, and the corresponding IC50 is determined to be 13μg/L. In addition to high sensitivity and good selectivity, this strategy also exhibits additional advantages of simplicity, low cost and easy operation. To the best of our knowledge, the as-proposed strategy is the first example demonstrating the application of CdS QDs formed in situ for biphasic PEC detection of enzyme activity and inhibition. More significantly, it opens up a new horizon for the development of homogenous PEC sensing platforms, and has great potential in probing many other analytes. Copyright © 2015 Elsevier B.V. All rights reserved.

Excitonic Transitions and Off-resonant Optical Limiting in CdS Quantum Dots Stabilized in a Synthetic Glue Matrix

PubMed Central

2007-01-01

Stable films containing CdS quantum dots of mean size 3.4 nm embedded in a solid host matrix are prepared using a room temperature chemical route of synthesis. CdS/synthetic glue nanocomposites are characterized using high resolution transmission electron microscopy, infrared spectroscopy, differential scanning calorimetry and thermogravimetric analysis. Significant blue shift from the bulk absorption edge is observed in optical absorption as well as photoacoustic spectra indicating strong quantum confinement. The exciton transitions are better resolved in photoacoustic spectroscopy compared to optical absorption spectroscopy. We assign the first four bands observed in photoacoustic spectroscopy to 1se–1sh, 1pe–1ph, 1de–1dhand 2pe–2phtransitions using a non interacting particle model. Nonlinear absorption studies are done using z-scan technique with nanosecond pulses in the off resonant regime. The origin of optical limiting is predominantly two photon absorption mechanism.

A simple route to shape controlled CdS nanoparticles

NASA Astrophysics Data System (ADS)

Nejo, Ayorinde O.; Nejo, Adeola A.; Pullabhotla, Rajasekhar V. S. R.; Revaprasadu, Neerish

2013-02-01

We report the synthesis of CdS nanoparticles in the form of spheres, triangles and wire-like structures. The method involves the reaction of reduced sulfur with a cadmium salt followed by thermolysis in hexadecylamine (HDA). The different shapes were obtained by variation of reaction conditions such as reaction time, temperature and cadmium source. The optical studies show the particles to be quantum confined and luminescent at room temperature.

Mid-IR colloidal quantum dot detectors enhanced by optical nano-antennas

NASA Astrophysics Data System (ADS)

Yifat, Yuval; Ackerman, Matthew; Guyot-Sionnest, Philippe

2017-01-01

We report the fabrication of a colloidal quantum dot based photodetector designed for the 3-5 μm mid infrared wavelength range incorporated with optical nano-antenna arrays to enhance the photocurrent. The fabricated arrays exhibit a resonant behavior dependent on the length of the nano-antenna rods, in good agreement with numerical simulation. The device exhibits a three-fold increase in the spectral photoresponse compared to a photodetector device without antennas, and the resonance is polarized parallel to the antenna orientation. We numerically estimate the device quantum efficiency and investigate its bias dependence.

Composition-Tunable Optical Properties of Zn x Cd(1 - x)S Quantum Dot-Carboxymethylcellulose Conjugates: Towards One-Pot Green Synthesis of Multifunctional Nanoplatforms for Biomedical and Environmental Applications

NASA Astrophysics Data System (ADS)

Mansur, Alexandra A. P.; Mansur, Herman S.; Caires, Anderson J.; Mansur, Rafael L.; Oliveira, Luiz C.

2017-07-01

Quantum dots (QDs) are colloidal semiconductor nanocrystals with unique properties that can be engineered by controlling the nanoparticle size and chemical composition by doping and alloying strategies. However, due to their potential toxicity, augmenting their biocompatibility is yet a challenge for expanding to several biomedical and environmentally friendly applications. Thus, the main goal of this study was to develop composition-tunable and biocompatible Zn x Cd1 - x S QDs using carboxymethylcellulose polysaccharide as direct capping ligand via green colloidal aqueous route at neutral pH and at room temperature for potential biomedical and environmental applications. The ternary alloyed QDs were extensively characterized using UV-vis spectroscopy, photoluminescence spectroscopy (PL), transmission electron microscopy (TEM), X-ray diffraction (XRD), electron energy loss spectroscopy (EELS), and X-ray photoelectrons spectroscopy (XPS). The results indicated that Zn x Cd(1 - x)S QDs were surface stabilized by carboxymethylcellulose biopolymer with spherical morphology for all composition of alloys and narrow sizes distributions ranging from 4 to 5 nm. The XRD results indicated that monophasic ternary alloyed Zn x Cd1 - x S nanocrystals were produced with homogenous composition of the core as evidenced by EELS and XPS analyses. In addition, the absorption and emission optical properties of Zn x Cd1 - x S QDs were red shifted with increasing the amount of Cd2+ in the alloyed nanocrystals, which have also increased the quantum yield compared to pure CdS and ZnS nanoparticles. These properties of alloyed nanomaterials were interpreted based on empirical model of Vegard's law and chemical bond model (CBM). As a proof of concept, these alloyed-QD conjugates were tested for biomedical and environmental applications. The results demonstrated that they were non-toxic and effective fluorophores for bioimaging live HEK293T cells (human embryonic kidney cells) using confocal laser scanning fluorescence microscopy. Moreover, these conjugates presented photocatalytic activity for photodegradation of methylene blue used as model organic industrial pollutant in water. Hence, composition-tunable optical properties of ternary Zn x Cd1 - x S ( x = 0-1) fluorescent alloyed QDs was achieved using a facile eco-friendly aqueous processing route, which can offer promising alternatives for developing innovative nanomaterials for applications in nanomedicine and environmental science and technology.

Structural, optical and photovoltaic properties of P3HT and Mn-doped CdS quantum dots based bulk hetrojunction hybrid layers

NASA Astrophysics Data System (ADS)

Jabeen, Uzma; Adhikari, Tham; Pathak, Dinesh; Shah, Syed Mujtaba; Nunzi, Jean-Michel

2018-04-01

Cadmium sulphide (CdS) and Mn-doped CdS nanocrystals were synthesized by co-precipitation method. The nanocrystals were characterized by Fluorescence, Fourier Transformed Infra-red Spectrometer (FTIR), UV-Visible, X-ray diffraction (XRD), X-ray photoelectron spectrometer (XPS), Field Emission Scanning Electron Microscope (FESEM), and High Resolution Transmission Electron Microscope (HRTEM). A considerable blue shift of absorption band with respect to the cadmium sulphide was observed by the Mn concentration (0.5 M) in the doped sample with decreasing the size of nanocrystals. Other reason for this may be Mn doping. Subsequently the band gap was altered from 2.11 to 2.21 eV due to quantum confinement effect. Scanning electron microscope supplemented with EDAX was operated to find grain size and chemical composition of the synthesized nanomaterials. The PL spectrum of Mn-doped CdS nanocrystals displays three PL bands the first one, within the range of 500 nm and the second band at 537 nm, and the third one around 713 nm is labelled red band emission due to attributed to a 4T1→6A1 transition within the 3d shell of divalent manganese. XRD analysis showed that the material was in cubic crystalline state. A comparative study of surfaces of un-doped and metal doped CdS nanocrystals were investigated using X-ray Photoelectron Spectroscopy (XPS). The synthesized nanomaterial in combination with polymer, poly (3-hexyl thiophene) was operated in the construction of photovoltaic cells. The photovoltaic devices with CdS nanocrystals exhibited power conversion efficiency of 0.34% without annealing and 0.38% with annealing. However, the power conversion efficiency was enhanced by a factor of 0.35 without annealing and 0.42 with annealing with corporation of Mn impurity in CdS lattice. Atomic Force Microscopy was employed for morphology and packing behavior of blend of nanocrystals with organic polymer.

Purcell effect in triangular plasmonic nanopatch antennas with three-layer colloidal quantum dots

NASA Astrophysics Data System (ADS)

Eliseev, S. P.; Kurochkin, N. S.; Vergeles, S. S.; Sychev, V. V.; Chubich, D. A.; Argyrakis, P.; Kolymagin, D. A.; Vitukhnovskii, A. G.

2017-05-01

A model describing a plasmonic nanopatch antenna based on triangular silver nanoprisms and multilayer cadmium chalcogenide quantum dots is introduced. Electromagnetic-field distributions in nanopatch antennas with different orientations of the quantum-dot dipoles are calculated for the first time with the finite element method for numerical electrodynamics simulations. The energy flux through the surface of an emitting quantum dot is calculated for the configurations with the dot in free space, on an aluminum substrate, and in a nanopatch antenna. It is shown that the radiative part of the Purcell factor is as large as 1.7 × 102 The calculated photoluminescence lifetimes of a CdSe/CdS/ZnS colloidal quantum dot in a nanopatch antenna based on a silver nanoprism agree well with the experimental results.

Compact and highly stable quantum dots through optimized aqueous phase transfer

NASA Astrophysics Data System (ADS)

Tamang, Sudarsan; Beaune, Grégory; Poillot, Cathy; De Waard, Michel; Texier-Nogues, Isabelle; Reiss, Peter

2011-03-01

A large number of different approaches for the aqueous phase transfer of quantum dots have been proposed. Surface ligand exchange with small hydrophilic thiols, such as L-cysteine, yields the lowest particle hydrodynamic diameter. However, cysteine is prone to dimer formation, which limits colloidal stability. We demonstrate that precise pH control during aqueous phase transfer dramatically increases the colloidal stability of InP/ZnS quantum dots. Various bifunctional thiols have been applied. The formation of disulfides, strongly diminishing the fluorescence QY has been prevented through addition of appropriate reducing agents. Bright InP/ZnS quantum dots with a hydrodynamic diameter <10 nm and long-term stability have been obtained. Finally we present in vitro studies of the quantum dots functionalized with the cell-penetrating peptide maurocalcine.

Optical and structural properties of ensembles of colloidal Ag{sub 2}S quantum dots in gelatin

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ovchinnikov, O. V., E-mail: Ovchinnikov-O-V@rambler.ru; Smirnov, M. S.; Shapiro, B. I.

2015-03-15

The size dependences of the absorption and luminescence spectra of ensembles of hydrophilic colloidal Ag{sub 2}S quantum dots produced by the sol-gel method and dispersed in gelatin are analyzed. By X-ray diffraction analysis and transmission electron microscopy, the formation of core/shell nanoparticles is detected. The characteristic feature of the nanoparticles is the formation of crystalline cores, 1.5–2.0 nm in dimensions, and shells of gelatin and its complexes with the components of synthesis. The observed slight size dependence of the position of infrared photoluminescence bands (in the range 1000–1400 nm) in the ensembles of hydrophilic colloidal Ag{sub 2}S quantum dots ismore » explained within the context of the model of the radiative recombination of electrons localized at structural and impurity defects with free holes.« less

Atomic layer deposition in nanostructured photovoltaics: tuning optical, electronic and surface properties

NASA Astrophysics Data System (ADS)

Palmstrom, Axel F.; Santra, Pralay K.; Bent, Stacey F.

2015-07-01

Nanostructured materials offer key advantages for third-generation photovoltaics, such as the ability to achieve high optical absorption together with enhanced charge carrier collection using low cost components. However, the extensive interfacial areas in nanostructured photovoltaic devices can cause high recombination rates and a high density of surface electronic states. In this feature article, we provide a brief review of some nanostructured photovoltaic technologies including dye-sensitized, quantum dot sensitized and colloidal quantum dot solar cells. We then introduce the technique of atomic layer deposition (ALD), which is a vapor phase deposition method using a sequence of self-limiting surface reaction steps to grow thin, uniform and conformal films. We discuss how ALD has established itself as a promising tool for addressing different aspects of nanostructured photovoltaics. Examples include the use of ALD to synthesize absorber materials for both quantum dot and plasmonic solar cells, to grow barrier layers for dye and quantum dot sensitized solar cells, and to infiltrate coatings into colloidal quantum dot solar cell to improve charge carrier mobilities as well as stability. We also provide an example of monolayer surface modification in which adsorbed ligand molecules on quantum dots are used to tune the band structure of colloidal quantum dot solar cells for improved charge collection. Finally, we comment on the present challenges and future outlook of the use of ALD for nanostructured photovoltaics.

Flow-injection chemiluminescence analysis for sensitive determination of atenolol using cadmium sulfide quantum dots

NASA Astrophysics Data System (ADS)

Khataee, Alireza; Lotfi, Roya; Hasanzadeh, Aliyeh; Iranifam, Mortaza; Joo, Sang Woo

2016-03-01

A sensitive, rapid and simple flow-injection chemiluminescence (CL) system based on the light emitted from KMnO4-cadmium sulfide quantum dots (CdS QDs) reaction in the presence of cetyltrimethylammonium bromide (CTAB) in acidic medium was developed as a CL probe for the sensitive determination of atenolol. Optical and structural features of CdS QDs capped with L-cysteine, which synthesized via hydrothermal approach, were investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM), photoluminescence (PL), and UV-Vis spectroscopy. The CL intensity of KMnO4-CdS QDs-CTAB was remarkably enhanced in the presence of trace level of atenolol. Under optimum experimental conditions, there is a linear relationship between the increase in CL intensity of KMnO4-CdS QDs-CTAB system and atenolol concentration in a range of 0.001 to 4.0 mg L- 1 and 4.0 to 18.0 mg L- 1, with a detection limit (3σ) of 0.0010 mg L- 1. A possible mechanism for KMnO4-CdS QDs-CTAB-atenolol CL reaction is proposed. To prove the practical application of the KMnO4-CdS QDs-CTAB CL method, the method was applied for the determination of atenolol in spiked environmental water samples and commercial pharmaceutical formulation. Furthermore, corona discharge ionization ion mobility spectrometry (CD-IMS) technique was utilized for determination of atenolol. Figure S2. Optimization of the CL reaction conditions: (a) effect of KMnO4 concentration. Conditions: the concentrations of H2SO4, CdS QDs and atenolol were 1 mol L-1, 0.35 mol L-1, and 4.0 mg L-1, respectively; (b) effect of acidic media. Conditions: the concentrations of KMnO4 was 0.04 mmol L-1, other conditions were as in (a); (c) effect of CdS QDs concentration. Conditions: H2SO4 concentration was 1.0 mol L-1, other conditions were as in (b), and (d) effect of CTAB concentration. Conditions: CdS QDs concentration was 0.35 mmol L-1, other conditions were as in (c). Figure S3. UV-Vis absorption spectra of KMnO4-CdS QDs-atenolol CL system, recorded at different time intervals after their mixing. Conditions: the concentrations of KMnO4, CdS QDs, H2SO4 and atenolol were 0.04 mmol L-1, 0.35 mmol L-1, 1.0 mol L-1 and 4.0 mg L-1, respectively.

Trap elimination and reduction of size dispersion due to aging in CdS x Se1- x quantum dots

NASA Astrophysics Data System (ADS)

Verma, Abhishek; Nagpal, Swati; Pandey, Praveen K.; Bhatnagar, P. K.; Mathur, P. C.

2007-12-01

Quantum Dots of CdS x Se1- x embedded in borosilicate glass matrix have been grown using Double-Step annealing method. Optical characterization of the quantum dots has been done through the combinative analysis of optical absorption and photoluminescence spectroscopy at room temperature. Decreasing trend of photoluminescence intensity with aging has been observed and is attributed to trap elimination. The changes in particle size, size distribution, number of quantum dots, volume fraction, trap related phenomenon and Gibbs free energy of quantum dots, has been explained on the basis of the diffusion-controlled growth process, which continues with passage of time. For a typical case, it was found that after 24 months of aging, the average radii increased from 3.05 to 3.12 nm with the increase in number of quantum dots by 190% and the size-dispersion decreased from 10.8% to 9.9%. For this sample, the initial size range of the quantum dots was 2.85 to 3.18 nm. After that no significant change was found in these parameters for the next 12 months. This shows that the system attains almost a stable nature after 24 months of aging. It was also observed that the size-dispersion in quantum dots reduces with the increase in annealing duration, but at the cost of quantum confinement effect. Therefore, a trade off optimization has to be done between the size-dispersion and the quantum confinement.

Exciton Relaxation and Electron Transfer Dynamics of Semiconductor Quantum Dots

NASA Astrophysics Data System (ADS)

Liu, Cunming

Quantum dots (QDs), also referred to as colloidal semiconductor nanocrystals, exhibit unique electronic and optical properties arising from their three-dimensional confinement and strongly enhanced coulomb interactions. Developing a detailed understanding of the exciton relaxation dynamics within QDs is important not only for sake of exploring the fundamental physics of quantum confinement processes, but also for their applications. Ultrafast transient absorption (TA) spectroscopy, as a powerful tool to explore the relaxation dynamics of excitons, was employed to characterize the hot single/multiexciton relaxation dynamics at the first four exciton states of CdSe/CdZnS QDs. We observed for the first time that the hot hole can relax through two possible pathways: Intraband multiple phonon coupling and intrinsic defect trapping, with a lifetime of ˜7 ps. Additionally, an ultra-short component of ˜ 8 ps, directly associated with the Auger recombination of highly energetic exciton states, was discovered. After exploring the exciton relaxation inside QDs, ultrafast TA spectroscopy was further applied to study the electron transferring outside from QDs. By using a brand-new photocatalytic system consisting of CdSe QDs and Ni-dihydrolipoic acid (Ni-DHLA) catalyst, which has represented a robust photocatalysis of H2 from water, the photoinduced electron transfer (ET) dynamics between QD and the catalyst, one of most important steps during H2 generation, was studied. We found smaller bare CdSe QDs exhibit a better ET performance and CdS shelling on the bare QDs leads to worsen the ET. The calculations of effective mass approximation (EMA) and Marcus theory show the ET process is mainly dominated by driving force, electronic coupling strength and reorganization energy between QD and the catalyst.

Facile synthesis of water-soluble and biocompatible fluorescent nitrogen-doped carbon dots for cell imaging.

PubMed

Wang, Weiping; Lu, Ya-Chun; Huang, Hong; Feng, Jiu-Ju; Chen, Jian-Rong; Wang, Ai-Jun

2014-04-07

A simple, facile and green hydrothermal method was developed in the synthesis of water-soluble nitrogen-doped carbon dots (N-CDs) from streptomycin. The as-prepared N-CDs displayed bright blue fluorescence under the irradiation of UV light, together with a high quantum yield of 7.6% and good biocompatibility as demonstrated by the cell viability assay. Thus, the N-CDs can be used as fluorescent probes for cell imaging, which have potential applications in bioimaging and related fields. This strategy opens a new way for the preparation of fluorescent carbon nanomaterials using small molecules as carbon sources.

Highly fluorescent Zn-doped carbon dots as Fenton reaction-based bio-sensors: an integrative experimental-theoretical consideration.

PubMed

Xu, Quan; Liu, Yao; Su, Rigu; Cai, Lulu; Li, Bofan; Zhang, Yingyuan; Zhang, Linzhou; Wang, Yajun; Wang, Yan; Li, Neng; Gong, Xiao; Gu, Zhipeng; Chen, Yusheng; Tan, Yanglan; Dong, Chenbo; Sreeprasad, Theruvakkattil Sreenivasan

2016-10-20

Heteroatom doped carbon dots (CDs), with high photoluminescence quantum yield (PLQY), are of keen interest in various applications such as chemical sensors, bio-imaging, electronics, and photovoltaics. Zinc, an important element assisting the electron-transfer process and an essential trace element for cells, is a promising metal dopant for CDs, which could potentially lead to multifunctional CDs. In this contribution, we report a single-step, high efficiency, hydrothermal method to synthesize Zn-doped carbon dots (Zn-CDs) with a superior PLQY. The PLQY and luminescence characteristic of Zn-CDs can be tuned by controlling the precursor ratio, and the surface oxidation in the CDs. Though a few studies have reported metal doped CDs with good PLQY, the as prepared Zn-Cds in the present method exhibited a PLQY up to 32.3%. To the best of our knowledge, there is no report regarding the facile preparation of single metal-doped CDs with a QY more than 30%. Another unique attribute of the Zn-CDs is the high monodispersity and the resultant highly robust excitation-independent luminescence that is stable over a broad range of pH values. Spectroscopic investigations indicated that the superior PLQY and luminescence of Zn-CDs are due to the heteroatom directed, oxidized carbon-based surface passivation. Furthermore, we developed a novel and sensitive biosensor for the detection of hydrogen peroxide and glucose leveraging the robust fluorescence properties of Zn-CDs. Under optimal conditions, Zn-CDs demonstrated high sensitivity and response to hydrogen peroxide and glucose over a wide range of concentrations, with a linear range of 10-80 μM and 5-100 μM, respectively, indicating their great potential as a fluorescent probe for chemical sensing.

Rapid solid-phase microwave synthesis of highly photoluminescent nitrogen-doped carbon dots for Fe3+ detection and cellular bioimaging

NASA Astrophysics Data System (ADS)

He, Guili; Xu, Minghan; Shu, Mengjun; Li, Xiaolin; Yang, Zhi; Zhang, Liling; Su, Yanjie; Hu, Nantao; Zhang, Yafei

2016-09-01

Recently, carbon dots (CDs) have been playing an increasingly important role in industrial production and biomedical field because of their excellent properties. As such, finding an efficient method to quickly synthesize a large scale of relatively high purity CDs is of great interest. Herein, a facile and novel microwave method has been applied to prepare nitrogen doped CDs (N-doped CDs) within 8 min using L-glutamic acid as the sole reaction precursor in the solid phase condition. The as-prepared N-doped CDs with an average size of 1.64 nm are well dispersed in aqueous solution. The photoluminescence of N-doped CDs is pH-sensitive and excitation-dependent. The N-doped CDs show a strong blue fluorescence with relatively high fluorescent quantum yield of 41.2%, which remains stable even under high ionic strength. Since the surface is rich in oxygen-containing functional groups, N-doped CDs can be applied to selectively detect Fe3+ with the limit of detection of 10-5 M. In addition, they are also used for cellular bioimaging because of their high fluorescent intensity and nearly zero cytotoxicity. The solid-phase microwave method seems to be an effective strategy to rapidly obtain high quality N-doped CDs and expands their applications in ion detection and cellular bioimaging.

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates.

PubMed

Patty, Kira; Sadeghi, Seyed M; Campbell, Quinn; Hamilton, Nathan; West, Robert G; Mao, Chuanbin

2014-09-21

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates

PubMed Central

Patty, Kira; Sadeghi, Seyed M.; Campbell, Quinn; Hamilton, Nathan; West, Robert G.; Mao, Chuanbin

2014-01-01

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide. PMID:25316953

InAs Colloidal Quantum Dots Synthesis via Aminopnictogen Precursor Chemistry.

PubMed

Grigel, Valeriia; Dupont, Dorian; De Nolf, Kim; Hens, Zeger; Tessier, Mickael D

2016-10-05

Despite their various potential applications, InAs colloidal quantum dots have attracted considerably less attention than more classical II-VI materials because of their complex syntheses that require hazardous precursors. Recently, amino-phosphine has been introduced as a cheap, easy-to-use and efficient phosphorus precursor to synthesize InP quantum dots. Here, we use aminopnictogen precursors to implement a similar approach for synthesizing InAs quantum dots. We develop a two-step method based on the combination of aminoarsine as the arsenic precursor and aminophosphine as the reducing agent. This results in state-of-the-art InAs quantum dots with respect to the size dispersion and band-gap range. Moreover, we present shell coating procedures that lead to the formation of InAs/ZnS(e) core/shell quantum dots that emit in the infrared region. This innovative synthesis approach can greatly facilitate the research on InAs quantum dots and may lead to synthesis protocols for a wide range of III-V quantum dots.

Ag plasmonic nanostructures and a novel gel electrolyte in a high efficiency TiO2/CdS solar cell.

PubMed

Kumar, P Naresh; Deepa, Melepurath; Srivastava, Avanish Kumar

2015-04-21

A novel photoanode architecture with plasmonic silver (Ag) nanostructures embedded in titania (TiO2), which served as the wide band gap semiconducting support and CdS quantum dots (QDs), as light absorbers, is presented. Ag nanostructures were prepared by a polyol method and are comprised of clumps of nanorods, 15-35 nm wide, interspersed with globular nanoparticles and they were characterized by a face centered cubic lattice. Optimization of Ag nanostructures was achieved on the basis of a superior power conversion efficiency (PCE) obtained for the cell with a Ag/TiO2/CdS electrode encompassing a mixed morphology of Ag nano-rods and particles, relative to analogous cells with either Ag nanoparticles or Ag nanorods. Interfacial charge transfer kinetics was unraveled by fluorescence quenching and lifetime studies. Ag nanostructures improve the light harvesting ability of the TiO2/CdS photoanode via (a) plasmonic and scattering effects, which induce both near- and far-field enhancements which translate to higher photocurrent densities and (b) charging effects, whereby, photoexcited electron transfer from TiO2 to Ag is facilitated by Fermi level equilibration. Owing to the spectacular ability of Ag nanostructures to increase light absorption, a greatly increased PCE of 4.27% and a maximum external quantum efficiency of 55% (at 440 nm) was achieved for the cell based on Ag/TiO2/CdS, greater by 42 and 66%, respectively, compared to the TiO2/CdS based cell. In addition, the liquid S(2-) electrolyte was replaced by a S(2-) gel containing fumed silica, and the redox potential, conductivity and p-type conduction of the two were deduced to be comparable. Although the gel based cells showed diminished solar cell performances compared to their liquid counterparts, nonetheless, the Ag/TiO2/CdS electrode continued to outperform the TiO2/CdS electrode. Our studies demonstrate that Ag nanostructures effectively capture a significant chunk of the electromagnetic spectrum and aid QD solar cells in delivering high power conversion efficiencies.

Design of a Hole Trapping Ligand

DOE PAGES

La Croix, Andrew D.; O’Hara, Andrew; Reid, Kemar R.; ...

2017-01-18

A new ligand that covalently attaches to the surface of colloidal CdSe/ CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate$-$bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic$-$organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer frommore » the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV$-$vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Lastly, theoretically predicted red shifts in absorbance were observed experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence« less

Design of a Hole Trapping Ligand

DOE Office of Scientific and Technical Information (OSTI.GOV)

La Croix, Andrew D.; O’Hara, Andrew; Reid, Kemar R.

A new ligand that covalently attaches to the surface of colloidal CdSe/ CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate$-$bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic$-$organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer frommore » the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV$-$vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Lastly, theoretically predicted red shifts in absorbance were observed experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence« less

Preparation of highly luminescent and color tunable carbon nanodots under visible light excitation for in vitro and in vivo bio-imaging

DOE PAGES

Zheng, Min; Li, Jing; Xie, Zhigang; ...

2015-11-10

Carbon nanodots (CDs) have generated enormous excitement because of their superiority in water solubility, chemical inertness, low toxicity, ease of functionalization and resistance to photobleaching. Here we report a facile thermal pyrolysis route to prepare CDs with high quantum yield (QY) using citric acid as the carbon source and ethylene diamine derivatives (EDAs) including triethylenetetramine (TETA), tetraethylenepentamine (TEPA) and polyene polyamine (PEPA) as the passivation agents. We find that the CDs prepared from EDAs, such as TETA, TEPA and PEPA, show relatively high photoluminescence (PL) QY (11.4, 10.6, and 9.8%, respectively) at 1 ex of 465 nm. The cytotoxicity ofmore » the CDs has been investigated through in vitro and in vivo bio-imaging studies. The results indicate that these CDs possess low toxicity and good biocompatibility. As a result, the unique properties such as the high PL QY at large excitation wave length and the low toxicity of the resulting CDs make them promising fluorescent nanoprobes for applications in optical bio-imaging and biosensing.« less

Light-Emitting Diodes Based on Colloidal Silicon Quantum Dots with Octyl and Phenylpropyl Ligands.

PubMed

Liu, Xiangkai; Zhao, Shuangyi; Gu, Wei; Zhang, Yuting; Qiao, Xvsheng; Ni, Zhenyi; Pi, Xiaodong; Yang, Deren

2018-02-14

Colloidal silicon quantum dots (Si QDs) hold ever-growing promise for the development of novel optoelectronic devices such as light-emitting diodes (LEDs). Although it has been proposed that ligands at the surface of colloidal Si QDs may significantly impact the performance of LEDs based on colloidal Si QDs, little systematic work has been carried out to compare the performance of LEDs that are fabricated using colloidal Si QDs with different ligands. Here, colloidal Si QDs with rather short octyl ligands (Octyl-Si QDs) and phenylpropyl ligands (PhPr-Si QDs) are employed for the fabrication of LEDs. It is found that the optical power density of PhPr-Si QD LEDs is larger than that of Octyl-Si QD LEDs. This is due to the fact that the surface of PhPr-Si QDs is more oxidized and less defective than that of Octyl-Si QDs. Moreover, the benzene rings of phenylpropyl ligands significantly enhance the electron transport of QD LEDs. It is interesting that the external quantum efficiency (EQE) of PhPr-Si QD LEDs is lower than that of Octyl-Si QD LEDs because the benzene rings of phenylpropyl ligands suppress the hole transport of QD LEDs. The unbalance between the electron and hole injection in PhPr-Si QD LEDs is more serious than that in Octyl-Si QD LEDs. The currently obtained highest optical power density of ∼0.64 mW/cm 2 from PhPr-Si QD LEDs and highest EQE of ∼6.2% from Octyl-Si QD LEDs should encourage efforts to further advance the development of high-performance optoelectronic devices based on colloidal Si QDs.

Label-free fluorimetric detection of CEA using carbon dots derived from tomato juice.

PubMed

Miao, Hong; Wang, Lan; Zhuo, Yan; Zhou, Zinan; Yang, Xiaoming

2016-12-15

A facile-green strategy to synthesize carbon dots (CDs) with a quantum yield (QY) of nearly 13.9% has been built up, while tomato juice served as the carbon source. Interestingly, not only the precursor of CDs and the whole synthesis procedure were environmental-friendly, but this type of CDs also exhibited multiple advantages including high fluorescent QY, excellent photostability, non-toxicity and satisfactory stability. Significantly, a label-free sensitive assay for detecting carcinoembryonic antigen (CEA) in a continuous and recyclable way has been proposed on the basis of adsorption and desorption of aptamers by the surface of CDs through a competitive mechanism. To be specific, the richness of carboxyl groups of the CDs enabled strong adsorption of ssDNA to the surface of CDs through π-π stacking interactions, resulting in the effective fluorescence quenching by forming CDs-aptamer complexes. The stronger binding affinity between CEA and CEA-aptamer than the π-π stacking interactions has been taken advantage to achieve immediate recovery of the fluorescence of CDs once CEA was introduced. Thereby, quantitative evaluation of CEA concentration in a broad range from 1ngmL(-1) to 0.5ngmL(-1) with the detection limit of 0.3ngmL(-1) was realized in this way. This strategy can be applied in a recyclable way, broadening the sensing application of CDs with biocompatibility. Besides, the CDs were used for cell imaging, potentiating them towards diverse purposes. Copyright © 2016 Elsevier B.V. All rights reserved.

Sideband pump-probe technique resolves nonlinear modulation response of PbS/CdS quantum dots on a silicon nitride waveguide

NASA Astrophysics Data System (ADS)

Kolarczik, Mirco; Ulbrich, Christian; Geiregat, Pieter; Zhu, Yunpeng; Sagar, Laxmi Kishore; Singh, Akshay; Herzog, Bastian; Achtstein, Alexander W.; Li, Xiaoqin; van Thourhout, Dries; Hens, Zeger; Owschimikow, Nina; Woggon, Ulrike

2018-01-01

For possible applications of colloidal nanocrystals in optoelectronics and nanophotonics, it is of high interest to study their response at low excitation intensity with high repetition rates, as switching energies in the pJ/bit to sub-pJ/bit range are targeted. We develop a sensitive pump-probe method to study the carrier dynamics in colloidal PbS/CdS quantum dots deposited on a silicon nitride waveguide after excitation by laser pulses with an average energy of few pJ/pulse. We combine an amplitude modulation of the pump pulse with phase-sensitive heterodyne detection. This approach permits to use co-linearly propagating co-polarized pulses. The method allows resolving transmission changes of the order of 10-5 and phase changes of arcseconds. We find a modulation on a sub-nanosecond time scale caused by Auger processes and biexciton decay in the quantum dots. With ground state lifetimes exceeding 1 μs, these processes become important for possible realizations of opto-electronic switching and modulation based on colloidal quantum dots emitting in the telecommunication wavelength regime.

Single-mode tunable laser emission in the single-exciton regime from colloidal nanocrystals

PubMed Central

Grivas, Christos; Li, Chunyong; Andreakou, Peristera; Wang, Pengfei; Ding, Ming; Brambilla, Gilberto; Manna, Liberato; Lagoudakis, Pavlos

2013-01-01

Whispering-gallery-mode resonators have been extensively used in conjunction with different materials for the development of a variety of photonic devices. Among the latter, hybrid structures, consisting of dielectric microspheres and colloidal core/shell semiconductor nanocrystals as gain media, have attracted interest for the development of microlasers and studies of cavity quantum electrodynamic effects. Here we demonstrate single-exciton, single-mode, spectrally tuned lasing from ensembles of optical antenna-designed, colloidal core/shell CdSe/CdS quantum rods deposited on silica microspheres. We obtain single-exciton emission by capitalizing on the band structure of the specific core/shell architecture that strongly localizes holes in the core, and the two-dimensional quantum confinement of electrons across the elongated shell. This creates a type-II conduction band alignment driven by coulombic repulsion that eliminates non-radiative multi-exciton Auger recombination processes, thereby inducing a large exciton–bi-exciton energy shift. Their ultra-low thresholds and single-mode, single-exciton emission make these hybrid lasers appealing for various applications, including quantum information processing. PMID:23974520

Stimulated emission and lasing from all-inorganic perovskite quantum dots

NASA Astrophysics Data System (ADS)

Sun, Handong; Wang, Yue; Li, Xiaoming; Haibo, Zeng

We present superior optical gain and lasing properties in a new class of emerging quantum materials, the colloidal all-inorganic cesium lead halide perovskite quantum dots (IPQDs) (CsPbX3, X = Cl, Br, I). Our result has indicated that such material system show combined merits of both colloidal quantum dots and halide perovskites. Low-threshold and ultrastable stimulated emission was demonstrated under atmospheric condition. The flexibility and advantageous optical gain properties of these CsPbX3 IPQDs were manifested by demonstration of an optically pumped micro-laser. The nonlinear optical properties including the multi-photon absorption and resultant photoluminescence of the CsPbX3 nanocrystals were investigated. A large two-photon absorption cross-section of up to ~1.2×105 GM is determined from 9 nm-sized CsPbBr3 nanocrystals. Moreover, low-threshold frequency-upconverted stimulated emission by two-photon absorption was observed from the thin films of close-packed CsPbBr3 nanocrystals. We further realize the three-photon pumped stimulated emission in green spectra range from colloidal IPQD.

Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

NASA Astrophysics Data System (ADS)

Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek; Nyk, Marcin

2015-11-01

Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation. The most significant value of two-photon absorption cross section σ2 for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ2Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.

XANES: observation of quantum confinement in the conduction band of colloidal PbS quantum dots

NASA Astrophysics Data System (ADS)

Demchenko, I. N.; Chernyshova, M.; He, X.; Minikayev, R.; Syryanyy, Y.; Derkachova, A.; Derkachov, G.; Stolte, W. C.; Piskorska-Hommel, E.; Reszka, A.; Liang, H.

2013-04-01

The presented investigations aimed at development of inexpensive method for synthesized materials suitable for utilization of solar energy. This important issue was addressed by focusing, mainly, on electronic local structure studies with supporting x-ray diffraction (XRD) and transmission electron microscopy (TEM) analysis of colloidal galena nano-particles (NPs) and quantum dots (QDs) synthesized using wet chemistry under microwave irradiation. Performed x-ray absorption near edge structure (XANES) analysis revealed an evidence of quantum confinement for the sample with QDs, where the bottom of the conduction band was shifted to higher energy. The QDs were found to be passivated with oxides at the surface. Existence of sulfate/sulfite and thiosulfate species in pure PbS and QDs, respectively, was identified.

Determination of carrier lifetime and mobility in colloidal quantum dot films via impedance spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rath, Arup K.; Lasanta, Tania; Bernechea, Maria

2014-02-10

Impedance Spectroscopy (IS) proves to be a powerful tool for the determination of carrier lifetime and majority carrier mobility in colloidal quantum dot films. We employ IS to determine the carrier lifetime in PbS quantum dot Schottky solar cells with Al and we verify the validity of the technique via transient photovoltage. We also present a simple approach based on an RC model that allows the determination of carrier mobility in PbS quantum dot films and we corroborate the results via comparison with space charge limited measurements. In summary, we demonstrate the potential of IS to characterize key-to-photovoltaics optoelectronic properties,more » carrier lifetime, and mobility, in a facile way.« less

Functionalized CdS quantum dots-based luminescence probe for detection of heavy and transition metal ions in aqueous solution.

PubMed

Chen, Jinlong; Zheng, Aifang; Gao, Yingchun; He, Chiyang; Wu, Genhua; Chen, Youcun; Kai, Xiaoming; Zhu, Changqing

2008-03-01

Strong luminescence CdS quantum dots (QDs) have been prepared and modified with l-cysteine by a facile seeds-assistant technique in water. They are water-soluble and highly stable in aqueous solution. CdS QDs evaluated as a luminescence probe for heavy and transition metal (HTM) ions in aqueous solution was systematically studied. Five HTM ions such as silver(I) ion, copper(II) ion, mercury(II) ion, cobalt(II) ion, and nickel(II) ion significantly influence the photophysics of the emission from the functionalized CdS QDs. Experiment results showed that the fluorescence emission from CdS QDs was enhanced significantly by silver ion without any spectral shift, while several other bivalent HTM ions, such as Hg(2+), Cu(2+), Co(2+), and Ni(2+), exhibited effective optical quenching effect on QDs. Moreover, an obvious red-shift of emission band was observed in the quenching of CdS QDs for Hg(2+) and Cu(2+) ions. Under the optimal conditions, the response was linearly proportional to the concentration of Ag(+) ion ranging from 1.25 x 10(-7) to 5.0 x 10(-6)molL(-1) with a detection limit of 2.0 x 10(-8)molL(-1). The concentration dependence of the quenching effect on functionalized QDs for the other four HTM ions could be well described by typical Stern-Volmer equation, with the linear response of CdS QDs emission proportional to the concentration ranging from 1.50 x 10(-8) to 7.50 x 10(-7)molL(-1) for Hg(2+) ion, 3.0 x 10(-7) to 1.0 x 10(-5)molL(-1) for Ni(2+) ion, 4.59 x 10(-8) to 2.295 x 10(-6)molL(-1) for Cu(2+) ion, and 1.20 x 10(-7) to 6.0 x 10(-6)molL(-1) Co(2+) ion, respectively. Based on the distinct optical properties of CdS QDs system with the five HTM ions, and the relatively wide linear range and rapid response to HTM ions, CdS QDs can be developed as a potential identified luminescence probe for familiar HTM ions detection in aqueous solution.

Camphor-mediated synthesis of carbon nanoparticles, graphitic shell encapsulated carbon nanocubes and carbon dots for bioimaging

PubMed Central

Oza, Goldie; Ravichandran, M.; Merupo, Victor-Ishrayelu; Shinde, Sachin; Mewada, Ashmi; Ramirez, Jose Tapia; Velumani, S.; Sharon, Madhuri; Sharon, Maheshwar

2016-01-01

A green method for an efficient synthesis of water-soluble carbon nanoparticles (CNPs), graphitic shell encapsulated carbon nanocubes (CNCs), Carbon dots (CDs) using Camphor (Cinnamomum camphora) is demonstrated. Here, we describe a competent molecular fusion and fission route for step-wise synthesis of CDs. Camphor on acidification and carbonization forms CNPs, which on alkaline hydrolysis form CNCs that are encapsulated by thick graphitic layers and on further reduction by sodium borohydride yielded CDs. Though excitation wavelength dependent photoluminescence is observed in all the three carbon nanostructures, CDs possess enhanced photoluminescent properties due to more defective carbonaceous structures. The surface hydroxyl and carboxyl functional groups make them water soluble in nature. They possess excellent photostability, higher quantum yield, increased absorption, decreased cytotoxicity and hence can be utilized as a proficient bio imaging agent. PMID:26905737

Camphor-mediated synthesis of carbon nanoparticles, graphitic shell encapsulated carbon nanocubes and carbon dots for bioimaging

NASA Astrophysics Data System (ADS)

Oza, Goldie; Ravichandran, M.; Merupo, Victor-Ishrayelu; Shinde, Sachin; Mewada, Ashmi; Ramirez, Jose Tapia; Velumani, S.; Sharon, Madhuri; Sharon, Maheshwar

2016-02-01

A green method for an efficient synthesis of water-soluble carbon nanoparticles (CNPs), graphitic shell encapsulated carbon nanocubes (CNCs), Carbon dots (CDs) using Camphor (Cinnamomum camphora) is demonstrated. Here, we describe a competent molecular fusion and fission route for step-wise synthesis of CDs. Camphor on acidification and carbonization forms CNPs, which on alkaline hydrolysis form CNCs that are encapsulated by thick graphitic layers and on further reduction by sodium borohydride yielded CDs. Though excitation wavelength dependent photoluminescence is observed in all the three carbon nanostructures, CDs possess enhanced photoluminescent properties due to more defective carbonaceous structures. The surface hydroxyl and carboxyl functional groups make them water soluble in nature. They possess excellent photostability, higher quantum yield, increased absorption, decreased cytotoxicity and hence can be utilized as a proficient bio imaging agent.

Femtosecond laser-induced size reduction and emission quantum yield enhancement of colloidal silicon nanocrystals: Effect of laser ablation time.

PubMed

Zhang, Yingxiong; Wu, Wenshun; Hao, Huilian; Shen, Wenzhong

2018-06-19

Colloidal silicon (Si) nanocrystals (NCs) with different sizes were successfully prepared by femtosecond laser ablation under different laser ablation time (LAT). The mean size decreases from 4.23 to 1.42 nm with increasing LAT from 30 to 120 min. In combination with structural characterization, temperature-dependent photoluminescence (PL), time-resolved PL, and PL excitation spectra, we attribute room temperature blue emissions peaked at 405 and 430 nm to the radiative recombination of electron-hole pairs via the oxygen deficient centers related to Si-C-H2 and Si-O-Si bonds of colloidal Si NCs prepared in 1-octene, respectively. In particular, the measured PL quantum yield of colloidal Si NCs has been enhanced significantly from 23.6% to 55.8% with prolonging LAT from 30 to 120 min. © 2018 IOP Publishing Ltd.

Phosphorus, and nitrogen co-doped carbon dots as a fluorescent probe for real-time measurement of reactive oxygen and nitrogen species inside macrophages.

PubMed

Gong, Yunqian; Yu, Bin; Yang, Wen; Zhang, Xiaoling

2016-05-15

Phosphorus and nitrogen doped carbon dots (PN-CDs) were conveniently prepared by carbonization of adenosine-5'-triphosphate using a hydrothermal treatment. The PN-CDs with P/C atomic ratio of ca. 9.2/100 emit blue luminescence with high quantum yields of up to 23.5%. The PN-CDs were used as a novel sensing platform for live cell imaging of reactive oxygen species (ROS) and reactive nitrogen species (RNS), including ClO(-), ONOO(-), and NO in macrophages. The nanosensor design is based on our new finding that the strong fluorescence of the PN-CDs can be sensitively and selectively quenched by ROS and RNS both in vitro and in vivo. These results reveal that the PN-CDs can serve as a sensitive sensor for rapid imaging of ROS and RNS signaling with high selectivity and contrast. Copyright © 2016 Elsevier B.V. All rights reserved.

Fluorescent Carbon Dots Derived from Maillard Reaction Products: Their Properties, Biodistribution, Cytotoxicity, and Antioxidant Activity.

PubMed

Li, Dongmei; Na, Xiaokang; Wang, Haitao; Xie, Yisha; Cong, Shuang; Song, Yukun; Xu, Xianbing; Zhu, Bei-Wei; Tan, Mingqian

2018-02-14

Food-borne nanoparticles have received great attention because of their unique physicochemical properties and potential health risk. In this study, carbon dots (CDs) formed during one of the most important chemical reactions in the food processing field, the Maillard reaction from the model system including glucose and lysine, were investigated. The CDs purified from Maillard reaction products emitted a strong blue fluorescence under ultraviolet light with a fluorescent quantum yield of 16.30%. In addition, they were roughly spherical, with sizes of around 4.3 nm, and mainly composed of carbon, oxygen, hydrogen, and nitrogen. Their surface groups such as hydroxyl, amino, and carboxyl groups were found to possibly enable CDs to scavenge DPPH and hydroxyl radicals. Furthermore, the cytotoxicity assessment of CDs showed that they could readily enter HepG2 cells while causing negligible cell death at low concentration. However, high CDs concentrations were highly cytotoxic and led to cell death via interference of the glycolytic pathway.

Mechanisms of Local Stress Sensing in Multifunctional Polymer Films Using Fluorescent Tetrapod Nanocrystals

DOE PAGES

Raja, Shilpa N.; Zherebetskyy, Danylo; Wu, Siva; ...

2016-07-13

Nanoscale stress-sensing can be used across fields ranging from detection of incipient cracks in structural mechanics to monitoring forces in biological tissues. We demonstrate how tetrapod quantum dots (tQDs) embedded in block copolymers act as sensors of tensile/compressive stress. Remarkably, tQDs can detect their own composite dispersion and mechanical properties with a switch in optomechanical response when tQDs are in direct contact. Using experimental characterizations, atomistic simulations and finite-element analyses, we show that under tensile stress, densely packed tQDs exhibit a photoluminescence peak shifted to higher energies ("blue-shift") due to volumetric compressive stress in their core; loosely packed tQDs exhibitmore » a peak shifted to lower energies ("red-shift") from tensile stress in the core. The stress shifts result from the tQD's unique branched morphology in which the CdS arms act as antennas that amplify the stress in the CdSe core. Our nanocomposites exhibit excellent cyclability and scalability with no degraded properties of the host polymer. Colloidal tQDs allow sensing in many materials to potentially enable autoresponsive, smart structural nanocomposites that self-predict upcoming fracture.« less

High-Efficiency All-Solution-Processed Light-Emitting Diodes Based on Anisotropic Colloidal Heterostructures with Polar Polymer Injecting Layers.

PubMed

Castelli, Andrea; Meinardi, Francesco; Pasini, Mariacecilia; Galeotti, Francesco; Pinchetti, Valerio; Lorenzon, Monica; Manna, Liberato; Moreels, Iwan; Giovanella, Umberto; Brovelli, Sergio

2015-08-12

Colloidal quantum dots (QDs) are emerging as true candidates for light-emitting diodes with ultrasaturated colors. Here, we combine CdSe/CdS dot-in-rod heterostructures and polar/polyelectrolytic conjugated polymers to demonstrate the first example of fully solution-based quantum dot light-emitting diodes (QD-LEDs) incorporating all-organic injection/transport layers with high brightness, very limited roll-off and external quantum efficiency as high as 6.1%, which is 20 times higher than the record QD-LEDs with all-solution-processed organic interlayers and exceeds by over 200% QD-LEDs embedding vacuum-deposited organic molecules.

Direct electrochemical stripping detection of cystic-fibrosis-related DNA linked through cadmium sulfide quantum dots

NASA Astrophysics Data System (ADS)

Marin, Sergio; Merkoçi, Arben

2009-02-01

Electrochemical detection of a cadmium sulfide quantum dots (CdS QDs)-DNA complex connected to paramagnetic microbeads (MB) was performed without the need for chemical dissolving. The method is based on dropping 20 µl of CdS QD-DNA-MB suspension on the surface of a screen-printed electrode. It is followed by magnetic collection on the surface of the working electrode and electrochemical detection using square-wave voltammetry (SWV), giving a well-shaped and sensitive analytical signal. A cystic-fibrosis-related DNA sequence was sandwiched between the two DNA probes. One DNA probe is linked via biotin-streptavidin bonding with MB and the other one via thiol groups with the CdS QD used as tags. Nonspecific signals of DNA were minimized using a blocking agent and the results obtained were successfully employed in a model DNA sensor with an interest in future applications in the clinical field. The developed nanoparticle biosensing system may offer numerous opportunities in other fields where fast, low cost and efficient detection of small volume samples is required.

A genome-wide nanotoxicology screen of Saccharomyces cerevisiae mutants reveals the basis for cadmium sulphide quantum dot tolerance and sensitivity.

PubMed

Marmiroli, M; Pagano, L; Pasquali, F; Zappettini, A; Tosato, V; Bruschi, C V; Marmiroli, N

2016-01-01

The use of cadmium sulphide quantum dots (CdS QDs) is increasing, particularly in the electronics industry. Their size (1-10 nm in diameter) is, however, such that they can be taken up by living cells. Here, a bakers' yeast (Saccharomyces cerevisiae) deletion mutant collection has been exploited to provide a high-throughput means of revealing the genetic basis for tolerance/susceptibility to CdS QD exposure. The deletion of 112 genes, some associated with the abiotic stress response, some with various metabolic processes, some with mitochondrial organization, some with transport and some with DNA repair, reduced the level of tolerance to CdS QDs. A gene ontology analysis highlighted the role of oxidative stress in determining the cellular response. The transformation of sensitive mutants with centromeric plasmids harbouring DNA from a wild type strain restored the wild type growth phenotype when the complemented genes encoded either HSC82, DSK2 or ALD3. The use of these simple eukaryote knock-out mutants for functional toxicogenomic analysis will inform studies focusing on higher organisms.

Enhancement of emission efficiency of colloidal CdSe quantum dots on silicon substrate via an ultra-thin layer of aluminum oxide.

PubMed

Patty, K; Sadeghi, S M; Nejat, A; Mao, C-B

2014-04-18

We demonstrate that an ultra-thin layer of aluminum oxide can significantly enhance the emission efficiency of colloidal quantum dots on a Si substrate. For an ensemble of single quantum dots, our results show that this super brightening process can increase the fluorescence of CdSe quantum dots, forming well-resolved spectra, while in the absence of this layer the emission remains mostly at the noise level. We demonstrate that this process can be further enhanced with irradiation of the quantum dots, suggesting a significant photo-induced fluorescence enhancement via considerable suppression of non-radiative decay channels of the quantum dots. We study the impact of the Al oxide thickness on Si and interdot interactions, and discuss the results in terms of photo-induced catalytic properties of the Al oxide and the effects of such an oxide on the Coulomb blockade responsible for suppression of photo-ionization of the quantum dots.

A customizable class of colloidal-quantum-dot spasers and plasmonic amplifiers

PubMed Central

Kress, Stephan J. P.; Cui, Jian; Rohner, Patrik; Kim, David K.; Antolinez, Felipe V.; Zaininger, Karl-Augustin; Jayanti, Sriharsha V.; Richner, Patrizia; McPeak, Kevin M.; Poulikakos, Dimos; Norris, David J.

2017-01-01

Colloidal quantum dots are robust, efficient, and tunable emitters now used in lighting, displays, and lasers. Consequently, when the spaser—a laser-like source of high-intensity, narrow-band surface plasmons—was first proposed, quantum dots were specified as the ideal plasmonic gain medium for overcoming the significant intrinsic losses of plasmons. Many subsequent spasers, however, have required a single material to simultaneously provide gain and define the plasmonic cavity, a design unable to accommodate quantum dots and other colloidal nanomaterials. In addition, these and other designs have been ill suited for integration with other elements in a larger plasmonic circuit, limiting their use. We develop a more open architecture that decouples the gain medium from the cavity, leading to a versatile class of quantum dot–based spasers that allow controlled generation, extraction, and manipulation of plasmons. We first create aberration-corrected plasmonic cavities with high quality factors at desired locations on an ultrasmooth silver substrate. We then incorporate quantum dots into these cavities via electrohydrodynamic printing or drop-casting. Photoexcitation under ambient conditions generates monochromatic plasmons (0.65-nm linewidth at 630 nm, Q ~ 1000) above threshold. This signal is extracted, directed through an integrated amplifier, and focused at a nearby nanoscale tip, generating intense electromagnetic fields. More generally, our device platform can be straightforwardly deployed at different wavelengths, size scales, and geometries on large-area plasmonic chips for fundamental studies and applications. PMID:28948219

Efficient synthesis of highly fluorescent carbon dots by microreactor method and their application in Fe3+ ion detection.

PubMed

Rao, Longshi; Tang, Yong; Li, Zongtao; Ding, Xinrui; Liang, Guanwei; Lu, Hanguang; Yan, Caiman; Tang, Kairui; Yu, Binhai

2017-12-01

Rapidly obtaining strong photoluminescence (PL) of carbon dots with high stability is crucial in all practical applications of carbon dots, such as cell imaging and biological detection. In this study, we proposed a rapid, continuous carbon dots synthesis technique by using a microreactor method. By taking advantage of the microreactor, we were able to rapidly synthesized CDs at a large scale in less than 5min, and a high quantum yield of 60.1% was achieved. This method is faster and more efficient than most of the previously reported methods. To explore the relationship between the microreactor structure and CDs PL properties, Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) were carried out. The results show the surface functional groups and element contents influence the PL emission. Subsequent ion detection experiments indicated that CDs are very suitable for use as nanoprobes for Fe 3+ ion detection, and the lowest detection limit for Fe 3+ is 0.239μM, which is superior to many other research studies. This rapid and simple synthesis method will not only aid the development of the quantum dots industrialization but also provide a powerful and portable tool for the rapid and continuous online synthesis of quantum dots supporting their application in cell imaging and safety detection. Copyright © 2017 Elsevier B.V. All rights reserved.

Synthesis of N-acetyl-L-cysteine capped Mn:doped CdS quantum dots for quantitative detection of copper ions

NASA Astrophysics Data System (ADS)

Yang, Xiupei; Jia, Zhihui; Cheng, Xiumei; Luo, Na; Choi, Martin M. F.

2018-06-01

In this work, a new assembled copper ions sensor based on the Mn metal-enhanced fluorescence of N-acetyl-L-cysteine protected CdS quantum dots (NAC-Mn:CdS QDs) was developed. The NAC and Mn:CdS QDs nanoparticles were assembled into NAC-Mn:CdS QDs complexes through the formation of Cdsbnd S and Mnsbnd S bonds. As compared to NAC capped CdS QDs, higher fluorescence quantum yields of NAC-Mn:CdS QDs was observed, which is attributed to the surface plasmon resonance of Mn metal. In addition, the fluorescence intensity of as-formed complexes weakened in the presence of copper ions. The decrease in fluorescence intensity presented a linear relationship with copper ions concentration in the range from 0.16-3.36 μM with a detection limit of 0.041 μM . The characterization of as-formed QDs was analyzed by photoluminescence (PL), ultra violet-visible (UV-vis), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and energy dispersive spectroscopy (EDS) respectively. Furthermore, the recoveries and relative standard deviations of Cu2+ spiked in real water samples for the intra-day and inter-day analyses were 88.20-117.90, 95.20-109.90, 0.80-5.80 and 1.20-3.20%, respectively. Such a metal-enhanced QDs fluorescence system may have promising application in chemical and biological sensors.

In situ capping for size control of monochalcogenides (ZnS, CdS, and SnS) nanocrystals produced by anaerobic metal-reducing bacteria

DOE PAGES

Jang, Gyoung Gug; Jacobs, Christopher B.; Ivanov, Ilia N.; ...

2015-07-24

Metal monochalcogenide quantum dot nanocrystals of ZnS, CdS and SnS were prepared by anaerobic, metal-reducing bacteria using in situ capping by oleic acid or oleylamine. Furthermore, the capping agent preferentially adsorbs on the surface of the nanocrystal, suppressing the growth process in the early stages, thus leading to production of nanocrystals with a diameter of less than 5 nm.

Role of ZnO photoanode nanostructures and sensitizer deposition approaches on the photovoltaic properties of CdS/CdSe and CdS1-xSex quantum dot-sensitized solar cells

NASA Astrophysics Data System (ADS)

Şişman, İlkay; Tekir, Oktay; Karaca, Hüseyin

2017-02-01

Hierarchical bundle-like ZnO nanorod arrays (BNRs) were synthesized by a one-pot hydrothermal method based on two consecutive temperature steps for cascade CdS/CdSe and ternary CdS1-xSex alloy quantum dot-sensitized solar cells (QDSSCs) as photoanode. The CdS/CdSe and CdS1-xSex QDs were deposited on the surface of the ZnO BNRs by conventional and modified successive ionic-layer adsorption and reaction (SILAR) methods, respectively. Using the ZnO BNRs/CdS/CdSe photoanode, the power conversion efficiency reaches 2.08%, which is 1.8 times higher than that of pristine ZnO nanorods/CdS/CdSe photoanode, while by applying ZnO BNRs/CdS1-xSex, the power conversion efficiency improves 2.52%. The remarkably improved photovoltaic performance is mainly derived from the bundle-like nanorod arrays structure, which increases the QDs loading amount and the scattering effect for light absorption, and the appropriate conduction band energy, sufficient Se amount and well coverage of the ternary CdS1-xSex QDs result in enhanced photogenerated electron injection, high light absorption and reduced recombination, respectively. As a result, ZnO BNRs/CdS1-xSex combination can significantly improve performance of QDSSCs.

Antimicrobial activity, cytotoxicity and DNA binding studies of carbon dots

NASA Astrophysics Data System (ADS)

Jhonsi, Mariadoss Asha; Ananth, Devanesan Arul; Nambirajan, Gayathri; Sivasudha, Thilagar; Yamini, Rekha; Bera, Soumen; Kathiravan, Arunkumar

2018-05-01

In recent years, quantum dots (QDs) are one of the most promising nanomaterials in life sciences community due to their unexploited potential in biomedical applications; particularly in bio-labeling and sensing. In the advanced nanomaterials, carbon dots (CDs) have shown promise in next generation bioimaging and drug delivery studies. Therefore the knowledge of the exact nature of interaction with biomolecules is of great interest to designing better biosensors. In this study, the interaction between CDs derived from tamarind and calf thymus DNA (ct-DNA) has been studied by vital spectroscopic techniques, which revealed that the CDs could interact with DNA via intercalation. The apparent association constant has been deduced from the absorption spectral changes of ct-DNA-CDs using the Benesi-Hildebrand equation. From the DNA induced emission quenching experiments the apparent DNA binding constant of the CDs (Kapp) have also been evaluated. Furthermore, we have analyzed the antibacterial and antifungal activity of CDs using disc diffusion assay method which exhibited excellent activity against E. coli and C. albicans with inhibition zone in the range of 7-12 mm. The biocompatible nature of CDs was confirmed by an in vitro cytotoxicity test on L6 normal rat myoblast cells by using MTT assay. The cell viability is not affected till the high dosage of CDs (200 μg/mL) for >48 h. As a consequence of the work, future development of CDs for microbial control and DNA sensing among the various biomolecules is possible in view of emerging biofields.

Tricolor White-Light-Emitting Carbon Dots with Multiple-Cores@Shell Structure for WLED Application.

PubMed

Zhang, Tianyi; Zhao, Feifei; Li, Li; Qi, Bin; Zhu, Dongxia; Lü, Jianhua; Lü, Changli

2018-06-13

The past few years have witnessed the rapid development of carbon dots (CDs) due to their outstanding optical properties and a wide range of applications. However, the design and control of CDs with long-wavelength multicolor emission are still huge challenges to be addressed for their practical use in different fields. Here, novel nitrogen-doped multiple-core@shell-structured AC-CDs with tricolor emissions of red, green, and blue were constructed via one-pot hydrothermal method from 5-amino-1,10-phenanthroline and citric acid as reactants and the growth process of AC-CDs was monitored with the reaction time in the synthetic system. The origin of different fluorescence emissions was explored using the unique coordination ability of the surface groups of AC-CDs. An obvious concentration dependence of fluorescent properties was observed for the as-prepared AC-CDs, and a highly fluorescent quantum yield (QY) of 67% for red emission at 630 nm can be obtained by adjusting concentration of AC-CDs. The pure white-light emission (0.33, 0.33; Commission Internationale de l'Elcairage coordinate) was carried out from single carbon dot with QY of 29% through regulation of the excitation and concentration of multiple-core@shell-structured AC-CDs. In addition, because of their excellent photoluminescent properties, the white-emitting AC-CDs as emitting phosphor can be easily used in the fabrication of white-light-emitting diode with good anti-photobleaching and temperature stability.

Turn-off fluorescence sensor for the detection of ferric ion in water using green synthesized N-doped carbon dots and its bio-imaging.

PubMed

Edison, Thomas Nesakumar Jebakumar Immanuel; Atchudan, Raji; Shim, Jae-Jin; Kalimuthu, Senthilkumar; Ahn, Byeong-Cheol; Lee, Yong Rok

2016-05-01

This paper reports turn-off fluorescence sensor for Fe(3+) ion in water using fluorescent N-doped carbon dots as a probe. A simple and efficient hydrothermal carbonization of Prunus avium fruit extract for the synthesis of fluorescent nitrogen-doped carbon dots (N-CDs) is described. This green approach proceeds quickly and provides good quality N-CDs. The mean size of synthesized N-CDs was approximately 7nm calculated from the high-resolution transmission electron microscopic images. X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy revealed the presence of -OH, -NH2, -COOH, and -CO functional groups over the surface of CDs. The N-CDs showed excellent fluorescent properties, and emitted blue fluorescence at 411nm upon excitation at 310nm. The calculated quantum yield of the synthesized N-CDs is 13% against quinine sulfate as a reference fluorophore. The synthesized N-CDs were used as a fluorescent probe towards the selective and sensitive detection of biologically important Fe(3+) ions in water by fluorescence spectroscopy and for bio-imaging of MDA-MB-231 cells. The limit of detection (LOD) and the Stern-Volmer quenching constant for the synthesized N-CDs were 0.96μM and 2.0958×10(3)M of Fe(3+) ions. The green synthesized N-CDs are efficiently used as a promising candidate for the detection of Fe(3+) ions and bio-imaging. Copyright © 2016 Elsevier B.V. All rights reserved.

Influence of wide band gap oxide substrates on the photoelectrochemical properties and structural disorder of CdS nanoparticles grown by the successive ionic layer adsorption and reaction (SILAR) method

PubMed Central

Malashchonak, Mikalai V; Korolik, Olga V; Streltsov, Еugene А; Kulak, Anatoly I

2015-01-01

Summary The photoelectrochemical properties of nanoheterostructures based on the wide band gap oxide substrates (ZnO, TiO2, In2O3) and CdS nanoparticles deposited by the successive ionic layer adsorption and reaction (SILAR) method have been studied as a function of the CdS deposition cycle number (N). The incident photon-to-current conversion efficiency (IPCE) passes through a maximum with the increase of N, which is ascribed to the competition between the increase in optical absorption and photocarrier recombination. The maximal IPCE values for the In2O3/CdS and ZnO/CdS heterostructures are attained at N ≈ 20, whereas for TiO2/CdS, the appropriate N value is an order of magnitude higher. The photocurrent and Raman spectroscopy studies of CdS nanoparticles revealed the occurrence of the quantum confinement effect, demonstrating the most rapid weakening with the increase of N in ZnO/CdS heterostructures. The structural disorder of CdS nanoparticles was characterized by the Urbach energy (E U), spectral width of the CdS longitudinal optical (LO) phonon band and the relative intensity of the surface optical (SO) phonon band in the Raman spectra. Maximal values of E U (100–120 meV) correspond to СdS nanoparticles on a In2O3 surface, correlating with the fact that the CdS LO band spectral width and intensity ratio for the CdS SO and LO bands are maximal for In2O3/CdS films. A notable variation in the degree of disorder of CdS nanoparticles is observed only in the initial stages of CdS growth (several tens of deposition cycles), indicating the preservation of the nanocrystalline state of CdS over a wide range of SILAR cycles. PMID:26734517

Influence of wide band gap oxide substrates on the photoelectrochemical properties and structural disorder of CdS nanoparticles grown by the successive ionic layer adsorption and reaction (SILAR) method.

PubMed

Malashchonak, Mikalai V; Mazanik, Alexander V; Korolik, Olga V; Streltsov, Еugene А; Kulak, Anatoly I

2015-01-01

The photoelectrochemical properties of nanoheterostructures based on the wide band gap oxide substrates (ZnO, TiO2, In2O3) and CdS nanoparticles deposited by the successive ionic layer adsorption and reaction (SILAR) method have been studied as a function of the CdS deposition cycle number (N). The incident photon-to-current conversion efficiency (IPCE) passes through a maximum with the increase of N, which is ascribed to the competition between the increase in optical absorption and photocarrier recombination. The maximal IPCE values for the In2O3/CdS and ZnO/CdS heterostructures are attained at N ≈ 20, whereas for TiO2/CdS, the appropriate N value is an order of magnitude higher. The photocurrent and Raman spectroscopy studies of CdS nanoparticles revealed the occurrence of the quantum confinement effect, demonstrating the most rapid weakening with the increase of N in ZnO/CdS heterostructures. The structural disorder of CdS nanoparticles was characterized by the Urbach energy (E U), spectral width of the CdS longitudinal optical (LO) phonon band and the relative intensity of the surface optical (SO) phonon band in the Raman spectra. Maximal values of E U (100-120 meV) correspond to СdS nanoparticles on a In2O3 surface, correlating with the fact that the CdS LO band spectral width and intensity ratio for the CdS SO and LO bands are maximal for In2O3/CdS films. A notable variation in the degree of disorder of CdS nanoparticles is observed only in the initial stages of CdS growth (several tens of deposition cycles), indicating the preservation of the nanocrystalline state of CdS over a wide range of SILAR cycles.

A Novel Quantum Dots-Based Point of Care Test for Syphilis

NASA Astrophysics Data System (ADS)

Yang, Hao; Li, Ding; He, Rong; Guo, Qin; Wang, Kan; Zhang, Xueqing; Huang, Peng; Cui, Daxiang

2010-05-01

One-step lateral flow test is recommended as the first line screening of syphilis for primary healthcare settings in developing countries. However, it generally shows low sensitivity. We describe here the development of a novel fluorescent POC (Point Of Care) test method to be used for screening for syphilis. The method was designed to combine the rapidness of lateral flow test and sensitiveness of fluorescent method. 50 syphilis-positive specimens and 50 healthy specimens conformed by Treponema pallidum particle agglutination (TPPA) were tested with Quantum Dot-labeled and colloidal gold-labeled lateral flow test strips, respectively. The results showed that both sensitivity and specificity of the quantum dots-based method reached up to 100% (95% confidence interval [CI], 91-100%), while those of the colloidal gold-based method were 82% (95% CI, 68-91%) and 100% (95% CI, 91-100%), respectively. In addition, the naked-eye detection limit of quantum dot-based method could achieve 2 ng/ml of anti-TP47 polyclonal antibodies purified by affinity chromatography with TP47 antigen, which was tenfold higher than that of colloidal gold-based method. In conclusion, the quantum dots were found to be suitable for labels of lateral flow test strip. Its ease of use, sensitiveness and low cost make it well-suited for population-based on-the-site syphilis screening.

Simple and green synthesis of protein-conjugated CdS nanoparticles and spectroscopic study on the interaction between CdS and zein

NASA Astrophysics Data System (ADS)

Qin, Dezhi; Zhang, Li; Du, Xian; Wang, Yabo; Zhang, Qiuxia

2016-09-01

The present study demonstrates the role of zein molecules in synthesizing CdS nanoassemblies through protein-directed, green synthetic approach. Zein molecules can as capping ligand and stabilizing agent to regulate the nucleation and growth of CdS nanocrystals, and the obtained products are organic-inorganic nanocomposites. The analysis of surface charge and conductivity indicates that strong electrostatic force restricts mobility of ions, which creates a local supersaturation surrounding the binding sites of zein and reduces the activated energy of nucleation. The interaction between Cd2+/CdS and zein molecules was systematically investigated through spectroscopy techniques. Fourier transform infrared (FT-IR) spectra were used to envisage the binding of the functional groups of zein with the surface of CdS nanoparticles. Ultraviolet visible (UV-Vis) and photoluminescence (PL) spectra results show that Cd2+/CdS might interact with the aromatic amino acids of protein molecules and change its chemical microenvironment. The quantum-confined effect of nanocrystals is confirmed by optical absorption spectrum due to the small size (3-5 nm) of CdS particles. The data of circular dichroism (CD) spectra indicate that the formation of CdS nanocrystals could lead to the conformational change of zein molecules. Moreover, the possible mechanism of CdS nanocrystals growth in zein solution was also discussed. The weak interactions such as Van der Waals, hydrophobic forces and hydrogen bonds in zein molecules should play a crucial factor in the self-assembly of small nanoparticles.

Optical and structural properties of sputtered CdS films for thin film solar cell applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kim, Donguk; Park, Young; Kim, Minha

2015-09-15

Graphical abstract: Photo current–voltage curves (a) and the quantum efficiency (QE) (b) for the solar cell with CdS film grown at 300 °C. - Highlights: • CdS thin films were grown by a RF magnetron sputtering method. • Influence of growth temperature on the properties of CdS films was investigated. • At higher T{sub g}, the crystallinity of the films improved and the grains enlarged. • CdS/CdTe solar cells with efficiencies of 9.41% were prepared at 300 °C. - Abstract: CdS thin films were prepared by radio frequency magnetron sputtering at various temperatures. The effects of growth temperature on crystallinity,more » surface morphology and optical properties of the films were characterized with X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Raman spectra, UV–visible spectrophotometry, and photoluminescence (PL) spectra. As the growth temperature was increased, the crystallinity of the sputtered CdS films was improved and the grains were enlarged. The characteristics of CdS/CdTe thin film solar cell appeared to be significantly influenced by the growth temperature of the CdS films. Thin film CdS/CdTe solar cells with efficiencies of 9.41% were prepared at a growth temperature of 300 °C.« less

Efficient nanosecond photoluminescence from infrared PbS quantum dots coupled to plasmonic nanoantennas

DOE PAGES

Akselrod, Gleb M.; Weidman, Mark C.; Li, Ying; ...

2016-09-13

Infrared (IR) light sources with high modulation rates are critical components for on-chip optical communications. Lead-based colloidal quantum dots are promising nonepitaxial materials for use in IR light-emitting diodes, but their slow photoluminescence lifetime is a serious limitation. Here we demonstrate coupling of PbS quantum dots to colloidal plasmonic nanoantennas based on film-coupled metal nanocubes, resulting in a dramatic 1300-fold reduction in the emission lifetime from the microsecond to the nanosecond regime. This lifetime reduction is primarily due to a 1100-fold increase in the radiative decay rate owing to the high quantum yield (65%) of the antenna. The short emissionmore » lifetime is accompanied by high antenna quantum efficiency and directionality. Lastly, this nonepitaxial platform points toward GHz frequency, electrically modulated, telecommunication wavelength light-emitting diodes and single-photon sources.« less

Studies of mist deposition for the formation of quantum dot CdSe films

NASA Astrophysics Data System (ADS)

Price, S. C.; Shanmugasundaram, K.; Ramani, S.; Zhu, T.; Zhang, F.; Xu, J.; Mohney, S. E.; Zhang, Q.; Kshirsagar, A.; Ruzyllo, J.

2009-10-01

Films of CdSe(ZnS) colloidal nanocrystalline quantum dots (NQDs) were deposited on bare silicon, glass and polymer coated silicon using mist deposition. This effort is a part of an exploratory investigation in which this deposition technique is studied for the first time as a method to form semiconductor NQD films. The process parameters, including deposition time, solution concentration and electric field, were varied to change the thickness of the deposited film. Blanket films and films deposited through a shadow mask were created to investigate the method's ability to pattern films during the deposition process. The differences between these deposition modes in terms of film morphology were observed. Overall, the results show that mist deposition of quantum dots is a viable method for creating thin, patterned quantum dot films using colloidal solution as the precursor. It is concluded that this technique shows very good promise for quantum dot (light emitting diode, LED) fabrication.

High Performance Photoluminescent Carbon Dots for In Vitro and In Vivo Bioimaging: Effect of Nitrogen Doping Ratios.

PubMed

Wang, Junqing; Zhang, Pengfei; Huang, Chao; Liu, Gang; Leung, Ken Cham-Fai; Wáng, Yì Xiáng J

2015-07-28

Photoluminescent carbon dots (CDs) have received ever-increasing attention in the application of optical bioimaging because of their low toxicity, tunable fluorescent properties, and ultracompact size. We report for the first time on enhanced photoluminescence (PL) performance influenced by structure effects among the various types of nitrogen doped (N-doped) PL CDs. These CDs were facilely synthesized from condensation carbonization of linear polyethylenic amine (PEA) analogues and citric acid (CA) of different ratios. Detailed structural and property studies demonstrated that either the structures or the molar ratio of PEAs altered the PL properties of the CDs. The content of conjugated π-domains with C═N in the carbon backbone was correlated with their PL Quantum Yield (QY) (up to 69%). The hybridization between the surface/molecule state and the carbon backbone synergistically affected the chemical/physical properties. Also, long-chain polyethylenic amine (PEA) molecule-doped CDs exhibit increasing photostability, but at the expense of PL efficiency, proving that the PL emission of high QY CDs arise not only from the sp(2)/sp(3) carbon core and surface passivation of CDs, but also from the molecular fluorophores integrated in the CDs. In vitro and in vivo bioimaging of these N-doped CDs showed strong photoluminescence signals. Good biocompatibility demonstrates their potential feasibility for bioimaging applications. In addition, the overall size profile of the as-prepared CDs is comparable to the average size of capillary pores in normal living tissues (∼5 nm). Our study provides valuable insights into the effects of the PEA doping ratios on photoluminescence efficiency, biocompatibility, cellular uptake, and optical bioimaging of CDs.

ZnO Hierarchical Nanostructure Photoanode in a CdS Quantum Dot-Sensitized Solar Cell

PubMed Central

Liu, Huan; Zhang, Gengmin; Sun, Wentao; Shen, Ziyong; Shi, Mingji

2015-01-01

A hierarchical array of ZnO nanocones covered with ZnO nanospikes was hydrothermally fabricated and employed as the photoanode in a CdS quantum dot-sensitized solar cell (QDSSC). This QDSSC outperformed the QDSSC based on a simple ZnO nanocone photoanode in all the four principal photovoltaic parameters. Using the hierarchical photoanode dramatically increased the short circuit current density and also slightly raised the open circuit voltage and the fill factor. As a result, the conversion efficiency of the QDSSC based on the hierarchical photoanode was more than twice that of the QDSSC based on the simple ZnO nanocone photoanode. This improvement is attributable to both the enlarged specific area of the photoanode and the reduction in the recombination of the photoexcited electrons. PMID:26379268

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patty, Kira; Campbell, Quinn; Hamilton, Nathan

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggestsmore » the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.« less

The use of a microreactor for rapid screening of the reaction conditions and investigation of the photoluminescence mechanism of carbon dots.

PubMed

Lu, Yue; Zhang, Ling; Lin, Hengwei

2014-04-07

A microreactor is applied and reported, for the first time, in the field of research of carbon dots (CDs), including rapid screening of the reaction conditions and investigation of the photoluminescence (PL) mechanism. Various carbonaceous precursors and solvents were selected and hundreds of reaction conditions were screened (ca. 15 min on average per condition). Through analyzing the screened conditions, tunable PL emission maxima, from about 330 to 550 nm with respectable PL quantum yields, were achieved. Moreover, the relationship between different developmental stages of the CDs and the PL properties was explored by using the microreactor. The PL emission was observed to be independent of the composition, carbonization extent, and morphology/size of the CDs. This study unambiguously presents that a microreactor could serve as a promising tool for the research of CDs. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nitrogen doped carbon nanodots as fluorescent probes for selective detection and quantification of Ferric(III) ions

NASA Astrophysics Data System (ADS)

Chin, Suk-Fun; Tan, Shao-Chien; Pang, Suh-Cem; Ng, Sing-Muk

2017-11-01

Nitrogen (N) doped carbon dots (N-CDs) that showed blue fluorescence with quantum yield (QY) of 12.25% were synthesized by one step microwave irradiation of lysine in ortho-phosphoric acid at 1000 W for 5 min. The as-synthesized N-CDs were successfully explored as fluorescent probes for selective detection of ferric (Fe3+) ions in aqueous condition with a linear range from 0.2 to 5.0 mM and a detection limit of 0.074 mM ± 0.081 (S/N = 3). The N-CDs exhibited high selectivity towards the detection of Fe3+ ions even in the presence of interfering ions. The N-CDs also demonstrated the potential of practical application for determining of Fe3+ ions concentration in real samples with high recovery rate and low relative standard deviation error.

Luminescent properties and energy transfer of luminescent carbon dots assembled mesoporous Al(2)O(3): Eu(3) co-doped materials for temperature sensing.

PubMed

He, Youling; He, Jiangling; Zhang, Haoran; Liu, Yingliang; Lei, Bingfu

2017-06-15

Owning to the hydrogen-band interactions, blue-light-emitting luminescent carbon dots (CDs) synthesized by one-pot hydrothermal treatment were successfully assembled into Eu 3+ doped mesoporous aluminas (MAs). Interesting, dual-emissive CDs/MAs co-doped materials with higher quantum yield (QY), long-term stability, mesoporous structure, high thermal stability, and large surface areas were obtained. Furthermore, the obtained CDs/MAs co-doped materials possessed tunable color, and excellent temperature sensitivity due to the existing of energy transfer between CDs and Eu 3+ ion. The energy transfer efficiency (η) and energy transfer probability (P) for CDs/Eu 3+ co-doped materials possessed a monotonous tendency with the change of Eu 3+ content. More importantly, the dual-emissive colors can be regularly adjusted through regulating their excitation wavelength or relative mass ratio. In addition, the emission intensity of the CDs/MAs co-doped materials gradually decreased with increasing temperature showing the clear temperature dependence, this dual-emissive thermometer was with high sensitivity, owning a great fitted curve in the range from 100 to 360K under a single wavelength excitation. Copyright © 2017 Elsevier Inc. All rights reserved.

Toxicological impact of cadmium-based quantum dots towards aquatic biota: Effect of natural sunlight exposure.

PubMed

Silva, B F; Andreani, T; Gavina, A; Vieira, M N; Pereira, C M; Rocha-Santos, T; Pereira, R

2016-07-01

Cadmium-based quantum dots (QDs) are increasingly applied in existent and emerging technologies, especially in biological applications due to their exceptional photophysical and functionalization properties. However, they are very toxic compounds due to the high reactive and toxic cadmium core. The present study aimed to determine the toxicity of three different QDs (CdS 380, CdS 480 and CdSeS/ZnS) before and after the exposure of suspensions to sunlight, in order to assess the effect of environmentally relevant irradiation levels in their toxicity, which will act after their release to the environment. Therefore, a battery of ecotoxicological tests was performed with organisms that cover different functional and trophic levels, such as Vibrio fischeri, Raphidocelis subcapitata, Chlorella vulgaris and Daphnia magna. The results showed that core-shell type QDs showed lower toxic effects to V. fischeri in comparison to core type QDs before sunlight exposure. However, after sunlight exposure, there was a decrease of CdS 380 and CdS 480 QD toxicity to bacterium. Also, after sunlight exposure, an effective decrease of CdSeS/ZnS and CdS 480 toxicity for D. magna and R. subcapitata, and an evident increase in CdS 380 QD toxicity, at least for D. magna, were observed. The results of this study suggest that sunlight exposure has an effect in the aggregation and precipitation reactions of larger QDs, causing the degradation of functional groups and formation of larger bulks which may be less prone to photo-oxidation due to their diminished surface area. The same aggregation behaviour after sunlight exposure was observed for bare QDs. These results further emphasize that the shell of QDs seems to make them less harmful to aquatic biota, both under standard environmental conditions and after the exposure to a relevant abiotic factor like sunlight. Copyright © 2016 Elsevier B.V. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ruberu, T. Purnima A.; Albright, Haley R.; Callis, Brandon

We demonstrate molecular control of nanoscale composition, alloying, and morphology (aspect ratio) in CdS–CdSe nanocrystal dots and rods by modulating the chemical reactivity of phosphine–chalcogenide precursors. Specific molecular precursors studied were sulfides and selenides of triphenylphosphite (TPP), diphenylpropylphosphine (DPP), tributylphosphine (TBP), trioctylphosphine (TOP), and hexaethylphosphorustriamide (HPT). Computational (DFT), NMR (31P and 77Se), and high-temperature crossover studies unambiguously confirm a chemical bonding interaction between phosphorus and chalcogen atoms in all precursors. Phosphine–chalcogenide precursor reactivity increases in the order: TPPE < DPPE < TBPE < TOPE < HPTE (E = S, Se). For a given phosphine, the selenide is always more reactivemore » than the sulfide. CdS1–xSex quantum dots were synthesized via single injection of a R3PS–R3PSe mixture to cadmium oleate at 250 °C. X-ray diffraction (XRD), transmission electron microscopy (TEM), and UV/Vis and PL optical spectroscopy reveal that relative R3PS and R3PSe reactivity dictates CdS1–xSex dot chalcogen content and the extent of radial alloying (alloys vs core/shells). CdS, CdSe, and CdS1–xSex quantum rods were synthesized by injection of a single R3PE (E = S or Se) precursor or a R3PS–R3PSe mixture to cadmium–phosphonate at 320 or 250 °C. XRD and TEM reveal that the length-to-diameter aspect ratio of CdS and CdSe nanorods is inversely proportional to R3PE precursor reactivity. Purposely matching or mismatching R3PS–R3PSe precursor reactivity leads to CdS1–xSex nanorods without or with axial composition gradients, respectively. We expect these observations will lead to scalable and highly predictable “bottom-up” programmed syntheses of finely heterostructured nanomaterials with well-defined architectures and properties that are tailored for precise applications.« less

Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek

Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation.more » The most significant value of two-photon absorption cross section σ{sub 2} for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ{sub 2}Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.« less

The donor-supply electrode enhances performance in colloidal quantum dot solar cells.

PubMed

Maraghechi, Pouya; Labelle, André J; Kirmani, Ahmad R; Lan, Xinzheng; Adachi, Michael M; Thon, Susanna M; Hoogland, Sjoerd; Lee, Anna; Ning, Zhijun; Fischer, Armin; Amassian, Aram; Sargent, Edward H

2013-07-23

Colloidal quantum dot (CQD) solar cells combine solution-processability with quantum-size-effect tunability for low-cost harvesting of the sun's broad visible and infrared spectrum. The highest-performing colloidal quantum dot solar cells have, to date, relied on a depleted-heterojunction architecture in which an n-type transparent metal oxide such as TiO2 induces a depletion region in the p-type CQD solid. These devices have, until now, been limited by a modest depletion region depth produced in the CQD solid owing to limitations in the doping available in TiO2. Herein we report a new device geometry-one based on a donor-supply electrode (DSE)-that leads to record-performing CQD photovoltaic devices. Only by employing this new charge-extracting approach do we deepen the depletion region in the CQD solid and thereby extract notably more photocarriers, the key element in achieving record photocurrent and device performance. With the use of optoelectronic modeling corroborated by experiment, we develop the guidelines for building a superior CQD solar cell based on the DSE concept. We confirm that using a shallow-work-function terminal electrode is essential to producing improved charge extraction and enhanced performance.

Charge Transport between Coupling Colloidal Perovskite Quantum Dots Assisted by Functional Conjugated Ligands.

PubMed

Dai, Jinfei; Xi, Jun; Li, Lu; Zhao, JingFeng; Shi, Yifei; Zhang, Wenwen; Ran, Chenxin; Jiao, Bo; Hou, Xun; Duan, Xinhua; Wu, Zhaoxin

2018-05-14

Long alkyl-chain capping ligands are indispensable for preparing stable colloidal quantum dots. However, its insulating feature blocks efficient carrier transport among QDs, leading to inferior performance in light-emitting diodes (LEDs). The trade-off between conductivity and colloidal stability of QDs has now been overcome. Methylamine lead bromide (MAPbBr 3 ) QDs with a conjugated alkyl-amine, 3-phenyl-2-propen-1-amine (PPA), as ligands were prepared. Owing to electron cloud overlapping and the delocalization effect of conjugated molecules, the conductivity and carrier mobility of PPA-QDs films increased almost 22 times over that of OA-QD films without compromising colloidal stability and photoluminescence. PPA-QDs LEDs exhibit a maximum current efficiency of 9.08 cd A -1 , which is 8 times of that of OA-QDs LEDs (1.14 cd A -1 ). This work provides critical solution for the poor conductivity of QDs in applications of energy-related devices. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Sensitization of photoprocesses in colloidal Ag2S quantum dots by dye molecules

NASA Astrophysics Data System (ADS)

Ovchinnikov, Oleg V.; Kondratenko, Tamara S.; Grevtseva, Irina G.; Smirnov, Mikhail S.; Pokutnyi, Sergey I.

2016-07-01

The effect of photosensitization of IR luminescence excitation (1205 nm) of colloidal Ag2S quantum dots (QDs) with average size of 2.5±0.6 nm in gelatin at 600 to 660 nm by molecules of 3,3'-di-(γ-sulfopropyl)-4,4',5,5'-dibenzo-9-ethylthiacarbocyanine betaine pyridinium salt (Dye1) and thionine dye (Dye2) was registered. Cis-J-aggregates of Dye1 and cations monomer of Dye2 conjugated with Ag2S QDs take part in this process. The photosensitization of luminescence excitation of colloidal Ag2S QDs was interpreted by resonance nonradiation transfer of electronic excitation energy from cis-J-aggregates of Dye1 and cations of Dye2 to centers of recombination luminescence of Ag2S QDs.

Highly luminescent colloidal nanoplates of perovskite cesium lead halide and their oriented assemblies

DOE PAGES

Bekenstein, Yehonadav; Koscher, Brent A.; Eaton, Samuel W.; ...

2015-12-15

Anisotropic colloidal quasi-two-dimensional nanoplates (NPLs) hold great promise as functional materials due to their combination of low dimensional optoelectronic properties and versatility through colloidal synthesis. Recently, lead-halide perovskites have emerged as important optoelectronic materials with excellent efficiencies in photovoltaic and light-emitting applications. Here we report the synthesis of quantum confined all inorganic cesium lead halide nanoplates in the perovskite crystal structure that are also highly luminescent (PLQY 84%). The controllable self-assembly of nanoplates either into stacked columnar phases or crystallographic-oriented thin-sheet structures is demonstrated. Furthermore, the broad accessible emission range, high native quantum yields, and ease of self-assembly make perovskitemore » NPLs an ideal platform for fundamental optoelectronic studies and the investigation of future devices.« less

Photovoltaic properties of multilayered quantum dot/quantum rod-sensitized TiO₂ solar cells fabricated by SILAR and electrophoresis.

PubMed

Cerdán-Pasarán, Andrea; López-Luke, Tzarara; Esparza, Diego; Zarazúa, Isaac; De la Rosa, Elder; Fuentes-Ramírez, Rosalba; Alatorre-Ordaz, Alejandro; Sánchez-Solís, Ana; Torres-Castro, Alejandro; Zhang, Jin Z

2015-07-28

A multilayered semiconductor sensitizer structure composed of three differently sized CdSe quantum rods (QRs), labeled as Q530, Q575, Q590, were prepared and deposited on the surface of mesoporous TiO2 nanoparticles by electrophoretic deposition (EPD) for photovoltaic applications. By varying the arrangement of layers as well as the time of EPD, the photoconversion efficiency was improved from 2.0% with the single layer of CdSe QRs (TiO2/Q590/ZnS) to 2.9% for multilayers (TiO2/Q590Q575/ZnS). The optimal EPD time was shorter for the multilayered structures. The effect of CdS quantum dots (QDs) deposited by successive ionic layer adsorption and reaction (SILAR) was also investigated. The addition of CdS QDs resulted in the enhancement of efficiency to 4.1% for the configuration (TiO2/CdS/Q590Q575/ZnS), due to increased photocurrent and photovoltage. Based on detailed structural, optical, and photoelectrical studies, the increased photocurrent is attributed to broadened light absorption while the increased voltage is due to a shift in the relevant energy levels.

Synergistic doping of fullerene electron transport layer and colloidal quantum dot solids enhances solar cell performance.

PubMed

Yuan, Mingjian; Voznyy, Oleksandr; Zhitomirsky, David; Kanjanaboos, Pongsakorn; Sargent, Edward H

2015-02-04

The spatial location of the predominant source of performance-limiting recombination in today's best colloidal quantum dot (CQD) cells is identified, pinpointing the TiO2:CQD junction; then, a highly n-doped PCBM layer is introduced at the CQD:TiO2 heterointerface. An n-doped PCBM layer is essential to maintain the depletion region and allow for efficient current extraction, thereby producing a record 8.9% in overall power conversion efficiency. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Colloidal quantum dot active layers for light emitting diodes

NASA Astrophysics Data System (ADS)

Pagan, Jennifer G.; Stokes, Edward B.; Patel, Kinnari; Burkhart, Casey C.; Ahrens, Michael T.; Barletta, Philip T.; O'Steen, Mark

2006-07-01

In this paper the preliminary results of incorporating a novel active layer into a GaN light emitting diode (LED) are discussed. Integration of colloidal CdSe quantum dots into a GaN LED active layer is demonstrated. Properties of p-type Mg doped overgrowth GaN are examined via circular transmission line method (CTLM). Effects on surface roughness due to the active layer incorporation are examined using atomic force microscopy (AFM). Electroluminescence of LED test structures is reported, and an ideality factor of n = 1.6 is demonstrated.

Optical characterization of CdS nanoparticles embedded into the comb-type amphiphilic graft copolymer

NASA Astrophysics Data System (ADS)

Kalaycı, Özlem A.; Duygulu, Özgür; Hazer, Baki

2013-01-01

This study refers to the synthesis and characterization of a novel organic/inorganic hybrid nanocomposite material containing cadmium sulfide (CdS) nanoparticles. For this purpose, a series of polypropylene (PP)-g-polyethylene glycol (PEG), PP-g-PEG comb-type amphiphilic graft copolymers were synthesized. PEGs with Mn = 400, 2000, 3350, and 8000 Da were used and the graft copolymers obtained were coded as PPEG400, PPEG2000, PPEG3350, and PPEG8000. CdS nanoparticles were formed in tetrahydrofuran solution of PP-g-PEG amphiphilic comb-type copolymer by the reaction between aqueous solutions of Na2S and Cd(CH3COO)2 simultaneously. Micelle formation of PPEG2000 comb-type amphiphilic graft copolymer in both solvent/non-solvent (petroleum ether-THF) by transmission electron microscopy (TEM). The optical characteristics, size morphology, phase analysis, and dispersion of CdS nanoparticles embedded in PPEG400, PPEG2000, PPEG3350, and PPEG8000 comb-type amphiphilic graft copolymer micelles were determined by high resolution TEM (HRTEM), energy dispersive spectroscopy, UV-vis spectroscopy, and fluorescence emission spectroscopy techniques. The aggregate size of PPEG2000-CdS is between 10 and 50 nm; however, in the case of PPEG400-CdS, PPEG3350-CdS, and PPEG8000-CdS samples, it is up to approximately 100 nm. The size of CdS quantum dots in the aggregates for PPEG2000 and PPEG8000 samples was observed as 5 nm by HRTEM analysis, and this result was also supported by UV-vis absorbance spectra and fluorescence emission spectra.

Semiconductor electrolyte photovoltaic energy converter

NASA Technical Reports Server (NTRS)

Anderson, W. W.; Anderson, L. B.

1975-01-01

Feasibility and practicality of a solar cell consisting of a semiconductor surface in contact with an electrolyte are evaluated. Basic components and processes are detailed for photovoltaic energy conversion at the surface of an n-type semiconductor in contact with an electrolyte which is oxidizing to conduction band electrons. Characteristics of single crystal CdS, GaAs, CdSe, CdTe and thin film CdS in contact with aqueous and methanol based electrolytes are studied and open circuit voltages are measured from Mott-Schottky plots and open circuit photo voltages. Quantum efficiencies for short circuit photo currents of a CdS crystal and a 20 micrometer film are shown together with electrical and photovoltaic properties. Highest photon irradiances are observed with the GaAs cell.

Nitrogen-doped carbon dots originating from unripe peach for fluorescent bioimaging and electrocatalytic oxygen reduction reaction.

PubMed

Atchudan, Raji; Edison, Thomas Nesakumar Jebakumar Immanuel; Lee, Yong Rok

2016-11-15

This paper reports the robust hydrothermal synthesis of nitrogen doped carbon dots (N-CDs) using the unripe fruit of Prunus persica (peach) as the carbon precursor and aqueous ammonia as the nitrogen source. The optical properties of synthesized N-CDs were characterized by ultraviolet visible (UV-Vis) and fluorescence spectroscopy techniques. The synthesized N-CDs were emitted blue light when excitated with a portable UV lamp. The materials with the optical properties were characterized further by high resolution transmission electron microscope (HRTEM), X-ray diffraction (XRD), Raman, Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS). The mean size of the N-CDs was approximately 8nm, as calculated from the HRTEM image. The d-spacing of N-CDs, calculated using Bragg law, was approximately 0.21nm, which was consistent with the interlayer distance calculated from the HRTEM image. FT-IR spectroscopy and XPS revealed the presence of the phytoconstituents functionalities of peach fruit over the N-CDs surface and a high level of nitrogen doping on carbon dots (CDs) was confirmed by XPS studies. These results suggest that the unripe fruit extract of peach is an ideal candidate for the preparation of N-CDs. The resulting N-CDs showed excellent optical properties in water. The synthesized N-CDs exhibited a high fluorescence quantum yield and low cytotoxicity, and can be used as fluorescence imaging probes. In addition, the N-CDs were catalytically activite towards the oxygen reduction reaction (ORR). The N-CDs exhibited good catalytic activity in an alkaline medium (0.1M KOH) with a remarkable ORR of approximately 0.72V vs reversible hydrogen electrode (RHE), and O2 reduction follows mainly a 2 electron pathway by being reduced to hydrogen peroxide. The 2-electron reduction pathway is used in industry for H2O2 production. Copyright © 2016 Elsevier Inc. All rights reserved.

Near-Unity Emitting Copper-Doped Colloidal Semiconductor Quantum Wells for Luminescent Solar Concentrators.

PubMed

Sharma, Manoj; Gungor, Kivanc; Yeltik, Aydan; Olutas, Murat; Guzelturk, Burak; Kelestemur, Yusuf; Erdem, Talha; Delikanli, Savas; McBride, James R; Demir, Hilmi Volkan

2017-08-01

Doping of bulk semiconductors has revealed widespread success in optoelectronic applications. In the past few decades, substantial effort has been engaged for doping at the nanoscale. Recently, doped colloidal quantum dots (CQDs) have been demonstrated to be promising materials for luminescent solar concentrators (LSCs) as they can be engineered for providing highly tunable and Stokes-shifted emission in the solar spectrum. However, existing doped CQDs that are aimed for full solar spectrum LSCs suffer from moderately low quantum efficiency, intrinsically small absorption cross-section, and gradually increasing absorption profiles coinciding with the emission spectrum, which together fundamentally limit their effective usage. Here, the authors show the first account of copper doping into atomically flat colloidal quantum wells (CQWs). In addition to Stokes-shifted and tunable dopant-induced photoluminescence emission, the copper doping into CQWs enables near-unity quantum efficiencies (up to ≈97%), accompanied by substantially high absorption cross-section and inherently step-like absorption profile, compared to those of the doped CQDs. Based on these exceptional properties, the authors have demonstrated by both experimental analysis and numerical modeling that these newly synthesized doped CQWs are excellent candidates for LSCs. These findings may open new directions for deployment of doped CQWs in LSCs for advanced solar light harvesting technologies. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Detection of metronidazole in honey and metronidazole tablets using carbon dots-based sensor via the inner filter effect.

PubMed

Zhao, Jianru; Pan, Xiaohua; Sun, Xiaobo; Pan, Wei; Yu, Guifeng; Wang, Jinping

2018-06-01

In this work, carbon dots (CDs) with a high quantum yield (22.3%) were easily prepared by hydrothermal pyrolysis of acid fuchsin 6B and hydrogen peroxide at 180°C for 10 h. The resultant CDs possess a narrow size distribution in the range of 2.6 to 3.2 nm and emit blue fluorescence. Interestingly, the absorption band of metronidazole (MTZ) centered at 318 nm can complementary overlap with the excitation band of the as-prepared CDs centered at 320 nm, resulting in an inner filter effect (IFE) in high efficiency. In fact, the fluorescence quenching of the CDs depends on the concentration of MTZ. Therefore, a simple method for the detection of MTZ can be established using the CDs-based sensor via the IFE. The linear range of the proposed method was 0-10 μg mL -1 with the limit of detection as low as 0.257 μg mL -1 . This CDs-based sensor had been applied for the detection of MTZ in honey and MTZ tablets with the recoveries in the range of 98.0% to 105.1% and 95.7% to 106.5%, respectively. Therefore, the as-prepared CDs have a potential to be developed as a MTZ sensor with high selectivity, sensitivity and accuracy. Copyright © 2018 John Wiley & Sons, Ltd.

Determination of ethanol using permanganate-CdS quantum dot chemiluminescence system.

PubMed

Abolhasani, Jafar; Hassanzadeh, Javad

2015-08-01

A novel and highly sensitive chemiluminescence (CL) method for the determination of ethanol was developed based on the CdS quantum dots (QDs)-permanganate system. It was found that KMnO4 could directly oxidize CdS QDs in acidic media resulting in relatively high CL emission. A possible mechanism was proposed for this reaction based on UV/Vis absorption, fluorescence and the generated CL emission spectra. However, it was observed that ethanol had a remarkable inhibition effect on this system. This effect was exploited in the determination of ethanol within the concentration range 12-300 µg/L, with detection at 4.3 µg/L. In order to evaluate the capability of presented method, it was satisfactorily utilized in the determination of alcohol in real samples. Copyright © 2014 John Wiley & Sons, Ltd.

Effect of photoanode surface coverage by a sensitizer on the photovoltaic performance of titania based CdS quantum dot sensitized solar cells.

PubMed

Prasad, Rajendra M B; Pathan, Habib M

2016-04-08

In spite of the promising design and architecture, quantum dot sensitized solar cells (QDSSCs) have a long way to go before they attain the actual projected photoconversion efficiencies. Such an inferior performance displayed by QDSSCs is primarily because of many unwanted recombination losses of charge carriers at various interfaces of the cell. Electron recombination due to back electron transfer at the photoanode/electrolyte interface is an important one that needs to be addressed, to improve the efficiency of these third generation nanostructured solar cells. The present work highlights the importance of conformal coverage of CdS quantum dots (QDs) on the surface of the nanocrystalline titania photoanode in arresting such recombinations, leading to improvement in the performance of the cells. Using the successive ionic layer adsorption and reaction (SILAR) process, photoanodes are subjected to different amounts of CdS QD sensitization by varying the number of cycles of deposition. The sensitized electrodes are characterized using UV-visible spectroscopy, cyclic voltammetry and transmission electron microscopy to evaluate the extent of surface coverage of titania electrodes by QDs. Sandwich solar cells are then fabricated using these electrodes and characterized employing electrochemical impedance spectroscopy and J-V characteristics. It is observed that maximum solar cell efficiency is obtained for photoanodes with conformal coating of QDs and any further deposition of sensitizer leads to QD aggregation and so reduces the performance of the solar cells.

CdS quantum dots confined in mesoporous TiO2 with exceptional photocatalytic performance for degradation of organic polutants.

PubMed

Zhou, Panpan; Xie, Yu; Fang, Jing; Ling, Yun; Yu, Changling; Liu, Xiaoming; Dai, Yuhua; Qin, Yuancheng; Zhou, Dan

2017-07-01

In this paper, the mesoporous TiO 2 with different concentration of CdS quantum dots (i.e., x% CdS/TiO 2 ) was successfully fabricated by the sol-gel method. The composition, structure and morphology of the nanocomposites were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), UV-vis diffuse reflectance spectroscopy (UV-Vis/DRS) and nitrogen physical adsorption test and so on. The proportion of CdS and TiO 2 is very important for the photocatalytic performance. As a result, the photocatalytic degradation performance from the most to the least is in the order of 2% CdS/TiO 2 , 4% CdS/TiO 2 , 8% CdS/TiO 2 , pure TiO 2 and 1% CdS/TiO 2 . The photocatalytic (PC) activity of the 2% CdSTiO 2 is characterized by photocatalytic degradation of methyl orange, which can be completely degraded within 45 min better than 60 min TiO 2 takes. It is also much better than CdS. Moreover, other four organic pollutants, such as methylthionine chloride, bisphenol A, rhodamine B, malachite green can also be degraded quickly on the condition of 2% CdS/TiO 2 . What's more, the chemical stability and cycling capability of 2% CdS/TiO 2 are reflected by five cyclic degradation of methyl orange. Copyright © 2017 Elsevier Ltd. All rights reserved.

Exploring Step‐by‐Step Assembly of Nanoparticle:Cytochrome Biohybrid Photoanodes

PubMed Central

Hwang, Ee Taek; Orchard, Katherine L.; Hojo, Daisuke; Beton, Joseph; Lockwood, Colin W. J.; Adschiri, Tadafumi

2017-01-01

Abstract Coupling light‐harvesting semiconducting nanoparticles (NPs) with redox enzymes has been shown to create artificial photosynthetic systems that hold promise for the synthesis of solar fuels. High quantum yields require efficient electron transfer from the nanoparticle to the redox protein, a property that can be difficult to control. Here, we have compared binding and electron transfer between dye‐sensitized TiO2 nanocrystals or CdS quantum dots and two decaheme cytochromes on photoanodes. The effect of NP surface chemistry was assessed by preparing NPs capped with amine or carboxylic acid functionalities. For the TiO2 nanocrystals, binding to the cytochromes was optimal when capped with a carboxylic acid ligand, whereas for the CdS QDs, better adhesion was observed for amine capped ligand shells. When using TiO2 nanocrystals, dye‐sensitized with a phosphonated bipyridine Ru(II) dye, photocurrents are observed that are dependent on the redox state of the decaheme, confirming that electrons are transferred from the TiO2 nanocrystals to the surface via the decaheme conduit. In contrast, when CdS NPs are used, photocurrents are not dependent on the redox state of the decaheme, consistent with a model in which electron transfer from CdS to the photoanode bypasses the decaheme protein. These results illustrate that although the organic shell of NPs nanoparticles crucially affects coupling with proteinaceous material, the coupling can be difficult to predict or engineer. PMID:28920010

"Use of acidophilic bacteria of the genus Acidithiobacillus to biosynthesize CdS fluorescent nanoparticles (quantum dots) with high tolerance to acidic pH".

PubMed

Ulloa, G; Collao, B; Araneda, M; Escobar, B; Álvarez, S; Bravo, D; Pérez-Donoso, J M

2016-12-01

The use of bacterial cells to produce fluorescent semiconductor nanoparticles (quantum dots, QDs) represents a green alternative with promising economic potential. In the present work, we report for the first time the biosynthesis of CdS QDs by acidophilic bacteria of the Acidithiobacillus genus. CdS QDs were obtained by exposing A. ferrooxidans, A. thiooxidans and A. caldus cells to sublethal Cd 2+ concentrations in the presence of cysteine and glutathione. The fluorescence of cadmium-exposed cells moves from green to red with incubation time, a characteristic property of QDs associated with nanocrystals growth. Biosynthesized nanoparticles (NPs) display an absorption peak at 360nm and a broad emission spectra between 450 and 650nm when excited at 370nm, both characteristic of CdS QDs. Average sizes of 6 and 10nm were determined for green and red NPs, respectively. The importance of cysteine and glutathione on QDs biosynthesis in Acidithiobacillus was related with the generation of H 2 S. Interestingly, QDs produced by acidophilic bacteria display high tolerance to acidic pH. Absorbance and fluorescence properties of QDs was not affected at pH 2.0, a condition that totally inhibits the fluorescence of QDs produced chemically or biosynthesized by mesophilic bacteria (stable until pH 4.5-5.0). Results presented here constitute the first report of the generation of QDs with improved properties by using extremophile microorganisms. Copyright © 2016 Elsevier Inc. All rights reserved.

Preparation of SnS2 colloidal quantum dots and their application in organic/inorganic hybrid solar cells

PubMed Central

2011-01-01

Dispersive SnS2 colloidal quantum dots have been synthesized via hot-injection method. Hybrid photovoltaic devices based on blends of a conjugated polymer poly[2-methoxy-5-(3",7"dimethyloctyloxy)-1,4-phenylenevinylene] (MDMO-PPV) as electron donor and crystalline SnS2 quantum dots as electron acceptor have been studied. Photoluminescence measurement has been performed to study the surfactant effect on the excitons splitting process. The photocurrent of solar cells with the hybrid depends greatly on the ligands exchange as well as the device heat treatment. AFM characterization has demonstrated morphology changes happening upon surfactant replacement and annealing, which can explain the performance variation of hybrid solar cells. PMID:21711811

Ultrasound-assisted fabrication of nanoporous CdS films.

PubMed

Singh, R S; Sanagapalli, S; Jayaraman, V; Singh, V P

2004-01-01

A new method for fabricating nanoporous CdS films is reported. It involves exposing the CdS solution with ultrasound waves during the process of dip coating. Indium tin oxide (ITO)-coated glass and plastic (commercial transparency) were used as substrates. In each case three different precursors were used for dip coating. The precursors used were CdCl2 and thiourea in one case and CdS nanoparticles prepared by sonochemical and microwave-assisted methods in the other two cases. X-ray diffraction studies performed on these powders show a phase corresponding to cubic CdS. The Field Emission Scanning Electron Microscopy (FE-SEM) images of the films on plastic showed uniform pores with a diameter of 80 nm for all three methods. Optical absorption measurements indicated a blue shift and multiple peaks in the absorption curve. The FE-SEM observations of the films on an ITO/glass substrate indicated a crystalline film with voids. The UV-vis absorption results indicated a blue shift in the absorption with an absorption edge at 435, 380, and 365 nm for CdS films made by solution growth, sonochemical, and microwave routes, respectively. The magnitude of the absorption is dependent on film thickness, and the observed blue shift in the absorption can be explained on the basis of quantum confinement effects.

Carbon dots-based fluorescent probe for "off-on" sensing of Hg(II) and I⁻.

PubMed

He, Jiangling; Zhang, Haoran; Zou, Jinliang; Liu, Yingliang; Zhuang, Jianle; Xiao, Yong; Lei, Bingfu

2016-05-15

Herein, we report a simple, one-step reflux method for synthesis of photoluminescent carbon dots (CDs) using citric acid as the carbon source and diethylenetriamine (DETA) as the surface passivation reagent along with a high quantum yield (82.40%), the fluorescence intensity of the CDs was found to be effectively quenched by Hg(II) ions. Upon addition of I(-) to the CDs/Hg(II) complex dispersion, the fluorescence intensity of the CDs was significantly recovered. Furthermore, we developed an "off-on" fluorescence assay for the detection of I(-) using CDs/Hg(II) as a fluorescence probe. This probe enables the selective detection of Hg(II) with a linear range of 0-80 μM and a limit of detection is 0.201 µM and a limit of detection about I(-) is 0.234 µM with a linear range of 0-70 μM. Most importantly, the sensors can be successfully applied to the determination of Hg(II) and I(-) in real lake water and urine of cattles, the "off-on" sensor demonstrates high selectivity, repeatability, stability, which offer this CDs-based "off-on" fluorescent sensor a promising platform for environmental and biological sensing applications. Copyright © 2015 Elsevier B.V. All rights reserved.

High charge-carrier mobility enables exploitation of carrier multiplication in quantum-dot films

PubMed Central

Sandeep, C. S. Suchand; Cate, Sybren ten; Schins, Juleon M.; Savenije, Tom J.; Liu, Yao; Law, Matt; Kinge, Sachin; Houtepen, Arjan J.; Siebbeles, Laurens D. A.

2013-01-01

Carrier multiplication, the generation of multiple electron–hole pairs by a single photon, is of great interest for solar cells as it may enhance their photocurrent. This process has been shown to occur efficiently in colloidal quantum dots, however, harvesting of the generated multiple charges has proved difficult. Here we show that by tuning the charge-carrier mobility in quantum-dot films, carrier multiplication can be optimized and may show an efficiency as high as in colloidal dispersion. Our results are explained quantitatively by the competition between dissociation of multiple electron–hole pairs and Auger recombination. Above a mobility of ~1 cm2 V−1 s−1, all charges escape Auger recombination and are quantitatively converted to free charges, offering the prospect of cheap quantum-dot solar cells with efficiencies in excess of the Shockley–Queisser limit. In addition, we show that the threshold energy for carrier multiplication is reduced to twice the band gap of the quantum dots. PMID:23974282

Lead Selenide Colloidal Quantum Dot Solar Cells Achieving High Open-Circuit Voltage with One-Step Deposition Strategy.

PubMed

Zhang, Yaohong; Wu, Guohua; Ding, Chao; Liu, Feng; Yao, Yingfang; Zhou, Yong; Wu, Congping; Nakazawa, Naoki; Huang, Qingxun; Toyoda, Taro; Wang, Ruixiang; Hayase, Shuzi; Zou, Zhigang; Shen, Qing

2018-06-18

Lead selenide (PbSe) colloidal quantum dots (CQDs) are considered to be a strong candidate for high-efficiency colloidal quantum dot solar cells (CQDSCs) due to its efficient multiple exciton generation. However, currently, even the best PbSe CQDSCs can only display open-circuit voltage ( V oc ) about 0.530 V. Here, we introduce a solution-phase ligand exchange method to prepare PbI 2 -capped PbSe (PbSe-PbI 2 ) CQD inks, and for the first time, the absorber layer of PbSe CQDSCs was deposited in one step by using this PbSe-PbI 2 CQD inks. One-step-deposited PbSe CQDs absorber layer exhibits fast charge transfer rate, reduced energy funneling, and low trap assisted recombination. The champion large-area (active area is 0.35 cm 2 ) PbSe CQDSCs fabricated with one-step PbSe CQDs achieve a power conversion efficiency (PCE) of 6.0% and a V oc of 0.616 V, which is the highest V oc among PbSe CQDSCs reported to date.

Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

NASA Astrophysics Data System (ADS)

Shi, Wenqin; Eijt, Stephan W. H.; Suchand Sandeep, C. S.; Siebbeles, Laurens D. A.; Houtepen, Arjan J.; Kinge, Sachin; Brück, Ekkes; Barbiellini, Bernardo; Bansil, Arun

2016-02-01

Positron Two Dimensional Angular Correlation of Annihilation Radiation (2D-ACAR) measurements reveal modifications of the electronic structure and composition at the surfaces of PbSe quantum dots (QDs), deposited as thin films, produced by various ligands containing either oxygen or nitrogen atoms. In particular, the 2D-ACAR measurements on thin films of colloidal PbSe QDs capped with oleic acid ligands yield an increased intensity in the electron momentum density (EMD) at high momenta compared to PbSe quantum dots capped with oleylamine. Moreover, the EMD of PbSe QDs is strongly affected by the small ethylenediamine ligands, since these molecules lead to small distances between QDs and favor neck formation between near neighbor QDs, inducing electronic coupling between neighboring QDs. The high sensitivity to the presence of oxygen atoms at the surface can be also exploited to monitor the surface oxidation of PbSe QDs upon exposure to air. Our study clearly demonstrates that positron annihilation spectroscopy applied to thin films can probe surface transformations of colloidal semiconductor QDs embedded in functional layers.

Nanoscale science and engineering forum (706c) design of solid lipid particles with iron oxide quantum dots for the delivery of therapeutic agents

USDA-ARS?s Scientific Manuscript database

Solid lipid particles provide a method to encapsulate and control the release of drugs in vivo but lack the imaging capability provided by CdS quantum dots. This shortcoming was addressed by combining these two technologies into a model system that uses iron oxide as a non-toxic imaging component in...

Photoluminescence response of colloidal quantum dots on VO2 film across metal to insulator transition

PubMed Central

2014-01-01

We have proposed a method to probe metal to insulator transition in VO2 measuring photoluminescence response of colloidal quantum dots deposited on the VO2 film. In addition to linear luminescence intensity decrease with temperature that is well known for quantum dots, temperature ranges with enhanced photoluminescence changes have been found during phase transition in the oxide. Corresponding temperature derived from luminescence dependence on temperature closely correlates with that from resistance measurement during heating. The supporting reflectance data point out that photoluminescence response mimics a reflectance change in VO2 across metal to insulator transition. Time-resolved photoluminescence study did not reveal any significant change of luminescence lifetime of deposited quantum dots under metal to insulator transition. It is a strong argument in favor of the proposed explanation based on the reflectance data. PACS 71.30. + h; 73.21.La; 78.47.jd PMID:25404877

Near-unity quantum yields from chloride treated CdTe colloidal quantum dots

DOE PAGES

Page, Robert C.; Espinobarro-Velazquez, Daniel; Leontiadou, Marina A.; ...

2014-10-27

Colloidal quantum dots (CQDs) are promising materials for novel light sources and solar energy conversion. However, trap states associated with the CQD surface can produce non-radiative charge recombination that significantly reduces device performance. Here a facile post-synthetic treatment of CdTe CQDs is demonstrated that uses chloride ions to achieve near-complete suppression of surface trapping, resulting in an increase of photoluminescence (PL) quantum yield (QY) from ca. 5% to up to 97.2 ± 2.5%. The effect of the treatment is characterised by absorption and PL spectroscopy, PL decay, scanning transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. We find thismore » process also dramatically improves the air-stability of the CQDs: before treatment the PL is largely quenched after 1 hour of air-exposure, whilst the treated samples showed a PL QY of nearly 50% after more than 12 hours.« less

Bright and multicolor luminescent colloidal Si nanocrystals prepared by pulsed laser irradiation in liquid

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nakamura, Toshihiro, E-mail: nakamura@el.gunma-u.ac.jp; Watanabe, Kanta; Adachi, Sadao

2016-01-11

We reported the preparation of bright and multicolor luminescent colloidal Si nanocrystal (Si-nc) by pulsed UV laser irradiation to porous Si (PSi) in an organic solvent. The different-luminescence-color (different-sized) colloidal Si-nc was produced by the pulsed laser-induced fragmentation of different-sized porous nanostructures. The colloidal Si-nc samples were found to have higher photoluminescence quantum efficiencies (20%–23%) than the PSi samples (1%–3%). The brighter emission of the colloidal Si-nc was attributed to an enhanced radiative band-to-band transition rate due to the presence of a surface organic layer formed by UV laser-induced hydrosilylation.

Size-dependent optical properties of colloidal PbS quantum dots.

PubMed

Moreels, Iwan; Lambert, Karel; Smeets, Dries; De Muynck, David; Nollet, Tom; Martins, José C; Vanhaecke, Frank; Vantomme, André; Delerue, Christophe; Allan, Guy; Hens, Zeger

2009-10-27

We quantitatively investigate the size-dependent optical properties of colloidal PbS nanocrystals or quantum dots (Qdots), by combining the Qdot absorbance spectra with detailed elemental analysis of the Qdot suspensions. At high energies, the molar extinction coefficient epsilon increases with the Qdot volume d(3) and agrees with theoretical calculations using the Maxwell-Garnett effective medium theory and bulk values for the Qdot dielectric function. This demonstrates that quantum confinement has no influence on epsilon in this spectral range, and it provides an accurate method to calculate the Qdot concentration. Around the band gap, epsilon only increases with d(1.3), and values are comparable to the epsilon of PbSe Qdots. The data are related to the oscillator strength f(if) of the band gap transition and results agree well with theoretical tight-binding calculations, predicting a linear dependence of f(if) on d. For both PbS and PbSe Qdots, the exciton lifetime tau is calculated from f(if). We find values ranging between 1 and 3 mus, in agreement with experimental literature data from time-resolved luminescence spectroscopy. Our results provide a thorough general framework to calculate and understand the optical properties of suspended colloidal quantum dots. Most importantly, it highlights the significance of the local field factor in these systems.

A circular dichroism sensor for selective detection of Cd2 + and S2 - based on the in-situ generation of chiral CdS quantum dots

NASA Astrophysics Data System (ADS)

Sianglam, Pradthana; Kulchat, Sirinan; Tuntulani, Thawatchai; Ngeontae, Wittaya

2017-08-01

We demonstrate an advance in the fabrication of circular dichroism (CD) sensors for detection of Cd2 + and S2 - based on chiral CdS quantum dots (QDs) generated by a facile in-situ reaction. The chiral quantum dots are generated in solutions composed of Cd2 +, S2 -, cysteamine (CA) and L-penicillamine (L-PA), with the number of the generated particles limited by either the Cd2 + or S2 - concentration. We show that the magnitude of the CD signal produced by the QDs is linearly related to the initial concentration of Cd2 + and S2 -, with excellent selectivity over other ions. Our sensor functions over concentration ranges of 65-200 μM and 7-125 μM with detection limits of 59.7 and 1.6 μM for Cd2 + and S2 -, respectively. The sensor is applied in real water samples with results comparing favorably with those obtained from ICP-OES (for Cd2 +) and HPLC (for S2 -).

Synthetic Control of Exciton Behavior in Colloidal Quantum Dots.

PubMed

Pu, Chaodan; Qin, Haiyan; Gao, Yuan; Zhou, Jianhai; Wang, Peng; Peng, Xiaogang

2017-03-08

Colloidal quantum dots are promising optical and optoelectronic materials for various applications, whose performance is dominated by their excited-state properties. This article illustrates synthetic control of their excited states. Description of the excited states of quantum-dot emitters can be centered around exciton. We shall discuss that, different from conventional molecular emitters, ground-state structures of quantum dots are not necessarily correlated with their excited states. Synthetic control of exciton behavior heavily relies on convenient and affordable monitoring tools. For synthetic development of ideal optical and optoelectronic emitters, the key process is decay of band-edge excitons, which renders transient photoluminescence as important monitoring tool. On the basis of extensive synthetic developments in the past 20-30 years, synthetic control of exciton behavior implies surface engineering of quantum dots, including surface cation/anion stoichiometry, organic ligands, inorganic epitaxial shells, etc. For phosphors based on quantum dots doped with transition metal ions, concentration and location of the dopant ions within a nanocrystal lattice are found to be as important as control of the surface states in order to obtain bright dopant emission with monoexponential yet tunable photoluminescence decay dynamics.

A new hydrothermal refluxing route to strong fluorescent carbon dots and its application as fluorescent imaging agent.

PubMed

Zhang, Ye-Yun; Wu, Ming; Wang, Yan-Qin; He, Xi-Wen; Li, Wen-You; Feng, Xi-Zeng

2013-12-15

Due to their unique optical and biochemical properties, the water-soluble fluorescent carbon dots (CDs) have attracted a lot of attention recently. Here, strong fluorescent carbon dots with excellent quality have been synthesized by the hydrothermal refluxing method using lactose as carbon source and tris(hydroxymethyl) aminomethane (i.e. Tris) as surface passivation reagent. This facile approach was simple, efficient, economical, green without pollution, and allows large-scale production of CDs without any post-treatment. TEM measurements showed that the resulting particles exhibited an average diameter of 1.5 nm. The obtained CDs possess small particle sizes, good stability in a wide range of pH values (pH 3.5-9.5), high tolerance of salt concentration, strong resistibility to photobleaching, and a fluorescent quantum yield up to 12.5%. The CDs were applied to optical bioimaging of HeLa cells, showing low cytotoxicity and excellent biocompatibility. © 2013 Elsevier B.V. All rights reserved.

Invoking Direct Exciton-Plasmon Interactions by Catalytic Ag Deposition on Au Nanoparticles: Photoelectrochemical Bioanalysis with High Efficiency.

PubMed

Ma, Zheng-Yuan; Xu, Fei; Qin, Yu; Zhao, Wei-Wei; Xu, Jing-Juan; Chen, Hong-Yuan

2016-04-19

In this work, direct exciton-plasmon interactions (EPI) between CdS quantum dots (QDs) and Ag nanoparticles (NPs) were invoked ingeniously by catalytic Ag deposition on Au NPs for the stimulation of high efficient damping effect toward the excitonic responses in CdS QDs, on the basis of which a novel photoelectrochemical (PEC) bioanalytical format was achieved for sensitive microRNA detection. Specifically, upon the configurational change from the hairpin probe DNA to the "Y"-shaped ternary conjugate consisting of the original probe DNA, assistant DNA, and the target microRNA, the alkaline phosphatase (ALP) catalytic chemistry would then trigger the transition of the interparticle interplay from the CdS QDs-Au NPs to the CdS QDs-Ag NPs systems for the microRNA detection due to the dependence of the photocurrent quenching on the target concentration. This work not only provided a unique method for EPI generation among the PEC nanosystems but also offered a versatile and general protocol for future PEC bioanalysis development.

Modeling and studying of white light emitting diodes based on CdS/ZnS spherical quantum dots

NASA Astrophysics Data System (ADS)

Hasanirokh, K.; Asgari, A.

2018-07-01

In this paper, we propose a quantum dot (QD) based white light emitting diode (WLED) structure to study theoretically the material gain and quantum efficiency of the system. We consider the spherical QDs with a II-VI semiconductor core (CdS) that covered with a wider band gap semiconductor acting as a shell (ZnS). In order to generate white light spectrum, we use layers with different dot size that can emit blue, green and red colors. The blue emission originating from CdS core combines to green/orange components originating from ZnS shell and creates an efficiency white light emission. To model this device, at first, we solve Schrödinger and Poisson equations self consistently and obtain eigen energies and wave functions. Then, we calculate the optical gain and internal quantum efficiency (IQE) of a CdS/ZnS LED sample. We investigate the structural parameter effects on the optical properties of the WLED. The numerical results show that the gain profile and IQE curves depend strongly on the structural parameters such as dot size, carrier density and volume scaling parameter. The gain profile becomes higher and wider with increasing the core radius while it becomes less and narrower with increasing the shell thickness. Furthermore, it is found that the volume scaling parameter can manage the system quantum efficiency.

Effect of CdS Growth Time on the Optical Properties of One-Pot Preparation of CdS-Ag2S Binary Compounds

NASA Astrophysics Data System (ADS)

Karimipour, M.; Izadian, L.; Molaei, M.

2018-02-01

CdS-Ag2S binary nanoparticles were synthesized using a facile one-pot microwave irradiation method. The effect of initial nucleation of CdS quantum dots (QDs) using 3 min, 5 min, and 7 min of microwave irradiation on the optical properties of the final compound was studied. The composition and crystal structure of the compounds were verified using energy dispersive x-ray spectroscopy and x-ray diffraction. They revealed that existence of Ag and Cd elements with an atomic ratio of 0.19 crystalizes in the form of monoclinic Ag2S and hexagonal CdS. Scanning electron microscope images showed a spherical morphology of the resultant compound, and transmission electron microscope images showed the formation of fine particles of CdS-Ag2S composites with an average size of 5-7 nm and 10-14 nm for CdS and Ag2S, respectively. Photoluminescence spectroscopy revealed that the initial growth time of CdS has a crucial effect on the emission of binary compounds such that for 3 min and 5 min of irradiation of CdS solution, the binary compound obtains strong red and considerable near-IR emission (850 nm), but for longer time, it rapidly quenches. The results indicate that the strong red emission can be tuned from 600 nm up to 700 nm with prolonging nucleation time of CdS. This study also emphasized that the origin of red emission strongly depends on the size and defects created in the CdS QDs.

Facilitated preparation of bioconjugatable zwitterionic quantum dots using dual-lipid encapsulation.

PubMed

Shrake, Robert; Demillo, Violeta G; Ahmadiantehrani, Mojtaba; Zhu, Xiaoshan; Publicover, Nelson G; Hunter, Kenneth W

2015-01-01

Zwitterionic quantum dots prepared through incorporated zwitterionic ligands on quantum dot surfaces, are being paid significant attention in biomedical applications because of their excellent colloidal stability across a wide pH and ionic strength range, antifouling surface, good biocompatibility, etc. In this work, we report a dual-lipid encapsulation approach to prepare bioconjugatable zwitterionic quantum dots using amidosulfobetaine-16 lipids, dipalmitoyl-sn-glycero-3-phosphoethanolamine lipids with functional head groups, and CuInS2/ZnS quantum dots in a tetrahydrofuran/methanol/water solvent system with sonication. Amidosulfobetaine-16 is a zwitterionic lipid and dipalmitoyl-sn-glycero-3-phosphoethanolamine, with its functional head, provides bioconjugation capability. Under sonication, tetrahydrofuran/methanol containing amidosulfobetaine-16, dipalmitoyl-sn-glycero-3-phosphoethanolamine, and hydrophobic quantum dots are dispersed in water to form droplets. Highly water-soluble tetrahydrofuran/methanol in droplets is further displaced by water, which induces the lipid self-assembling on hydrophobic surface of quantum dots and thus forms water soluble zwitterionic quantum dots. The prepared zwitterionic quantum dots maintain colloidal stability in aqueous solutions with high salinity and over a wide pH range. They are also able to be conjugated with biomolecules for bioassay with minimal nonspecific binding. Copyright © 2014 Elsevier Inc. All rights reserved.

Fabrication of quantum dot/silica core-shell particles immobilizing Au nanoparticles and their dual imaging functions

NASA Astrophysics Data System (ADS)

Kobayashi, Yoshio; Matsudo, Hiromu; Li, Ting-ting; Shibuya, Kyosuke; Kubota, Yohsuke; Oikawa, Takahiro; Nakagawa, Tomohiko; Gonda, Kohsuke

2016-03-01

The present work proposes preparation methods for quantum dot/silica (QD/SiO2) core-shell particles that immobilize Au nanoparticles (QD/SiO2/Au). A colloid solution of QD/SiO2 core-shell particles with an average size of 47.0 ± 6.1 nm was prepared by a sol-gel reaction of tetraethyl orthosilicate in the presence of the QDs with an average size of 10.3 ± 2.1 nm. A colloid solution of Au nanoparticles with an average size of 17.9 ± 1.3 nm was prepared by reducing Au3+ ions with sodium citrate in water at 80 °C. Introduction of amino groups to QD/SiO2 particle surfaces was performed using (3-aminopropyl)-triethoxysilane (QD/SiO2-NH2). The QD/SiO2/Au particles were fabricated by mixing the Au particle colloid solution and the QD/SiO2-NH2 particle colloid solution. Values of radiant efficiency and computed tomography for the QD/SiO2/Au particle colloid solution were 2.23 × 107 (p/s/cm2/sr)/(μW/cm2) at a QD concentration of 8 × 10-7 M and 1180 ± 314 Hounsfield units and an Au concentration of 5.4 × 10-2 M. The QD/SiO2/Au particle colloid solution was injected into a mouse chest wall. Fluorescence emitted from the colloid solution could be detected on the skin covering the chest wall. The colloid solution could also be X-ray-imaged in the chest wall. Consequently, the QD/SiO2/Au particle colloid solution was found to have dual functions, i.e., fluorescence emission and X-ray absorption in vivo, which makes the colloid solution suitable to function as a contrast agent for dual imaging processes.

A flow injection chemiluminescence method for determination of nalidixic acid based on KMnO4-morin sensitized with CdS quantum dots

NASA Astrophysics Data System (ADS)

Khataee, Alireza; Lotfi, Roya; Hasanzadeh, Aliyeh; Iranifam, Mortaza; Joo, Sang Woo

2016-02-01

A simple and sensitive flow injection chemiluminescence (CL) method was developed for determination of nalidixic acid by application of CdS quantum dots (QDs) in KMnO4-morin CL system in acidic medium. Optical and structural features of L-cysteine capped CdS quantum dots which were synthesized via hydrothermal approach were investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM), photoluminescence (PL), and ultraviolet-visible (UV-Vis) spectroscopy. Moreover, the potential mechanism of the proposed CL method was described using the results of the kinetic curves of CL systems, the spectra of CL, PL and UV-Vis analyses. The CL intensity of the KMnO4-morin-CdS QDs system was considerably increased in the presence of nalidixic acid. Under the optimum condition, the enhanced CL intensity was linearly proportional to the concentration of nalidixic acid in the range of 0.0013 to 21.0 mg L- 1, with a detection limit of (3σ) 0.003 mg L- 1. Also, the proposed CL method was utilized for determination of nalidixic acid in environmental water samples, and commercial pharmaceutical formulation to approve its applicability. Furthermore, corona discharge ionization ion mobility spectrometry (CD-IMS) method was utilized for determination of nalidixic acid and the results of real sample analysis by two proposed methods were compared. Comparison the analytical features of these methods represented that the proposed CL method is preferable to CD-IMS method for determination of nalidixic acid due to its high sensitivity and precision.

A flow injection chemiluminescence method for determination of nalidixic acid based on KMnO₄-morin sensitized with CdS quantum dots.

PubMed

Khataee, Alireza; Lotfi, Roya; Hasanzadeh, Aliyeh; Iranifam, Mortaza; Joo, Sang Woo

2016-02-05

A simple and sensitive flow injection chemiluminescence (CL) method was developed for determination of nalidixic acid by application of CdS quantum dots (QDs) in KMnO4-morin CL system in acidic medium. Optical and structural features of L-cysteine capped CdS quantum dots which were synthesized via hydrothermal approach were investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM), photoluminescence (PL), and ultraviolet-visible (UV-Vis) spectroscopy. Moreover, the potential mechanism of the proposed CL method was described using the results of the kinetic curves of CL systems, the spectra of CL, PL and UV-Vis analyses. The CL intensity of the KMnO4-morin-CdS QDs system was considerably increased in the presence of nalidixic acid. Under the optimum condition, the enhanced CL intensity was linearly proportional to the concentration of nalidixic acid in the range of 0.0013 to 21.0 mg L(-1), with a detection limit of (3σ) 0.003 mg L(-1). Also, the proposed CL method was utilized for determination of nalidixic acid in environmental water samples, and commercial pharmaceutical formulation to approve its applicability. Furthermore, corona discharge ionization ion mobility spectrometry (CD-IMS) method was utilized for determination of nalidixic acid and the results of real sample analysis by two proposed methods were compared. Comparison the analytical features of these methods represented that the proposed CL method is preferable to CD-IMS method for determination of nalidixic acid due to its high sensitivity and precision. Copyright © 2015 Elsevier B.V. All rights reserved.

Thick-shell nanocrystal quantum dots

DOEpatents

Hollingsworth, Jennifer A [Los Alamos, NM; Chen, Yongfen [Eugene, OR; Klimov, Victor I [Los Alamos, NM; Htoon, Han [Los Alamos, NM; Vela, Javier [Los Alamos, NM

2011-05-03

Colloidal nanocrystal quantum dots comprising an inner core having an average diameter of at least 1.5 nm and an outer shell, where said outer shell comprises multiple monolayers, wherein at least 30% of the quantum dots have an on-time fraction of 0.80 or greater under continuous excitation conditions for a period of time of at least 10 minutes.

A simple and sensitive flow injection method based on the catalytic activity of CdS quantum dots in an acidic permanganate chemiluminescence system for determination of formaldehyde in water and wastewater.

PubMed

Khataee, Alireza; Lotfi, Roya; Hasanzadeh, Aliyeh; Iranifam, Mortaza

2016-04-01

A simple and sensitive flow injection chemiluminescence (CL) method in which CdS quantum dots (QDs) enhanced the CL intensity of a KMnO4-formaldehyde (HCHO) reaction was offered for the determination of HCHO. This CL system was based on the catalytic activity of CdS QDs and their participation in the CL resonance energy transfer (CRET) phenomenon. A possible mechanism for the supplied CL system was proposed using the kinetic curves of the CL systems and the spectra of CL, photoluminescence (PL) and ultraviolet-visible (UV-Vis). The emanated CL intensity of the KMnO4-CdS QDs system was amplified in the presence of a trace level of HCHO. Based on this enhancement effect, a simple and sensitive flow injection CL method was suggested for the determination of HCHO concentration in environmental water and wastewater samples. Under selected optimized experimental conditions, the increased CL intensity was proportional to the HCHO concentration in the range of 0.03-4.5 μg L(-1) and 4.5-10.0 μg L(-1). The detection limits (3σ) were 0.0003 μg L(-1) and 1.2 μg L(-1). The relative standard deviations (RSD%) for eleven replicate determinations of 4.0 μg L(-1) HCHO were 2.2%. Furthermore, the feasibility of the developed method was investigated via the determination of HCHO concentration in environmental water and wastewater samples.

The initial pump-probe polarization anisotropy of colloidal PbS quantum dots

DOE PAGES

Park, Samuel; Baranov, Dmitry; Ryu, Jisu; ...

2016-07-20

Pump-probe polarization anisotropy measurements with 15 fs pulses are employed to investigate the electronic structure of PbS quantum dots. Here, the initial anisotropy at the bandgap is anomalously low (<0.1) and suggests large electronic couplings.

A novel "dual-potential" electrochemiluminescence aptasensor array using CdS quantum dots and luminol-gold nanoparticles as labels for simultaneous detection of malachite green and chloramphenicol.

PubMed

Feng, Xiaobin; Gan, Ning; Zhang, Huairong; Yan, Qing; Li, Tianhua; Cao, Yuting; Hu, Futao; Yu, Hongwei; Jiang, Qianli

2015-12-15

A novel type of "dual-potential" electrochemiluminescence (ECL) aptasensor array was fabricated on a homemade screen-printed carbon electrode (SPCE) for simultaneous detection of malachite green (MG) and chloramphenicol (CAP) in one single assay. The SPCE substrate consisted of a common Ag/AgCl reference electrode, carbon counter electrode and two carbon working electrodes (WE1 and WE2). In the system, CdS quantum dots (QDs) were modified on WE1 as cathode ECL emitters and luminol-gold nanoparticles (L-Au NPs) were modified on WE2 as anode ECL emitters. Then the MG aptamer complementary strand (MG cDNA) and CAP aptamer complementary strand (CAP cDNA) were attached on CdS QDs and L-Au NPs, respectively. The cDNA would hybridize with corresponding aptamer that was respectively tagged with cyanine dye (Cy5) (as quenchers of CdS QDs) and chlorogenic acid (CA) (as quenchers of l-Au NPs) using poly(ethylenimine) (PEI) as a bridging agent. PEI could lead to a large number of quenchers on the aptamer, which increased the quenching efficiency. Upon MG and CAP adding, the targets could induce strand release due to the highly affinity of analytes toward aptamers. Meanwhile, it could release the Cy5 and CA, which recovered cathode ECL of CdS QDs and anode ECL of L-Au NPs simultaneously. This "dual-potential" ECL strategy could be used to detect MG and CAP with the linear ranges of 0.1-100 nM and 0.2-150 nM, with detection limits of 0.03 nM and 0.07 nM (at 3sB), respectively. More importantly, this designed method was successfully applied to determine MG and CAP in real fish samples and held great potential in the food analysis. Copyright © 2015 Elsevier B.V. All rights reserved.

Engineering surface states of carbon dots to achieve controllable luminescence for solid-luminescent composites and sensitive Be2+ detection

PubMed Central

Li, Xiaoming; Zhang, Shengli; Kulinich, Sergei A.; Liu, Yanli; Zeng, Haibo

2014-01-01

Luminescent carbon dots (L-CDs) with high quantum yield value (44.7%) and controllable emission wavelengths were prepared via a facile hydrothermal method. Importantly, the surface states of the materials could be engineered so that their photoluminescence was either excitation-dependent or distinctly independent. This was achieved by changing the density of amino-groups on the L-CD surface. The above materials were successfully used to prepare multicolor L-CDs/polymer composites, which exhibited blue, green, and even white luminescence. In addition, the excellent excitation-independent luminescence of L-CDs prepared at low temperature was tested for detecting various metal ions. As an example, the detection limit of toxic Be2+ ions, tested for the first time, was as low as 23 μM.

Coupling of Excitons and Discrete Acoustic Phonons in Vibrationally Isolated Quantum Emitters.

PubMed

Werschler, Florian; Hinz, Christopher; Froning, Florian; Gumbsheimer, Pascal; Haase, Johannes; Negele, Carla; de Roo, Tjaard; Mecking, Stefan; Leitenstorfer, Alfred; Seletskiy, Denis V

2016-09-14

The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.

The effect of temperature and dot size on the spectral properties of colloidal InP/ZnS core-shell quantum dots.

PubMed

Narayanaswamy, Arun; Feiner, L F; Meijerink, A; van der Zaag, P J

2009-09-22

Visual color changes between 300 and 510 K were observed in the photoluminescence (PL) of colloidal InP/ZnS core-shell nanocrystals. A subsequent study of PL spectra in the range 2-510 K and fitting the temperature dependent line shift and line width to theoretical models show that the dominant (dephasing) interaction is due to scattering by acoustic phonons of about 23 meV. Low temperature photoluminescence excitation measurements show that the excitonic band gap depends approximately inversely linearly on the quantum dot size d, which is distinctly weaker than the dependence predicted by current theories.

Improved performance of colloidal CdSe quantum dot-sensitized solar cells by hybrid passivation.

PubMed

Huang, Jing; Xu, Bo; Yuan, Chunze; Chen, Hong; Sun, Junliang; Sun, Licheng; Agren, Hans

2014-11-12

A hybrid passivation strategy is employed to modify the surface of colloidal CdSe quantum dots (QDs) for quantum dot-sensitized solar cells (QDSCs), by using mercaptopropionic acid (MPA) and iodide anions through a ligand exchange reaction in solution. This is found to be an effective way to improve the performance of QDSCs based on colloidal QDs. The results show that MPA can increase the coverage of the QDs on TiO2 electrodes and facilitate the hole extraction from the photoxidized QDs, and simultaneously, that the iodide anions can remedy the surface defects of the CdSe QDs and thus reduce the recombination loss in the device. This hybrid passivation treatment leads to a significant enhancement of the power conversion efficiency of the QDSCs by 41%. Furthermore, an optimal ratio of iodide ions to MPA was determined for favorable hybrid passivation; results show that excessive iodine anions are detrimental to the loading of the QDs. This study demonstrates that the improvement in QDSC performance can be realized by using a combination of different functional ligands to passivate the QDs, and that ligand exchange in solution can be an effective approach to introduce different ligands.

Aggregation-induced emission in lamellar solids of colloidal perovskite quantum wells

PubMed Central

Jagielski, Jakub; Kumar, Sudhir; Wang, Mingchao; Scullion, Declan; Lawrence, Robert; Li, Yen-Ting; Yakunin, Sergii; Tian, Tian; Kovalenko, Maksym V.; Chiu, Yu-Cheng; Santos, Elton J. G.; Lin, Shangchao; Shih, Chih-Jen

2017-01-01

The outstanding excitonic properties, including photoluminescence quantum yield (ηPL), of individual, quantum-confined semiconductor nanoparticles are often significantly quenched upon aggregation, representing the main obstacle toward scalable photonic devices. We report aggregation-induced emission phenomena in lamellar solids containing layer-controlled colloidal quantum wells (QWs) of hybrid organic-inorganic lead bromide perovskites, resulting in anomalously high solid-state ηPL of up to 94%. Upon forming the QW solids, we observe an inverse correlation between exciton lifetime and ηPL, distinct from that in typical quantum dot solid systems. Our multiscale theoretical analysis reveals that, in a lamellar solid, the collective motion of the surface organic cations is more restricted to orient along the [100] direction, thereby inducing a more direct bandgap that facilitates radiative recombination. Using the QW solids, we demonstrate ultrapure green emission by completely downconverting a blue gallium nitride light-emitting diode at room temperature, with a luminous efficacy higher than 90 lumen W−1 at 5000 cd m−2, which has never been reached in any nanomaterial assemblies by far. PMID:29282451

Luminescent nanocomposites of conducting polymers and in-situ grown CdS quantum dots

NASA Astrophysics Data System (ADS)

Borriello, C.; Masala, S.; Bizzarro, V.; Nenna, G.; Re, M.; Pesce, E.; Minarini, C.; Di Luccio, T.

2010-06-01

Luminescent PVK:CdS and P3HT:CdS nanocomposites with enhanced electrooptical properties have been synthesized. The nucleation and growth of CdS nanoparticles have been obtained by the thermolysis of a single Cd and S precursor dispersed in the polymers. The size distribution and morphology of the nanoparticles have been studied by TEM analyses. Monodispersive and very small nanoparticles of diameter below 3 nm in PVK and 2 nm in P3HT, have been obtained. The application of such nanocomposites as emitting layers in OLED devices is discussed.

Luminescent nanocomposites of conducting polymers and in-situ grown CdS quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borriello, C.; Masala, S.; Nenna, G.

2010-06-02

Luminescent PVK:CdS and P3HT:CdS nanocomposites with enhanced electrooptical properties have been synthesized. The nucleation and growth of CdS nanoparticles have been obtained by the thermolysis of a single Cd and S precursor dispersed in the polymers. The size distribution and morphology of the nanoparticles have been studied by TEM analyses. Monodispersive and very small nanoparticles of diameter below 3 nm in PVK and 2 nm in P3HT, have been obtained. The application of such nanocomposites as emitting layers in OLED devices is discussed.

Modeling photovoltaic performance in periodic patterned colloidal quantum dot solar cells.

PubMed

Fu, Yulan; Dinku, Abay G; Hara, Yukihiro; Miller, Christopher W; Vrouwenvelder, Kristina T; Lopez, Rene

2015-07-27

Colloidal quantum dot (CQD) solar cells have attracted tremendous attention mostly due to their wide absorption spectrum window and potentially low processability cost. The ultimate efficiency of CQD solar cells is highly limited by their high trap state density. Here we show that the overall device power conversion efficiency could be improved by employing photonic structures that enhance both charge generation and collection efficiencies. By employing a two-dimensional numerical model, we have calculated the characteristics of patterned CQD solar cells based of a simple grating structure. Our calculation predicts a power conversion efficiency as high as 11.2%, with a short circuit current density of 35.2 mA/cm2, a value nearly 1.5 times larger than the conventional flat design, showing the great potential value of patterned quantum dot solar cells.

Growth of MPS-capped ZnS quantum dots in self-assembled thin films: Influence of heat treatment

NASA Astrophysics Data System (ADS)

Koç, Kenan; Tepehan, Fatma Zehra; Tepehan, Galip Gültekin

2015-12-01

The colloidal ZnS quantum dots (QDs) were prepared using 3-mercaptopropyltrimethoxysilane (MPS) molecules. Sol-gel spin coating method was used to deposit the colloidal nanoparticles on a glass substrate. Several features of the MPS were made use to produce self assembled thin films of ZnS quantum dots in a SiO2 network. Produced films were heat treated in between 225 °C and 325 °C to investigate their growth kinetics. The result showed that their size changed approximately from 3 nm to 4 nm and the first excitation peak position changed from 4.6 eV to 4.1 eV in this temperature interval. The activation energy of the nanoparticles for the Ostwald ripening process was found to be 59 kJ/mol.

Synthesis and characterization of surface-modified colloidal CdTe Quantum Dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rajh, T.; Micic, O.I.; Nozik, A.J.

1993-11-18

The controlled synthesis of quantized colloidal CdTe nanocrystals (in aqueous solutions) with narrow size distributions and stabilized against rapid oxidation was achieved by capping the quantum dot particles with 3-mercapto-1,2-propanediol. Nanocrystals (i.e., quantum dots) with mean diameters of 20, 25, 35, and 40 A were produced. Optical absorption spectra showed strong excitonic peaks at the smallest size; the absorption coefficient was shown to follow an inverse cube dependence on particle diameter, while the extinction coefficient per particle remained constant. The quantum yield for photoluminescence increased with decreasing particle size and reached 20% at 20 A. The valence band edges ofmore » the CdTe quantum dots were determined by pulse radiolysis experiments (hole injection from oxidizing radicals); the bandgaps were estimated from pulse radiolysis data (redox potentials of hole and electron injecting radicals) and from the optical spectra. The dependence of the CdTe bandgap on quantum dot size was found to be much weaker than predicted by the effective mass approximation; this result is consistent with recently published theoretical calculations by several groups. 36 refs., 5 figs., 1 tab.« less

An ultrasensitive and selective method for the determination of Ceftriaxone using cysteine capped cadmium sulfide fluorescence quenched quantum dots as fluorescence probes

NASA Astrophysics Data System (ADS)

Samadi, Naser; Narimani, Saeedeh

2016-06-01

In this paper, L-cysteine (Cys) coated CdS quantum dots (QDs) have been prepared, which have excellent water-solubility and are highly stable in aqueous solution. These QDs is proposed as sensitizers for the determination of Ceftriaxone. The quantum dot nanoparticles were structurally and optically characterized by Ultra Violet-Visible absorption Spectroscopy (UV-vis absorption spectroscopy), Fourier transform infrared spectroscopy (FT-IR spectra) and photoluminescence (PL) emission spectroscopy. High resolution transmission electron microscopy (HRTEM) confirms that the Cys-CdS QDs have a spherical structure with good crystallinity. Therefore, a new simple and selective PL analysis system was developed for the determination of Ceftriaxone (CFX). Under the optimum conditions, The response of L-Cys capped CdS QDs as the probe was linearly proportional to the concentration of Ceftriaxone ions in the range of 1.6 × 10- 9-1.1 × 10- 3 M with a correlation coefficient (R2) of 0.9902. The limit of detection of this system was found to be 1.3 nM. This method is simple, sensitive and low cost.

The influence of CdS intermediate layer on CdSe/CdS co-sensitized free-standing TiO2 nanotube solar cells

NASA Astrophysics Data System (ADS)

Ren, Xuefeng; Yu, Libo; Li, Zhen; Song, Hai; Wang, Qingyun

2018-01-01

We build CdSe quantum dots (QDs) sensitized TiO2 NT solar cells (CdSe/TiO2 solar cells) by successive ionic layer adsorption reaction (SILAR) method on free-standing translucent TiO2 nanotube (NT) film. The best power conversion efficiency (PCE) 0.74% is obtained with CdSe/TiO2 NT solar cells, however, it is very low. Hence, we introduced the CdS QDs layer located between CdSe QDs and TiO2 NT to achieve an enhanced photovoltaic performance. The J-V test results indicated that the insert of CdS intermediate layer yield a significant improvement of PCE to 2.52%. Combining experimental and theoretical analysis, we find that the effects caused by a translucent TiO2 nanotube film, a better lattices match between CdS and TiO2, and a new formed stepwise band edges structure not only improve the light harvesting efficiency but also increase the driving force of electrons, leading to the improvement of photovoltaic performance.

One-step Synthesis of Highly Luminescent Nitrogen-doped Carbon Dots for Selective and Sensitive Detection of Mercury(II) Ions and Cellular Imaging.

PubMed

Liu, Ying; Liao, Mei; He, Xueling; Liu, Xia; Kou, Xingming; Xiao, Dan

2015-01-01

In this paper, nitrogen-doped carbon dots (N-CDs) with high quantum yield (QY) of 40.5% were prepared through a facile and straightforward hydrothermal route. The as-prepared N-CDs exhibited excellent photoluminescence properties, good water-solublity and photostability, negligible cytotoxicity and favourable biocompatibility. Such N-CDs were found to serve as an effective fluorescent sensor for selective and sensitive detection of Hg(2+) in a wide linear response concentration range of 0 - 8 μM with a limit of detection (LOD) of 0.087 μM and could be applied to the determination of Hg(2+) in environmental water samples. The corresponding mechanisms were discussed in detail. Moreover, another attractive finding was that the N-CDs showed satisfactory performance in bioimaging before and after the addition of Hg(2+) in human lung cancer PC14 cells. With excellent sensitivity, selectivity and biocompatibility, such cheap carbonmaterials are potentially suitable for monitoring of Hg(2+) in environmental applications and promising for biological applications.

CdS QDs-chitosan microcapsules with stimuli-responsive property generated by gas-liquid microfluidic technique.

PubMed

Chen, Yanjun; Yao, Rongyi; Wang, Yifeng; Chen, Ming; Qiu, Tong; Zhang, Chaocan

2015-01-01

This article describes a straightforward gas-liquid microfluidic approach to generate uniform-sized chitosan microcapsules containing CdS quantum dots (QDs). CdS QDs are encapsulated into the liquid-core of the microcapsules. The sizes of the microcapsules can be conveniently controlled by gas flow rate. QDs-chitosan microcapsules show good fluorescent stability in water, and exhibit fluorescent responses to chemical environmental stimuli. α-Cyclodextrin (α-CD) causes the microcapsules to deform and even collapse. More interestingly, α-CD induces obvious changes on the fluorescent color of the microcapsules. However, β-cyclodextrin (β-CD) has little influence on the shape and fluorescent color of the microcapsules. Based on the results of scanning electron microscopy, the possible mechanism about the effects of α-CD on the chitosan microcapsules is analyzed. These stimuli-responsive microcapsules are low-cost and easy to be prepared by gas-liquid microfluidic technique, and can be applied as a potential micro-detector to chemicals, such as CDs. Copyright © 2014 Elsevier B.V. All rights reserved.

Nanocrystal grain growth and device architectures for high-efficiency CdTe ink-based photovoltaics.

PubMed

Crisp, Ryan W; Panthani, Matthew G; Rance, William L; Duenow, Joel N; Parilla, Philip A; Callahan, Rebecca; Dabney, Matthew S; Berry, Joseph J; Talapin, Dmitri V; Luther, Joseph M

2014-09-23

We study the use of cadmium telluride (CdTe) nanocrystal colloids as a solution-processable "ink" for large-grain CdTe absorber layers in solar cells. The resulting grain structure and solar cell performance depend on the initial nanocrystal size, shape, and crystal structure. We find that inks of predominantly wurtzite tetrapod-shaped nanocrystals with arms ∼5.6 nm in diameter exhibit better device performance compared to inks composed of smaller tetrapods, irregular faceted nanocrystals, or spherical zincblende nanocrystals despite the fact that the final sintered film has a zincblende crystal structure. Five different working device architectures were investigated. The indium tin oxide (ITO)/CdTe/zinc oxide structure leads to our best performing device architecture (with efficiency >11%) compared to others including two structures with a cadmium sulfide (CdS) n-type layer typically used in high efficiency sublimation-grown CdTe solar cells. Moreover, devices without CdS have improved response at short wavelengths.

Morpholine Derivative-Functionalized Carbon Dots-Based Fluorescent Probe for Highly Selective Lysosomal Imaging in Living Cells.

PubMed

Wu, Luling; Li, Xiaolin; Ling, Yifei; Huang, Chusen; Jia, Nengqin

2017-08-30

The development of a suitable fluorescent probe for the specific labeling and imaging of lysosomes through the direct visual fluorescent signal is extremely important for understanding the dysfunction of lysosomes, which might induce various pathologies, including neurodegenerative diseases, cancer, and Alzheimer's disease. Herein, a new carbon dot-based fluorescent probe (CDs-PEI-ML) was designed and synthesized for highly selective imaging of lysosomes in live cells. In this probe, PEI (polyethylenimine) is introduced to improve water solubility and provide abundant amine groups for the as-prepared CDs-PEI, and the morpholine group (ML) serves as a targeting unit for lysosomes. More importantly, passivation with PEI could dramatically increase the fluorescence quantum yield of CDs-PEI-ML as well as their stability in fluorescence emission under different excitation wavelength. Consequently, experimental data demonstrated that the target probe CDs-PEI-ML has low cytotoxicity and excellent photostability. Additionally, further live cell imaging experiment indicated that CDs-PEI-ML is a highly selective fluorescent probe for lysosomes. We speculate the mechanism for selective staining of lysosomes that CDs-PEI-ML was initially taken up by lysosomes through the endocytic pathway and then accumulated in acidic lysosomes. It is notable that there was less diffusion of CDs-PEI-ML into cytoplasm, which could be ascribed to the presence of lysosome target group morpholine on surface of CDs-PEI-ML. The blue emission wavelength combined with the high photo stability and ability of long-lasting cell imaging makes CDs-PEI-ML become an alternative fluorescent probe for multicolor labeling and long-term tracking of lysosomes in live cells and the potential application in super-resolution imaging. To best of our knowledge, there are still limited carbon dots-based fluorescent probes that have been studied for specific lysosomal imaging in live cells. The concept of surface functionality of carbon dots will also pave a new avenue for developing carbon dots-based fluorescent probes for subcellular labeling.

A new nanobiosensor for glucose with high sensitivity and selectivity in serum based on fluorescence resonance Energy transfer (FRET) between CdTe quantum dots and Au nanoparticles.

PubMed

Tang, Bo; Cao, Lihua; Xu, Kehua; Zhuo, Linhai; Ge, Jiechao; Li, Qingling; Yu, Lijuan

2008-01-01

A novel assembled nanobiosensor QDs-ConA-beta-CDs-AuNPs was designed for the direct determination of glucose in serum with high sensitivity and selectivity. The sensing approach is based on fluorescence resonance energy transfer (FRET) between CdTe quantum dots (QDs) as an energy donor and gold nanoparticles (AuNPs) as an energy acceptor. The specific combination of concanavalin A (ConA)-conjugated QDs and thiolated beta-cyclodextrins (beta-SH-CDs)-modified AuNPs assembles a hyperefficient FRET nanobiosensor. In the presence of glucose, the AuNPs-beta-CDs segment of the nanobiosensor is displaced by glucose which competes with beta-CDs on the binding sites of ConA, resulting in the fluorescence recovery of the quenched QDs. Experimental results show that the increase in fluorescence intensity is proportional to the concentration of glucose within the range of 0.10-50 muM under the optimized experimental conditions. In addition, the nanobiosensor has high sensitivity with a detection limit as low as 50 nM, and has excellent selectivity for glucose over other sugars and most biological species present in serum. The nanobiosensor was applied directly to determine glucose in normal adult human serum, and the recovery and precision of the method were satisfactory. The unique combination of high sensitivity and good selectivity of this biosensor indicates its potential for the clinical determination of glucose directly and simply in serum, and provides the possibility to detect low levels of glucose in single cells or bacterial cultures. Moreover, the designed nanobiosensor achieves direct detection in biological samples, suggesting the use of nanobiotechnology-based assembled sensors for direct analytical applications in vivo or in vitro.

Optimizing photovoltaic performance in CuInS 2 and CdS quantum dot-sensitized solar cells by using an agar-based gel polymer electrolyte

DOE PAGES

Raphael, E.; Jara, D. H.; Schiavon, M. A.

2017-01-19

Quantum dot-sensitized solar cells (QDSSCs) offer new opportunities to address the clean energy challenge, being one of the top candidates for third generation photovoltaics. Like dye-sensitized solar cells (DSSCs), QDSSCs normally use liquid electrolytes that suffer from issues such as evaporation or leakage. In this study a gel polysulfide electrolyte was prepared containing a natural polymer, agar, and was used as a quasi-solid-state electrolyte in solar cells to replace the conventional liquid electrolytes. This gel electrolyte shows almost the same conductivity as the liquid one. The solar cells were fabricated using CuInS 2 quantum dots (QDs), previously synthesized, deposited onmore » TiO 2 photoanodes by electrophoretic deposition (EPD). CdS was deposited on TiO 2 by successive ionic layer adsorption and reaction (SILAR). Reduced graphene oxide (RGO)–Cu 2S, brass, and thin film CuxS were used as counter electrodes. Compared to a liquid polysulfide water based electrolyte, solar cells based on CuInS 2 and CdS using gel polymer electrolyte (GPE) exhibit greater incident photon to current conversion efficiency (IPCE = 51.7% at 520 nm and 72.7% at 440 nm), photocurrent density (J sc = 10.75 and 13.51 mA cm -2), and power conversion efficiency (η = 2.97 and 2.98%) while exhibiting significantly enhanced stability. The solar cells employing the agar-based gel polymeric electrolyte are about a factor of 0.20 more stable than using a liquid electrolyte. The higher photovoltaic performance is due to the good conductivity and high wettability as well as the superior permeation capability of the gel electrolyte into the mesoporous matrix of a TiO 2 film« less

Optimizing photovoltaic performance in CuInS 2 and CdS quantum dot-sensitized solar cells by using an agar-based gel polymer electrolyte

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raphael, E.; Jara, D. H.; Schiavon, M. A.

Quantum dot-sensitized solar cells (QDSSCs) offer new opportunities to address the clean energy challenge, being one of the top candidates for third generation photovoltaics. Like dye-sensitized solar cells (DSSCs), QDSSCs normally use liquid electrolytes that suffer from issues such as evaporation or leakage. In this study a gel polysulfide electrolyte was prepared containing a natural polymer, agar, and was used as a quasi-solid-state electrolyte in solar cells to replace the conventional liquid electrolytes. This gel electrolyte shows almost the same conductivity as the liquid one. The solar cells were fabricated using CuInS 2 quantum dots (QDs), previously synthesized, deposited onmore » TiO 2 photoanodes by electrophoretic deposition (EPD). CdS was deposited on TiO 2 by successive ionic layer adsorption and reaction (SILAR). Reduced graphene oxide (RGO)–Cu 2S, brass, and thin film CuxS were used as counter electrodes. Compared to a liquid polysulfide water based electrolyte, solar cells based on CuInS 2 and CdS using gel polymer electrolyte (GPE) exhibit greater incident photon to current conversion efficiency (IPCE = 51.7% at 520 nm and 72.7% at 440 nm), photocurrent density (J sc = 10.75 and 13.51 mA cm -2), and power conversion efficiency (η = 2.97 and 2.98%) while exhibiting significantly enhanced stability. The solar cells employing the agar-based gel polymeric electrolyte are about a factor of 0.20 more stable than using a liquid electrolyte. The higher photovoltaic performance is due to the good conductivity and high wettability as well as the superior permeation capability of the gel electrolyte into the mesoporous matrix of a TiO 2 film« less

A study of polaritonic transparency in couplers made from excitonic materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singh, Mahi R.; Racknor, Chris

2015-03-14

We have studied light matter interaction in quantum dot and exciton-polaritonic coupler hybrid systems. The coupler is made by embedding two slabs of an excitonic material (CdS) into a host excitonic material (ZnO). An ensemble of non-interacting quantum dots is doped in the coupler. The bound exciton polariton states are calculated in the coupler using the transfer matrix method in the presence of the coupling between the external light (photons) and excitons. These bound exciton-polaritons interact with the excitons present in the quantum dots and the coupler is acting as a reservoir. The Schrödinger equation method has been used tomore » calculate the absorption coefficient in quantum dots. It is found that when the distance between two slabs (CdS) is greater than decay length of evanescent waves the absorption spectrum has two peaks and one minimum. The minimum corresponds to a transparent state in the system. However, when the distance between the slabs is smaller than the decay length of evanescent waves, the absorption spectra has three peaks and two transparent states. In other words, one transparent state can be switched to two transparent states when the distance between the two layers is modified. This could be achieved by applying stress and strain fields. It is also found that transparent states can be switched on and off by applying an external control laser field.« less

Structural characterization of nanocrystalline cadmium sulphide powder prepared by solvent evaporation technique

NASA Astrophysics Data System (ADS)

Pandya, Samir; Tandel, Digisha; Chodavadiya, Nisarg

2018-05-01

CdS is one of the most important compounds in the II-VI group of semiconductor. There are numerous applications of CdS in the form of nanoparticles and nanocrystalline. Semiconductors nanoparticles (also known as quantum dots), belong to state of matter in the transition region between molecules and solids, have attracted a great deal of attention because of their unique electrical and optical properties, compared to bulk materials. In the field of optoelectronic, nanocrystalline form utilizes mostly in the field of catalysis and fluid technology. Considering these observations, presented work had been carried out, i.e. based on the nanocrystalline material preparation. In the present work CdS nano-crystalline powder was synthesized by a simple and cost effective chemical technique to grow cadmium sulphide (CdS) nanoparticles at 200 °C with different concentrations of cadmium. The synthesis parameters were optimized. The synthesized powder was structurally characterized by X-ray diffraction and particle size analyzer. In the XRD analysis, Micro-structural parameters such as lattice strain, dislocation density and crystallite size were analysed. The broadened diffraction peaks indicated nanocrystalline particles of the film material. In addition to that the size of the prepared particles was analyzed by particle size analyzer. The results show the average size of CdS particles ranging from 80 to 100 nm. The overall conclusion of the work can be very useful in the synthesis of nanocrystalline CdS powder.

A rapid microwave synthesis of nitrogen-sulfur co-doped carbon nanodots as highly sensitive and selective fluorescence probes for ascorbic acid.

PubMed

Duan, Junxia; Yu, Jie; Feng, Suling; Su, Li

2016-06-01

A ultrafast one-step microwave-assisted method was developed for the synthesis of nitrogen-sulfur co-doped carbon nanodots (N,S-CDs) by using ethylenediamine as the carbon source and sulfamic acid as the surface passivation reagent. The morphology and the properties of N,S-CDs were explored by a series of techniques, such as high-resolution transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, UV-vis absorption and fluorescence spectroscopy. The prepared N,S-CDs exhibit bright blue photoluminescence with a high fluorescence quantum yield (FLQY) up to 28%, and high stability and excellent water solubility. A N,S-CDs-based fluorescent probe was developed for sensitive detection ascorbic acid (AA) in the presence of Cu(2+), based on the mechanism that AA reduces Cu(2+) to Cu(+), then Cu(+) quenches the fluorescence of N,S-CDs through electron or energy transfer due to the interaction between Cu(+) and thiol ligand on the N,S-CDs surface. The observed linear response concentration range was from 0.057 to 4.0μM to AA with a detection limit as low as 18nM. The probe exhibited a highly selective response toward AA even in the presence of possible interfering substances, such as uric acid and citric acid. Moreover, these promising features made the sensing system used for the analysis of human serum and urine samples. Copyright © 2016 Elsevier B.V. All rights reserved.

Development of transition metal dichalcogenide based quantum dots for light emitting diodes

NASA Astrophysics Data System (ADS)

Seth, Subhashree; Sharma, S. K.

2018-05-01

Photoluminescent quantum dots (QDs) were synthesized by facile colloidal chemical route. Its properties were characterized and analysed by utilizing Fluorescence, FTIR and UV-Vis spectrophotometers. The resultant MoS2 QD exhibits fluorescence at 470 nm for excitation wavelength 400 nm. The as prepared sample exhibits excitation dependent emission due to polydispersion of MoS2 in the dispersive medium which is the characteristics of colloidal synthesis. It is also observed that resultant MoS2 QDs show size tunable emission in the visible region. The FTIR spectrum confirms the attachment of oleic acid on the surface of MoS2. Absorption spectrum shows a band at 346 nm and a shoulder band at 400 nm. The band gap of quantum dots was obtained as 3.5 eV. CIE diagram indicates the shifting of colour coordinates towards green region with increasing excitation wavelength.

Highly efficient multiple-layer CdS quantum dot sensitized III-V solar cells.

PubMed

Lin, Chien-Chung; Han, Hau-Vei; Chen, Hsin-Chu; Chen, Kuo-Ju; Tsai, Yu-Lin; Lin, Wein-Yi; Kuo, Hao-Chung; Yu, Peichen

2014-02-01

In this review, the concept of utilization of solar spectrum in order to increase the solar cell efficiency is discussed. Among the three mechanisms, down-shifting effect is investigated in detail. Organic dye, rare-earth minerals and quantum dots are three most popular down-shift materials. While the enhancement of solar cell efficiency was not clearly observed in the past, the advances in quantum dot fabrication have brought strong response out of the hybrid platform of a quantum dot solar cell. A multiple layer structure, including PDMS as the isolation layer, is proposed and demonstrated. With the help of pulse spray system, precise control can be achieved and the optimized concentration can be found.

Secondary treatment of films of colloidal quantum dots for optoelectronics and devices produced thereby

DOEpatents

Semonin, Octavi Escala; Luther, Joseph M; Beard, Matthew C; Chen, Hsiang-Yu

2014-04-01

A method of forming an optoelectronic device. The method includes providing a deposition surface and contacting the deposition surface with a ligand exchange chemical and contacting the deposition surface with a quantum dot (QD) colloid. This initial process is repeated over one or more cycles to form an initial QD film on the deposition surface. The method further includes subsequently contacting the QD film with a secondary treatment chemical and optionally contacting the surface with additional QDs to form an enhanced QD layer exhibiting multiple exciton generation (MEG) upon absorption of high energy photons by the QD active layer. Devices having an enhanced QD active layer as described above are also disclosed.

Efficient quasisolid dye- and quantum-dot-sensitized solar cells using thiolate/disulfide redox couple and CoS counter electrode.

PubMed

Meng, Ke; Thampi, K Ravindranathan

2014-12-10

For the first time, a quasisolid thiolate/disulfide-based electrolyte was prepared using succinonitrile as a matrix. An optimized configuration of the quasisolid electrolyte contains 5-mercapto-1-methyltetrazole N-tetramethylammonium/disulfide/LiClO4/N-methylbenzimidazole in the molar ratio of 0.8:0.8:0.1:0.1. Dye-sensitized solar cells fabricated using this quasisolid electrolyte, together with N719 dye-sensitized photoelectrode and CoS counter electrode, attained power conversion efficiencies of 4.25% at 1 sun and 6.19% at 0.1 sun illumination intensities. The optimized quasisolid electrolyte, when introduced to quasisolid CdS quantum-dot-sensitized solar cells, exhibited a power conversion efficiency of 0.94%, despite the fact that CdS absorbs only a small fraction of the visible light, unlike dyes. The encouraging results show the potential for the utilization of the quasisolid thiolate/disulfide-based electrolyte in sensitized solar cells.

Immobilization effects on the photocatalytic activity of CdS quantum Dots-Horseradish peroxidase hybrid nanomaterials.

PubMed

Iñarritu, Iker; Torres, Eduardo; Topete, Antonio; Campos-Terán, José

2017-11-15

The potential use of hybrid nanomaterials based on inorganic optically active nanoparticles known as quantum dots (QDs) and horseradish peroxidase (HRP) has been proposed by several authors as light-controllable nanocatalyzers, moreover, the immobilization within or over silica based supports represents an advantage over bulk-dispersed systems. However, the implications of the immobilization of such hybrid photoactivatable catalyzing systems have not been clarified with detail. Here, we present a thorough study of the functional photoactive efficiency and recycling of immobilized CdS QDs and HRP systems with different configurations, immobilized over silanized silica quartz crystal microbalance (QCM) sensors, allowing an accurate measure of the immobilized mass of each component and its correlation with the initial reaction rate of conversion of Amplex Red (AR) to resorufin. As well, the conversion efficiency is compared between the different systems and also to non-immobilized QD-HRP complexed systems. Copyright © 2017 Elsevier Inc. All rights reserved.

A molecularly imprinted dual-emission carbon dot-quantum dot mesoporous hybrid for ratiometric determination of anti-inflammatory drug celecoxib

NASA Astrophysics Data System (ADS)

Amjadi, Mohammad; Jalili, Roghayeh

2018-02-01

We report on a ratiometric fluorescent sensor based on dual-emission molecularly imprinted mesoporous silica embedded with carbon dots and CdTe quantum dots (mMIP@CDs/QDs) for celecoxib (CLX) as target molecule. The fluorescence of the embedded CDs is insensitive to the analyte while the green emissive QDs are selectively quenched by it. This effect is much stronger for the MIP than for the non-imprinted polymer, which indicates a good recognition ability of the mesoporous MIP. The hybrid sensor also exhibited good selectivity to CLX over other substances. The ratio of the intensity at two wavelengths (F550/F440) proportionally decreased with the increasing of CLX concentration in the range of 0.08-0.90 μM. A detection limit as low as 57 nM was achieved. Experimental results testified that this sensor was highly sensitive and selective for the detection of CLX in human serum samples.

Enhanced oxidation stability of quasi core-shell alloyed CdSeS quantum dots prepared through aqueous microwave synthesis technique.

PubMed

Zhan, Hong-Ju; Zhou, Pei-Jiang; Ma, Rong; Liu, Xi-Jing; He, Yu-Ning; Zhou, Chuan-Yun

2014-01-01

Quasi core shell alloyed CdSeS quantum dots (QDs) have been prepared through a facile aqueous-phase route employing microwave irradiation technique. The optical spectroscopy and structure characterization evidenced the quasi core shell alloyed structures of CdSeS QDs. The X-ray diffraction patterns of the obtained CdSeS QDs displayed peak positions very close to those of bulk cubic CdS crystal structures and the result of X-ray photoelectron spectroscopy data re-confirmed the thick CdS shell on the CdSe core. The TEM images and HRTEM images of the CdSeS QDs ascertained the well-defined spherical particles and a relatively narrow size distribution. On the basis, the stability of the obtained QDs in an oxidative environment was also discussed using etching reaction by H2O2. The experiments result showed the as-prepared QDs present high tolerance towards H2O2, obviously superior to the commonly used CdTe QDs and core-shell CdTe/CdS QDs, which was attributed to the unique quasi core-shell CdSeS crystal structure and the small lattice mismatch between CdSe and CdS semiconductor materials. This assay provided insight to obtain high stable crystal structured semiconductor nanocrystals in the design and synthesis process.

One-step colloidal synthesis of biocompatible water-soluble ZnS quantum dot/chitosan nanoconjugates

NASA Astrophysics Data System (ADS)

Ramanery, Fábio P.; Mansur, Alexandra AP; Mansur, Herman S.

2013-12-01

Quantum dots (QDs) are luminescent semiconductor nanocrystals with great prospective for use in biomedical and environmental applications. Nonetheless, eliminating the potential cytotoxicity of the QDs made with heavy metals is still a challenge facing the research community. Thus, the aim of this work was to develop a novel facile route for synthesising biocompatible QDs employing carbohydrate ligands in aqueous colloidal chemistry with optical properties tuned by pH. The synthesis of ZnS QDs capped by chitosan was performed using a single-step aqueous colloidal process at room temperature. The nanobioconjugates were extensively characterised by several techniques, and the results demonstrated that the average size of ZnS nanocrystals and their fluorescent properties were influenced by the pH during the synthesis. Hence, novel 'cadmium-free' biofunctionalised systems based on ZnS QDs capped by chitosan were successfully developed exhibiting luminescent activity that may be used in a large number of possible applications, such as probes in biology, medicine and pharmacy.

Solar cells using quantum funnels.

PubMed

Kramer, Illan J; Levina, Larissa; Debnath, Ratan; Zhitomirsky, David; Sargent, Edward H

2011-09-14

Colloidal quantum dots offer broad tuning of semiconductor bandstructure via the quantum size effect. Devices involving a sequence of layers comprised of quantum dots selected to have different diameters, and therefore bandgaps, offer the possibility of funneling energy toward an acceptor. Here we report a quantum funnel that efficiently conveys photoelectrons from their point of generation toward an intended electron acceptor. Using this concept we build a solar cell that benefits from enhanced fill factor as a result of this quantum funnel. This concept addresses limitations on transport in soft condensed matter systems and leverages their advantages in large-area optoelectronic devices and systems.

Tailoring growth conditions for efficient tuning of band edge of CdS nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Susha, N.; Nair, Swapna S., E-mail: swapna.s.nair@gmail.com; Aravind, P. B.

2015-06-24

CdS nanoparticles are successively synthesized by chemical precipitation method. The samples prepared at different reaction time and temperature are characterized by X-ray diffraction, Diffuse reflectance spectroscopy, Photoluminescence spectroscopy ans Energy dispersive x-ray analysis. Visible color variation is noted from light yellow to orange, indicates the quantum confinement effect and the results are again got confirmed from the optical studies. A shift in absorption peak is observed towards the lower region of the visible spectra - the “blue shift”- upon decrease in reaction time and temperature. Blue emission observed in the photoluminescence spectrum confirms the grain size induced confinement.

Clustering of Cyclodextrin-Functionalized Microbeads by an Amphiphilic Biopolymer: Real-Time Observation of Structures Resembling Blood Clots.

PubMed

Arya, Chandamany; Saez Cabesas, Camila A; Huang, Hubert; Raghavan, Srinivasa R

2017-10-25

Colloidal particles can be induced to cluster by adding polymers in a process called bridging flocculation. For bridging to occur, the polymer must bind strongly to the surfaces of adjacent particles, such as via electrostatic interactions. Here, we introduce a new system where bridging occurs due to specific interactions between the side chains of an amphiphilic polymer and supramolecules on the particle surface. The polymer is a hydrophobically modified chitosan (hmC) while the particles are uniform polymeric microbeads (∼160 μm in diameter) made by a microfluidic technique and functionalized on their surface by α-cyclodextrins (CDs). The CDs have hydrophobic binding pockets that can capture the n-alkyl hydrophobes present along the hmC chains. Clustering of CD-coated microbeads in water by hmC is visualized in real time using optical microscopy. Interestingly, the clustering follows two distinct stages: first, the microbeads are bridged into clusters by hmC chains, which occurs by the interaction of individual chains with the CDs on adjacent particles. Thereafter, additional hmC from the solution adsorbs onto the surfaces of the microbeads and an hmC "mesh" grows around the clusters. This growing nanostructured mesh can trap surrounding microsized objects and sequester them within the overall cluster. Such clustering is reminiscent of blood clotting where blood platelets initially cluster at a wound site, whereupon they induce growth of a protein (fibrin) mesh around the clusters, which entraps other passive cells. Clustering does not occur with the native chitosan (lacking hydrophobes) or with the bare particles (lacking CDs); these results confirm that the clustering is indeed due to hydrophobic interactions between the hmC and the CDs. Microbead clustering via amphiphilic biopolymers could be applicable in embolization, which is a surgical technique used to block blood flow to a particular area of the body, or in agglutination assays.

High Quantum Yield Blue Emission from Lead-Free Inorganic Antimony Halide Perovskite Colloidal Quantum Dots.

PubMed

Zhang, Jian; Yang, Ying; Deng, Hui; Farooq, Umar; Yang, Xiaokun; Khan, Jahangeer; Tang, Jiang; Song, Haisheng

2017-09-26

Colloidal quantum dots (QDs) of lead halide perovskite have recently received great attention owing to their remarkable performances in optoelectronic applications. However, their wide applications are hindered from toxic lead element, which is not environment- and consumer-friendly. Herein, we utilized heterovalent substitution of divalent lead (Pb 2+ ) with trivalent antimony (Sb 3+ ) to synthesize stable and brightly luminescent Cs 3 Sb 2 Br 9 QDs. The lead-free, full-inorganic QDs were fabricated by a modified ligand-assisted reprecipitation strategy. A photoluminescence quantum yield (PLQY) was determined to be 46% at 410 nm, which was superior to that of other reported halide perovskite QDs. The PL enhancement mechanism was unraveled by surface composition derived quantum-well band structure and their large exciton binding energy. The Br-rich surface and the observed 530 meV exciton binding energy were proposed to guarantee the efficient radiative recombination. In addition, we can also tune the inorganic perovskite QD (Cs 3 Sb 2 X 9 ) emission wavelength from 370 to 560 nm via anion exchange reactions. The developed full-inorganic lead-free Sb-perovskite QDs with high PLQY and stable emission promise great potential for efficient emission candidates.

Patterned mist deposition of tri-colour CdSe/ZnS quantum dot films toward RGB LED devices

NASA Astrophysics Data System (ADS)

Pickering, S.; Kshirsagar, A.; Ruzyllo, J.; Xu, J.

2012-06-01

In this experiment a technique of mist deposition was explored as a way to form patterned ultra-thin-films of CdSe/ZnS core/shell nanocrystalline quantum dots using colloidal solutions. The objective of this study was to investigate the feasibility of mist deposition as a patterning method for creating multicolour quantum dot light emitting diodes. Mist deposition was used to create three rows of quantum dot light emitting diodes on a single device with each row having a separate colour. The colours chosen were red, green and yellow with corresponding peak wavelengths of 620 nm, 558 nm, and 587 nm. The results obtained from this experiment show that it is possible to create multicolour devices on a single substrate. The peak brightnesses obtained in this experiment for the red, green, and yellow were 508 cd/m, 507 cd/m, and 665 cd/m, respectively. The similar LED brightness is important in display technologies using colloidal quantum dots in a precursor solution to ensure one colour does not dominate the emitted spectrum. Results obtained in-terms of brightness were superior to those achieved with inkjet deposition. This study has shown that mist deposition is a viable method for patterned deposition applied to quantum dot light emitting diode display technologies.

Phosphine-free synthesis and characterization of type-II ZnSe/CdS core-shell quantum dots

NASA Astrophysics Data System (ADS)

Ghasemzadeh, Roghayyeh; Armanmehr, Mohammad Hasan; Abedi, Mohammad; Fateh, Davood Sadeghi; Bahreini, Zaker

2018-01-01

A phosphine-free route for synthesis of type-II ZnSe/CdS core-shell quantum dots, using green, low cost and environmentally friendly reagents and phosphine-free solvents such as 1-octadecene (ODE) and liquid paraffin has been reported. Hot-injection technique has been used for the synthesis of ZnSe core quantum dots. The CdS shell quantum dots prepared by reaction of CdO precursor and S powder in 1-octadecene (ODE). The ZnSe/CdS core-shell quantum dots were synthesized via successive ion layer adsorption and reaction (SILAR) technique. The characterization of produced quantum dots were performed by absorption and fluorescence spectroscopy, X-ray diffraction (XRD) and energy dispersive X-ray spectroscopy (EDX) and transmission electron microscopy (TEM). The results showed the formation of type-II ZnSe/CdS core-shell quantum dots with FWHM 32 nm and uniform size distribution.

Mn-doped quantum dot sensitized solar cells: a strategy to boost efficiency over 5%.

PubMed

Santra, Pralay K; Kamat, Prashant V

2012-02-08

To make Quantum Dot Sensitized Solar Cells (QDSC) competitive, it is necessary to achieve power conversion efficiencies comparable to other emerging solar cell technologies. By employing Mn(2+) doping of CdS, we have now succeeded in significantly improving QDSC performance. QDSC constructed with Mn-doped-CdS/CdSe deposited on mesoscopic TiO(2) film as photoanode, Cu(2)S/Graphene Oxide composite electrode, and sulfide/polysulfide electrolyte deliver power conversion efficiency of 5.4%.

Colloidal quantum dot solar cells exploiting hierarchical structuring.

PubMed

Labelle, André J; Thon, Susanna M; Masala, Silvia; Adachi, Michael M; Dong, Haopeng; Farahani, Maryam; Ip, Alexander H; Fratalocchi, Andrea; Sargent, Edward H

2015-02-11

Extremely thin-absorber solar cells offer low materials utilization and simplified manufacture but require improved means to enhance photon absorption in the active layer. Here, we report enhanced-absorption colloidal quantum dot (CQD) solar cells that feature transfer-stamped solution-processed pyramid-shaped electrodes employed in a hierarchically structured device. The pyramids increase, by up to a factor of 2, the external quantum efficiency of the device at absorption-limited wavelengths near the absorber band edge. We show that absorption enhancement can be optimized with increased pyramid angle with an appreciable net improvement in power conversion efficiency, that is, with the gain in current associated with improved absorption and extraction overcoming the smaller fractional decrease in open-circuit voltage associated with increased junction area. We show that the hierarchical combination of micron-scale structured electrodes with nanoscale films provides for an optimized enhancement at absorption-limited wavelengths. We fabricate 54.7° pyramid-patterned electrodes, conformally apply the quantum dot films, and report pyramid CQD solar cells that exhibit a 24% improvement in overall short-circuit current density with champion devices providing a power conversion efficiency of 9.2%.

Efficient Carrier Multiplication in Colloidal Silicon Nanorods

DOE PAGES

Stolle, Carl Jackson; Lu, Xiaotang; Yu, Yixuan; ...

2017-08-01

In this study, auger recombination lifetimes, absorption cross sections, and the quantum yields of carrier multiplication (CM), or multiexciton generation (MEG), were determined for solvent-dispersed silicon (Si) nanorods using transient absorption spectroscopy (TAS). Nanorods with an average diameter of 7.5 nm and aspect ratios of 6.1, 19.3, and 33.2 were examined. Colloidal Si nanocrystals of similar diameters were also studied for comparison. The nanocrystals and nanorods were passivated with organic ligands by hydrosilylation to prevent surface oxidation and limit the effects of surface trapping of photoexcited carriers. All samples used in the study exhibited relatively efficient photoluminescence. The Auger lifetimesmore » increased with nanorod length, and the nanorods exhibited higher CM quantum yield and efficiency than the nanocrystals with a similar band gap energy E g. Beyond a critical length, the CM quantum yield decreases. Finally, nanorods with the aspect ratio of 19.3 had the highest CM quantum yield of 1.6 ± 0.2 at 2.9E g, which corresponded to a multiexciton yield that was twice as high as observed for the spherical nanocrystals.« less

Organic molecules as tools to control the growth, surface structure, and redox activity of colloidal quantum dots.

PubMed

Weiss, Emily A

2013-11-19

In order to achieve efficient and reliable technology that can harness solar energy, the behavior of electrons and energy at interfaces between different types or phases of materials must be understood. Conversion of light to chemical or electrical potential in condensed phase systems requires gradients in free energy that allow the movement of energy or charge carriers and facilitate redox reactions and dissociation of photoexcited states (excitons) into free charge carriers. Such free energy gradients are present at interfaces between solid and liquid phases or between inorganic and organic materials. Nanostructured materials have a higher density of these interfaces than bulk materials. Nanostructured materials, however, have a structural and chemical complexity that does not exist in bulk materials, which presents a difficult challenge: to lower or eliminate energy barriers to electron and energy flux that inevitably result from forcing different materials to meet in a spatial region of atomic dimensions. Chemical functionalization of nanostructured materials is perhaps the most versatile and powerful strategy for controlling the potential energy landscape of their interfaces and for minimizing losses in energy conversion efficiency due to interfacial structural and electronic defects. Colloidal quantum dots are semiconductor nanocrystals synthesized with wet-chemical methods and coated in organic molecules. Chemists can use these model systems to study the effects of chemical functionalization of nanoscale organic/inorganic interfaces on the optical and electronic properties of a nanostructured material, and the behavior of electrons and energy at interfaces. The optical and electronic properties of colloidal quantum dots have an intense sensitivity to their surface chemistry, and their organic adlayers make them dispersible in solvent. This allows researchers to use high signal-to-noise solution-phase spectroscopy to study processes at interfaces. In this Account, I describe the varied roles of organic molecules in controlling the structure and properties of colloidal quantum dots. Molecules serve as surfactant that determines the mechanism and rate of nucleation and growth and the final size and surface structure of a quantum dot. Anionic surfactant in the reaction mixture allows precise control over the size of the quantum dot core but also drives cation enrichment and structural disordering of the quantum dot surface. Molecules serve as chemisorbed ligands that dictate the energetic distribution of surface states. These states can then serve as thermodynamic traps for excitonic charge carriers or couple to delocalized states of the quantum dot core to change the confinement energy of excitonic carriers. Ligands, therefore, in some cases, dramatically shift the ground state absorption and photoluminescence spectra of quantum dots. Molecules also act as protective layers that determine the probability of redox processes between quantum dots and other molecules. How much the ligand shell insulates the quantum dot from electron exchange with a molecular redox partner depends less on the length or degree of conjugation of the native ligand and more on the density and packing structure of the adlayer and the size and adsorption mode of the molecular redox partner. Control of quantum dot properties in these examples demonstrates that nanoscale interfaces, while complex, can be rationally designed to enhance or specify the functionality of a nanostructured system.

Aqueous Synthesis of PEGylated Quantum Dots with Increased Colloidal Stability and Reduced Cytotoxicity.

PubMed

Ulusoy, Mehriban; Jonczyk, Rebecca; Walter, Johanna-Gabriela; Springer, Sergej; Lavrentieva, Antonina; Stahl, Frank; Green, Mark; Scheper, Thomas

2016-02-17

Ligands used on the surface of colloidal nanoparticles (NPs) have a significant impact on physiochemical properties of NPs and their interaction in biological environments. In this study, we report a one-pot aqueous synthesis of 3-mercaptopropionic acid (MPA)-functionalized CdTe/CdS/ZnS quantum dots (Qdots) in the presence of thiol-terminated methoxy polyethylene glycol (mPEG) molecules as a surface coordinating ligand. The resulting mPEG-Qdots were characterized by using ζ potential, FTIR, thermogravimetric (TG) analysis, and microscale thermophoresis (MST) studies. We investigated the effect of mPEG molecules and their grafting density on the Qdots photophysical properties, colloidal stability, protein binding affinity, and in vitro cellular toxicity. Moreover, cellular binding features of the resulting Qdots were examined by using three-dimensional (3D) tumor-like spheroids, and the results were discussed in detail. Promisingly, mPEG ligands were found to increase colloidal stability of Qdots, reduce adsorption of proteins to the Qdot surface, and mitigate Qdot-induced side effects to a great extent. Flow cytometry and confocal microscopy studies revealed that PEGylated Qdots exhibited distinctive cellular interactions with respect to their mPEG grafting density. As a result, mPEG molecules demonstrated a minimal effect on the ZnS shell deposition and the Qdot fluorescence efficiency at a low mPEG density, whereas they showed pronounced effect on Qdot colloidal stability, protein binding affinity, cytotoxicity, and nonspecific binding at a higher mPEG grafting amount.

Preparation of an Efficient Ratiometric Fluorescent Nanoprobe (m-CDs@[Ru(bpy)3]2+) for Visual and Specific Detection of Hypochlorite on Site and in Living Cells.

PubMed

Zhan, Yuanjin; Luo, Fang; Guo, Longhua; Qiu, Bin; Lin, Yuhong; Li, Juan; Chen, Guonan; Lin, Zhenyu

2017-11-22

Hypochlorite (ClO - ) is one of the most important reactive oxygen species (ROS), which plays an important role in sustaining human innate immunity during microbial invasion. Moreover, ClO - is a powerful oxidizer for water treatment. The safety of drinking water is closely related to its content. Herein, m-phenylenediamine (mPD) is used as a precursor to prepare carbon dots (named m-CDs) with highly fluorescent quantum yield (31.58% in water), and our investigation shows that the strong fluorescent emission of m-CDs can be effectively quenched by ClO - . Based on these findings, we developed a novel fluorescent nanoprobe (m-CDs) for highly selective detection of ClO - . The linear range was from 0.05 to 7 μM (R 2 = 0.998), and the limit of detection (S/N = 3) was as low as 0.012 μM. Moreover, a portable agarose hydrogel solid matrix-based ratiometric fluorescent nanoprobe (m-CDs@[Ru(bpy) 3 ] 2+ ) sensor was subsequently developed for visual on-site detection of ClO - with the naked eyes under a UV lamp, suggesting its potential in practical application with low cost and excellent performance in water quality monitoring. Additionally, intracellular detection of exogenous ClO - was demonstrated via ratiometric imaging microscopy.

Modulation of the photoluminescence in carbon dots through surface modification: from mechanism to white light-emitting diodes.

PubMed

Zhu, Jinyang; Shao, He; Bai, Xue; Zhai, Yue; Zhu, Yongsheng; Chen, Xu; Pan, Gencai; Dong, Biao; Xu, Lin; Zhang, Hanzhuang; Song, Hongwei

2018-06-15

Carbon dots (CDs) have emerged as a new type of fluorescent material because of their unique optical advantages, such as high photoluminescence quantum yields (QYs), excellent photo-stability, excitation-dependent emissions, and low toxicity. However, the photoluminescence mechanism for CDs remains unclear, which limits their further practical application. Here, CDs were synthesized via a solvothermal route from citric acid and urea. Through the oxidation and reduction treatment of pristine CDs, the origin of the photoluminescence and the involved mechanism were revealed. We found that the blue/green/red emissions originated from three diverse emitting states, i.e. the intrinsic state, and C=O- and C=N-related surface states, respectively. Based on the as-prepared CDs, a pH sensor depending on the radiometric luminescence detection was developed. Furthermore, we constructed CD/PVP (PVP, polyvinylpyrrolidone) composite films, which exhibited white light emission with photoluminescence QYs of 15.3%. The white light emission with different correlated color temperatures (CCTs), from 4807 K to 3319 K, was obtained by simply changing the amount of PVP solution. Benefiting from the white light-emitting solid-state films, single-component white light-emitting diodes were fabricated with an average color rendering index value (Ra) of 80.0, luminous efficiency of 10.2 lm W -1 , and good working stability, thus indicating a promising potential for practical lighting applications.

Modulation of the photoluminescence in carbon dots through surface modification: from mechanism to white light-emitting diodes

NASA Astrophysics Data System (ADS)

Zhu, Jinyang; Shao, He; Bai, Xue; Zhai, Yue; Zhu, Yongsheng; Chen, Xu; Pan, Gencai; Dong, Biao; Xu, Lin; Zhang, Hanzhuang; Song, Hongwei

2018-06-01

Carbon dots (CDs) have emerged as a new type of fluorescent material because of their unique optical advantages, such as high photoluminescence quantum yields (QYs), excellent photo-stability, excitation-dependent emissions, and low toxicity. However, the photoluminescence mechanism for CDs remains unclear, which limits their further practical application. Here, CDs were synthesized via a solvothermal route from citric acid and urea. Through the oxidation and reduction treatment of pristine CDs, the origin of the photoluminescence and the involved mechanism were revealed. We found that the blue/green/red emissions originated from three diverse emitting states, i.e. the intrinsic state, and C=O- and C=N-related surface states, respectively. Based on the as-prepared CDs, a pH sensor depending on the radiometric luminescence detection was developed. Furthermore, we constructed CD/PVP (PVP, polyvinylpyrrolidone) composite films, which exhibited white light emission with photoluminescence QYs of 15.3%. The white light emission with different correlated color temperatures (CCTs), from 4807 K to 3319 K, was obtained by simply changing the amount of PVP solution. Benefiting from the white light-emitting solid-state films, single-component white light-emitting diodes were fabricated with an average color rendering index value (Ra) of 80.0, luminous efficiency of 10.2 lm W‑1, and good working stability, thus indicating a promising potential for practical lighting applications.

Liquid Crystal Colloids

NASA Astrophysics Data System (ADS)

Smalyukh, Ivan I.

2018-03-01

Colloids are abundant in nature, science, and technology, with examples ranging from milk to quantum dots and the colloidal atom paradigm. Similarly, liquid crystal ordering is important in contexts ranging from biological membranes to laboratory models of cosmic strings and liquid crystal displays in consumer devices. Some of the most exciting recent developments in both of these soft matter fields emerge at their interface, in the fast-growing research arena of liquid crystal colloids. Mesoscale self-assembly in such systems may lead to artificial materials and to structures with emergent physical behavior arising from patterning of molecular order and nano- or microparticles into precisely controlled configurations. Liquid crystal colloids show exceptional promise for new discovery that may impinge on composite material fabrication, low-dimensional topology, photonics, and so on. Starting from physical underpinnings, I review the state of the art in this fast-growing field, with a focus on its scientific and technological potential.

Sulfur and nitrogen binary doped carbon dots derived from ammonium thiocyanate for selective probing doxycycline in living cells and multicolor cell imaging.

PubMed

Xue, Mingyue; Zhang, Liangliang; Zhan, Zhihua; Zou, Mengbing; Huang, Yong; Zhao, Shulin

2016-04-01

A novel sulfur and nitrogen binary doped carbon dots (S,N-CDs) was synthesized by one-step manner through the hydrothermal treatment of citric acid (CA) and ammonium thiocyanate, and the procedures for biomedical applications, including probing doxycycline in living cells and multicolor cell imaging were developed. The obtained S,N-CDs are stable in aqueous solution, possess a very high quantum yield (QY, 74.15%) and good photostability. The fluorescence of S,N-CDs can be specifically quenched by doxycycline, providing a convenient turn-off assay of doxycycline. This assay shows a wide linear detection range from 0.08 to 60 μM with a low detection limit of 20 nM. The present method also displays a good selectivity. More importantly, the S,N-CDs have an excellent biocompatibility and low cytotoxicity, allowing the multicolor cell imaging and doxycycline detection in living cells. Consequently, the developed doxycycline methods is facile, low-cost, biocompatible, sensitive and selective, which may hold the potential applications in the fields of food safety and environmental monitoring, as well as cancer therapy and related mechanism research. Copyright © 2015 Elsevier B.V. All rights reserved.

Constructing a MoS₂ QDs/CdS Core/Shell Flowerlike Nanosphere Hierarchical Heterostructure for the Enhanced Stability and Photocatalytic Activity.

PubMed

Liang, Shijing; Zhou, Zhouming; Wu, Xiuqin; Zhu, Shuying; Bi, Jinhong; Zhou, Limin; Liu, Minghua; Wu, Ling

2016-02-15

MoS₂ quantum dots (QDs)/CdS core/shell nanospheres with a hierarchical heterostructure have been prepared by a simple microwave hydrothermal method. The as-prepared samples are characterized by XRD, TEM, SEM, UV-VIS diffuse reflectance spectra (DRS) and N₂-sorption in detail. The photocatalytic activities of the samples are evaluated by water splitting into hydrogen. Results show that the as-prepared MoS₂ QDs/CdS core/shell nanospheres with a diameter of about 300 nm are composed of the shell of CdS nanorods and the core of MoS₂ QDs. For the photocatalytic reaction, the samples exhibit a high stability of the photocatalytic activity and a much higher hydrogen evolution rate than the pure CdS, the composite prepared by a physical mixture, and the Pt-loaded CdS sample. In addition, the stability of CdS has also been greatly enhanced. The effect of the reaction time on the formations of nanospheres, the photoelectric properties and the photocatalytic activities of the samples has been investigated. Finally, a possible photocatalytic reaction process has also been proposed.

Highly efficient visible-light-driven photocatalytic hydrogen production of CdS-cluster-decorated graphene nanosheets.

PubMed

Li, Qin; Guo, Beidou; Yu, Jiaguo; Ran, Jingrun; Zhang, Baohong; Yan, Huijuan; Gong, Jian Ru

2011-07-20

The production of clean and renewable hydrogen through water splitting using photocatalysts has received much attention due to the increasing global energy crises. In this study, a high efficiency of the photocatalytic H(2) production was achieved using graphene nanosheets decorated with CdS clusters as visible-light-driven photocatalysts. The materials were prepared by a solvothermal method in which graphene oxide (GO) served as the support and cadmium acetate (Cd(Ac)(2)) as the CdS precursor. These nanosized composites reach a high H(2)-production rate of 1.12 mmol h(-1) (about 4.87 times higher than that of pure CdS nanoparticles) at graphene content of 1.0 wt % and Pt 0.5 wt % under visible-light irradiation and an apparent quantum efficiency (QE) of 22.5% at wavelength of 420 nm. This high photocatalytic H(2)-production activity is attributed predominantly to the presence of graphene, which serves as an electron collector and transporter to efficiently lengthen the lifetime of the photogenerated charge carriers from CdS nanoparticles. This work highlights the potential application of graphene-based materials in the field of energy conversion.

Controlled waveguide coupling for photon emission from colloidal PbS quantum dot using tunable microcavity made of optical polymer and silicon

NASA Astrophysics Data System (ADS)

Nozaka, Takahiro; Mukai, Kohki

2016-04-01

A tunable microcavity device composed of optical polymer and Si with a colloidal quantum dot (QD) is proposed as a single-photon source for planar optical circuit. Cavity size is controlled by electrostatic micromachine behavior with the air bridge structure to tune timing of photon injection into optical waveguide from QD. Three-dimensional positioning of a QD in the cavity structure is available using a nanohole on Si processed by scanning probe microscope lithography. We fabricated the prototype microcavity with PbS-QD-mixed polymenthyl methacrylate on a SOI (semiconductor-on-insulator) substrate to show the tunability of cavity size as the shift of emission peak wavelength of QD ensemble.

Lasing from colloidal InP/ZnS quantum dots.

PubMed

Gao, Shuai; Zhang, Chunfeng; Liu, Yanjun; Su, Huaipeng; Wei, Lai; Huang, Tony; Dellas, Nicholas; Shang, Shuzhen; Mohney, Suzanne E; Wang, Jingkang; Xu, Jian

2011-03-14

High-quality InP/ZnS core-shell nanocrystal quantum dots (NQDs) were synthesized as a heavy-metal-free alternative to the gain media of cadmium-based colloidal nanoparticles. Upon UV excitation, amplified spontaneous emission (ASE) and optical gain were observed, for the first time, in close-packed InP/ZnS core-shell NQDs. The ASE wavelength can be selected by tailoring the nanocrystal size over a broad range of the spectrum. Moreover, the optical gain profile of InP/ZnS NQDs was matched to the second order feedback of holographic polymer-dispersed liquid crystal gratings, leading to the very first demonstration of an optically-pumped, nanocrystal laser based on InP/ZnS core-shell NQDs.

sp-d Exchange Interactions in Wave Function Engineered Colloidal CdSe/Mn:CdS Hetero-Nanoplatelets.

PubMed

Muckel, Franziska; Delikanli, Savas; Hernández-Martínez, Pedro Ludwig; Priesner, Tamara; Lorenz, Severin; Ackermann, Julia; Sharma, Manoj; Demir, Hilmi Volkan; Bacher, Gerd

2018-03-14

In two-dimensional (2D) colloidal semiconductor nanoplatelets, which are atomically flat nanocrystals, the precise control of thickness and composition on the atomic scale allows for the synthesis of heterostructures with well-defined electron and hole wave function distributions. Introducing transition metal dopants with a monolayer precision enables tailored magnetic exchange interactions between dopants and band states. Here, we use the absorption based technique of magnetic circular dichroism (MCD) to directly prove the exchange coupling of magnetic dopants with the band charge carriers in hetero-nanoplatelets with CdSe core and manganese-doped CdS shell (CdSe/Mn:CdS). We show that the strength of both the electron as well as the hole exchange interactions with the dopants can be tuned by varying the nanoplatelets architecture with monolayer accuracy. As MCD is highly sensitive for excitonic resonances, excited level spectroscopy allows us to resolve and identify, in combination with wave function calculations, several excited state transitions including spin-orbit split-off excitonic contributions. Thus, our study not only demonstrates the possibility to expand the extraordinary physical properties of colloidal nanoplatelets toward magneto-optical functionality by transition metal doping but also provides an insight into the excited state electronic structure in this novel two-dimensional material.

Enabling two-dimensional fourier transform electronic spectroscopy on quantum dots

NASA Astrophysics Data System (ADS)

Hill, Robert John, Jr.

Colloidal semiconductor nanocrystals exhibit unique properties not seen in their bulk counterparts. Quantum confinement of carriers causes a size-tunable bandgap, making them attractive candidates for solar cells. Fundamental understanding of their spectra and carrier dynamics is obscured by inhomogeneous broadening arising from the size distribution. Because quantum dots have long excited state lifetimes and are sensitive to both air and moisture, there are many potential artifacts in femtosecond experiments. Two-dimensional electronic spectroscopy promises insight into the photo-physics, but required key instrumental advances. Optics that can process a broad bandwidth without distortion are required for a two-dimensional optical spectrometer. To control pathlength differences for femtosecond time delays, hollow retro-reflectors are used on actively stabilized delay lines in interferometers. The fabrication of rigid, lightweight, precision hollow rooftop retroreflectors that allow beams to be stacked while preserving polarization is described. The rigidity and low mass enable active stabilization of an interferometer to within 0.6 nm rms displacement, while the return beam deviation is sufficient for Fourier transform spectroscopy with a frequency precision of better than 1 cm -1. Keeping samples oxygen and moisture free while providing fresh sample between laser shots is challenging in an interferometer. A low-vibration spinning sample cell was designed and built to keep samples oxygen free for days while allowing active stabilization of interferometer displacement to ˜1 nm. Combining these technologies has enabled 2D short-wave infrared spectroscopy on colloidal PbSe nanocrystals. 2D spectra demonstrate the advantages of this key instrumentation while providing valuable insight into the low-lying electronic states of colloidal quantum dots.

Ag colloids and arrays for plasmonic non-radiative energy transfer from quantum dots to a quantum well

NASA Astrophysics Data System (ADS)

Murphy, Graham P.; Gough, John J.; Higgins, Luke J.; Karanikolas, Vasilios D.; Wilson, Keith M.; Garcia Coindreau, Jorge A.; Zubialevich, Vitaly Z.; Parbrook, Peter J.; Bradley, A. Louise

2017-03-01

Non-radiative energy transfer (NRET) can be an efficient process of benefit to many applications including photovoltaics, sensors, light emitting diodes and photodetectors. Combining the remarkable optical properties of quantum dots (QDs) with the electrical properties of quantum wells (QWs) allows for the formation of hybrid devices which can utilize NRET as a means of transferring absorbed optical energy from the QDs to the QW. Here we report on plasmon-enhanced NRET from semiconductor nanocrystal QDs to a QW. Ag nanoparticles in the form of colloids and ordered arrays are used to demonstrate plasmon-mediated NRET from QDs to QWs with varying top barrier thicknesses. Plasmon-mediated energy transfer (ET) efficiencies of up to ˜25% are observed with the Ag colloids. The distance dependence of the plasmon-mediated ET is found to follow the same d -4 dependence as the direct QD to QW ET. There is also evidence for an increase in the characteristic distance of the interaction, thus indicating that it follows a Förster-like model with the Ag nanoparticle-QD acting as an enhanced donor dipole. Ordered Ag nanoparticle arrays display plasmon-mediated ET efficiencies up to ˜21%. To explore the tunability of the array system, two arrays with different geometries are presented. It is demonstrated that changing the geometry of the array allows a transition from overall quenching of the acceptor QW emission to enhancement, as well as control of the competition between the QD donor quenching and ET rates.

Topological protection of multiparticle dissipative transport

NASA Astrophysics Data System (ADS)

Loehr, Johannes; Loenne, Michael; Ernst, Adrian; de Las Heras, Daniel; Fischer, Thomas M.

2016-06-01

Topological protection allows robust transport of localized phenomena such as quantum information, solitons and dislocations. The transport can be either dissipative or non-dissipative. Here, we experimentally demonstrate and theoretically explain the topologically protected dissipative motion of colloidal particles above a periodic hexagonal magnetic pattern. By driving the system with periodic modulation loops of an external and spatially homogeneous magnetic field, we achieve total control over the motion of diamagnetic and paramagnetic colloids. We can transport simultaneously and independently each type of colloid along any of the six crystallographic directions of the pattern via adiabatic or deterministic ratchet motion. Both types of motion are topologically protected. As an application, we implement an automatic topologically protected quality control of a chemical reaction between functionalized colloids. Our results are relevant to other systems with the same symmetry.

Picosecond Dynamics of Excitonic Magnetic Polarons in Colloidal Diffusion-Doped Cd(1-x)Mn(x)Se Quantum Dots.

PubMed

Nelson, Heidi D; Bradshaw, Liam R; Barrows, Charles J; Vlaskin, Vladimir A; Gamelin, Daniel R

2015-11-24

Spontaneous magnetization is observed at zero magnetic field in photoexcited colloidal Cd(1-x)Mn(x)Se (x = 0.13) quantum dots (QDs) prepared by diffusion doping, reflecting strong Mn(2+)-exciton exchange coupling. The picosecond dynamics of this phenomenon, known as an excitonic magnetic polaron (EMP), are examined using a combination of time-resolved photoluminescence, magneto-photoluminescence, and Faraday rotation (TRFR) spectroscopies, in conjunction with continuous-wave absorption, magnetic circular dichroism (MCD), and magnetic circularly polarized photoluminescence (MCPL) spectroscopies. The data indicate that EMPs form with random magnetization orientations at zero external field, but their formation can be directed by an external magnetic field. After formation, however, external magnetic fields are unable to reorient the EMPs within the luminescence lifetime, implicating anisotropy in the EMP potential-energy surfaces. TRFR measurements in a transverse magnetic field reveal rapid (<5 ps) spin transfer from excitons to Mn(2+) followed by coherent EMP precession at the Mn(2+) Larmor frequency for over a nanosecond. A dynamical TRFR phase inversion is observed during EMP formation attributed to the large shifts in excitonic absorption energies during spontaneous magnetization. Partial optical orientation of the EMPs by resonant circularly polarized photoexcitation is also demonstrated. Collectively, these results highlight the extraordinary physical properties of colloidal diffusion-doped Cd(1-x)Mn(x)Se QDs that result from their unique combination of strong quantum confinement, large Mn(2+) concentrations, and relatively narrow size distributions. The insights gained from these measurements advance our understanding of spin dynamics and magnetic exchange in colloidal doped semiconductor nanostructures, with potential ramifications for future spin-based information technologies.

Modification of quantum dots with nucleic acids

NASA Astrophysics Data System (ADS)

Kocherginskaya, P. B.; Romanova, A. V.; Prokhorenko, I. A.; Itkis, Daniil M.; Korshun, V. A.; Goodilin, Eugene A.; Tretyakov, Yuri D.

2011-12-01

The key principles and modern approaches to targeted modification of semiconductor colloidal nanoparticles, quantum dots, which exhibit unique photophysical properties and are a promising class of luminescent markers, are discussed. Attention is given to the preparation of their bioconjugates with nucleic acids, promising tools for biological microchips and resonance energy transfer sensors. The bibliography includes 80 references.

Study of the Spectral Properties of Nanocomposites with CdSe Quantum Dots in a Wide Range of Low Temperatures

NASA Astrophysics Data System (ADS)

Magaryan, K. A.; Eremchev, I. Y.; Karimullin, K. R.; Knyazev, M. V.; Mikhailov, M. A.; Vasilieva, I. A.; Klimusheva, G. V.

2015-09-01

Luminescence spectra of the colloidal solution of CdSe quantum dots (in toluene) were studied in a wide range of low temperatures. Samples were synthesized in the liquid crystal matrix of cadmium octanoate (CdC8). A comparative analysis of the obtained data with previous results was performed.

Novel one-step route for synthesizing CdS/polystyrene nanocomposite hollow spheres.

PubMed

Wu, Dazhen; Ge, Xuewu; Zhang, Zhicheng; Wang, Mozhen; Zhang, Songlin

2004-06-22

CdS/polystyrene nanocomposite hollow spheres with diameters between 240 and 500 nm were synthesized under ambient conditions by a novel microemulsion method in which the polymerization of styrene and the formation of CdS nanoparticles were initiated by gamma-irradiation. The product was characterized by transmission electron microscopy (TEM), field-emission scanning electron microscopy (FESEM), X-ray powder diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, and thermogravimetric analysis (TGA), which show the walls of the hollow spheres are porous and composed of polystyrene containing homogeneously dispersed CdS nanoparticles. The quantum-confined effect of the CdS/polystyrene nanocomposite hollow spheres is confirmed by the ultraviolet-visible (UV-vis) and photoluminescent (PL) spectra. We propose that the walls of these nanocomposite hollow spheres originate from the simultaneous synthesis of polystyrene and CdS nanoparticles at the interface of microemulsion droplets. This novel method is expected to produce various inorganic/polymer nanocomposite hollow spheres with potential applications in the fields of materials science and biotechnology.

Synthesis and characterization of CdS/PVA nanocomposite films

NASA Astrophysics Data System (ADS)

Wang, Hongmei; Fang, Pengfei; Chen, Zhe; Wang, Shaojie

2007-08-01

A series CdS/PVA nanocomposite films with different amount of Cd salt have been prepared by means of the in situ synthesis method via the reaction of Cd 2+-dispersed poly vinyl-alcohol (PVA) with H 2S. The as-prepared films were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), ultraviolet-visible (UV-vis) absorption, photoluminescence (PL) spectra, Fourier transform infrared spectroscope (FTIR) and thermogravimetric analysis (TGA). The XRD results indicated the formation of CdS nanoparticles with hexagonal phase in the PVA matrix. The primary FTIR spectra of CdS/PVA nanocomposite in different processing stages have been discussed. The vibrational absorption peak of Cd sbnd S bond at 405 cm -1 was observed, which further testified the generation of CdS nanoparticles. The TGA results showed incorporation of CdS nanoparticles significantly altered the thermal properties of PVA matrix. The photoluminescence and UV-vis spectroscopy revealed that the CdS/PVA films showed quantum confinement effect.

Phosphorene Co-catalyst Advancing Highly Efficient Visible-Light Photocatalytic Hydrogen Production.

PubMed

Ran, Jingrun; Zhu, Bicheng; Qiao, Shi-Zhang

2017-08-21

Transitional metals are widely used as co-catalysts boosting photocatalytic H 2 production. However, metal-based co-catalysts suffer from high cost, limited abundance and detrimental environment impact. To date, metal-free co-catalyst is rarely reported. Here we for the first time utilized density functional calculations to guide the application of phosphorene as a high-efficiency metal-free co-catalyst for CdS, Zn 0.8 Cd 0.2 S or ZnS. Particularly, phosphorene modified CdS shows a high apparent quantum yield of 34.7 % at 420 nm. This outstanding activity arises from the strong electronic coupling between phosphorene and CdS, as well as the favorable band structure, high charge mobility and massive active sites of phosphorene, supported by computations and advanced characterizations, for example, synchrotron-based X-ray absorption near edge spectroscopy. This work brings new opportunities to prepare highly-active, cheap and green photocatalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis and Characterization of Aqueous Lead Selenide Quantum Dots for Solar Cell Application

NASA Astrophysics Data System (ADS)

Albert, Ancy; Sreekala, C. O.; Prabhakaran, Malini

2018-02-01

High quality, colloidal lead selenide (PbSe) nanoparticles possessing cube shaped morphology have been successfully synthesized by organometallic synthesis method, using oleic acid (OA) as capping agent. The use of non-coordinating solvent, 1-Octadecene (ODE), during the synthesis results in good quality nanocrystals. Morphology analysis by transmission electron microscopy reveals that cube-shaped nanocrystals with a size range of 10 nm have been produced during the synthesis. The absorption and PL spectra analysis showed an emission peak at 675 nm when excited to a wavelength of 610 nm, further confirmed the formation of PbSe nanocrystals. The surface modification of this colloidal quantum dots was then carried out using L- cysteine ligand, to make them water soluble, for solar cell application. The J-V characteristics study of this PbSe quantum dots solar cell (PbSe QDSC) showed a little power conversion efficiency which intern it shows significant advance toward effective utilization of PbSe nanocrystals sensitized in solar cells.

Understanding chemically processed solar cells based on quantum dots

NASA Astrophysics Data System (ADS)

Malgras, Victor; Nattestad, Andrew; Kim, Jung Ho; Dou, Shi Xue; Yamauchi, Yusuke

2017-12-01

Photovoltaic energy conversion is one of the best alternatives to fossil fuel combustion. Petroleum resources are now close to depletion and their combustion is known to be responsible for the release of a considerable amount of greenhouse gases and carcinogenic airborne particles. Novel third-generation solar cells include a vast range of device designs and materials aiming to overcome the factors limiting the current technologies. Among them, quantum dot-based devices showed promising potential both as sensitizers and as colloidal nanoparticle films. A good example is the p-type PbS colloidal quantum dots (CQDs) forming a heterojunction with a n-type wide-band-gap semiconductor such as TiO2 or ZnO. The confinement in these nanostructures is also expected to result in marginal mechanisms, such as the collection of hot carriers and generation of multiple excitons, which would increase the theoretical conversion efficiency limit. Ultimately, this technology could also lead to the assembly of a tandem-type cell with CQD films absorbing in different regions of the solar spectrum.

Understanding chemically processed solar cells based on quantum dots.

PubMed

Malgras, Victor; Nattestad, Andrew; Kim, Jung Ho; Dou, Shi Xue; Yamauchi, Yusuke

2017-01-01

Photovoltaic energy conversion is one of the best alternatives to fossil fuel combustion. Petroleum resources are now close to depletion and their combustion is known to be responsible for the release of a considerable amount of greenhouse gases and carcinogenic airborne particles. Novel third-generation solar cells include a vast range of device designs and materials aiming to overcome the factors limiting the current technologies. Among them, quantum dot-based devices showed promising potential both as sensitizers and as colloidal nanoparticle films. A good example is the p-type PbS colloidal quantum dots (CQDs) forming a heterojunction with a n-type wide-band-gap semiconductor such as TiO 2 or ZnO. The confinement in these nanostructures is also expected to result in marginal mechanisms, such as the collection of hot carriers and generation of multiple excitons, which would increase the theoretical conversion efficiency limit. Ultimately, this technology could also lead to the assembly of a tandem-type cell with CQD films absorbing in different regions of the solar spectrum.

A colloidal quantum dot photonic crystal phosphor: nanostructural engineering of the phosphor for enhanced color conversion.

PubMed

Min, Kyungtaek; Jung, Hyunho; Park, Yeonsang; Cho, Kyung-Sang; Roh, Young-Geun; Hwang, Sung Woo; Jeon, Heonsu

2017-06-29

Phosphors, long-known color-converting photonic agents, are gaining increasing attention owing to the interest in white LEDs and related applications. Conventional material-based approaches to phosphors focus on obtaining the desired absorption/emission wavelengths and/or improving quantum efficiency. Here, we report a novel approach for enhancing the performance of phosphors: structural modification of phosphors. We incorporated inorganic colloidal quantum dots (CQDs) into a lateral one-dimensional (1D) photonic crystal (PhC) thin-film structure, with its photonic band-edge (PBE) modes matching the energy of 'excitation photons' (rather than 'emitted photons', as in most other PBE application devices). At resonance, we observed an approximately 4-fold enhancement of fluorescence over the reference bulk phosphor, which reflects an improved absorption of the excitation photons. This nano-structural engineering approach is a paradigm shift in the phosphor research area and may help to develop next-generation higher efficiency phosphors with novel characteristics.

Los Alamos Quantum Dots for Solar, Display Technology

ScienceCinema

Klimov, Victor

2018-05-01

Quantum dots are ultra-small bits of semiconductor matter that can be synthesized with nearly atomic precision via modern methods of colloidal chemistry. Their emission color can be tuned by simply varying their dimensions. Color tunability is combined with high emission efficiencies approaching 100 percent. These properties have recently become the basis of a new technology – quantum dot displays – employed, for example, in the newest generation of e-readers and video monitors.

Quantum Confined Semiconductors

DTIC Science & Technology

2015-02-01

diodes [8-10], metamaterials [11-13], and solar cells [14,15]. As a consequence, the optical and electrical stability of colloidal quantum dots...PbS quantum dot solar cells with high fill factor,” ACS Nano, 4 (7), 3743–3752 (2010). [15] Gur, I., Fromer, N. A., Geier, M. L. and Alivisatos, A...P., “Air-stable all-inorganic nanocrystal solar cells processed from solution,” Sci. 310, 462–465 (2005). [16] Dai, Q., Wang, Y. N., Zhang, Y

CdTe and CdSe quantum dots: synthesis, characterizations and applications in agriculture

NASA Astrophysics Data System (ADS)

Dieu Thuy Ung, Thi; Tran, Thi Kim Chi; Nga Pham, Thu; Nghia Nguyen, Duc; Khang Dinh, Duy; Liem Nguyen, Quang

2012-12-01

This paper highlights the results of the whole work including the synthesis of highly luminescent quantum dots (QDs), characterizations and testing applications of them in different kinds of sensors. Concretely, it presents: (i) the successful synthesis of colloidal CdTe and CdSe QDs, their core/shell structures with single- and/or double-shell made by CdS, ZnS or ZnSe/ZnS; (ii) morphology, structural and optical characterizations of the synthesized QDs; and (iii) testing examples of QDs as the fluorescence labels for agricultural-bio-medical objects (for tracing residual pesticide in agricultural products, residual clenbuterol in meat/milk and for detection of H5N1 avian influenza virus in breeding farms). Overall, the results show that the synthesized QDs have very good crystallinity, spherical shape and strongly emit at the desired wavelengths between ˜500 and 700 nm with the luminescence quantum yield (LQY) of 30-85%. These synthesized QDs were used in fabrication of the three testing fluorescence QD-based sensors for the detection of residual pesticides, clenbuterol and H5N1 avian influenza virus. The specific detection of parathion methyl (PM) pesticide at a content as low as 0.05 ppm has been realized with the biosensors made from CdTe/CdS and CdSe/ZnSe/ZnS QDs and the acetylcholinesterase (AChE) enzymes. Fluorescence resonance energy transfer (FRET)-based nanosensors using CdTe/CdS QDs conjugated with 2-amino-8-naphthol-6-sulfonic acid were fabricated that enable detection of diazotized clenbuterol at a content as low as 10 pg ml-1. For detection of H5N1 avian influenza virus, fluorescence biosensors using CdTe/CdS QDs bound on the surface of chromatophores extracted and purified from bacteria Rhodospirillum rubrum were prepared and characterized. The specific detection of H5N1 avian influenza virus in the range of 3-50 ng μl-1 with a detection limit of 3 ng μL-1 has been performed based on the antibody-antigen recognition.

Förster resonance energy transfer in hybrid associates of colloidal Ag2S quantum dots with thionine molecules

NASA Astrophysics Data System (ADS)

Ovchinnikov, Oleg V.; Smirnov, Mikhail S.; Kondratenko, Tamara S.; Ambrosevich, Sergey A.; Metlin, Mikhail T.; Grevtseva, Irina G.; Perepelitsa, Aleksey S.

2017-12-01

Nonradiative resonance energy transfer in hydrophilic hybrid associates of thionine molecules (TH+) with colloidal Ag2S quantum dots (QDs) with average diameter of 3.5 nm was studied. Photoluminescence spectra and its decay shown that for these systems the supplemental photosensitization of recombination luminescence of Ag2S QDs (1200 nm) from the region of TH+ fluorescence (618 nm) is possible. It was found that the average lifetime of TH+ molecules luminescence is shortened during their association with Ag2S QDs. Approximation of luminescence decay by stretched exponent with value of parameter β = 0.5 indicates on the inductive-resonance dipole-dipole (Förster) mechanism of nonradiative energy transfer (FRET). The efficiency of FRET was 0.29-0.41.

Nanotechnology: Colourful Particles for Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anheier, Norman C.

2015-07-01

In 1857 Michael Faraday gave a well-attended lecture at the Royal Institution of Great Britain, in which he presented his pioneering experimental work that investigated the interaction of light with matter. Faraday’s study probed the fundamental properties of light as it was reflected and absorbed by progressively smaller particles. Very fine gold particles dispersed in liquid were shown to produce vivid colors not seen in larger particles. Faraday did not know he had created colloidal suspensions of quantum dots, but his insight correctly concluded that the distinct colors were somehow due to the minute size of the gold particles. Thismore » great experimental physicist had actually glimpsed a special condition where the particle’s quantum nature was expressed. This work set the future course for nanoscience and quantum theory, but it would take another 125 years before the physical basis of this phenomenon would be explained by quantum size effects. It is now known that when quantum dots are exposed to UV light, some of the electrons are excited as they gain energy, however they remain confined to discrete energy levels not observed in larger particles and solid materials. When the electrons relax and lose their energy, the quantum dot emits light at a specific color that varies with the size of the quantum dot. Bao and Bawendi have cleverly exploited the unique optical properties intrinsic to colloidal quantum dots to develop an innovative compact optical spectrometer that could be integrated with a smart phone camera or as a versatile miniature handheld sensing tool.« less

In Situ Enzymatically Generated Photoswitchable Oxidase Mimetics and Their Application for Colorimetric Detection of Glucose Oxidase.

PubMed

Cao, Gen-Xia; Wu, Xiu-Ming; Dong, Yu-Ming; Li, Zai-Jun; Wang, Guang-Li

2016-07-09

In this study, a simple and amplified colorimetric assay is developed for the detection of the enzymatic activity of glucose oxidase (GOx) based on in situ formation of a photoswitchable oxidase mimetic of PO₄(3-)-capped CdS quantum dots (QDs). GOx catalyzes the oxidation of 1-thio-β-d-glucose to give 1-thio-β-d-gluconic acid which spontaneously hydrolyzes to β-d-gluconic acid and H₂S; the generated H₂S instantly reacts with Cd(2+) in the presence of Na₃PO₄ to give PO₄(3-)-stabilized CdS QDs in situ. Under visible-light (λ ≥ 400 nm) stimulation, the PO₄(3-)-capped CdS QDs are a new style of oxidase mimic derived by producing some active species, such as h⁺, (•)OH, O₂(•-) and a little H₂O₂, which can oxidize the typical substrate (3,3,5,5-tetramethylbenzydine (TMB)) with a color change. Based on the GOx-triggered growth of the oxidase mimetics of PO₄(3-)-capped CdS QDs in situ, we developed a simple and amplified colorimetric assay to probe the enzymatic activity of GOx. The proposed method allowed the detection of the enzymatic activity of GOx over the range from 25 μg/L to 50 mg/L with a low detection limit of 6.6 μg/L. We believe the PO₄(3-)-capped CdS QDs generated in situ with photo-stimulated enzyme-mimicking activity may find wide potential applications in biosensors.

Carbon dots for fluorescent detection of α-glucosidase activity using enzyme activated inner filter effect and its application to anti-diabetic drug discovery.

PubMed

Kong, Weiheng; Wu, Di; Xia, Lian; Chen, Xuefeng; Li, Guoliang; Qiu, Nannan; Chen, Guang; Sun, Zhiwei; You, Jinmao; Wu, Yongning

2017-06-22

Recently, α-glucosidase inhibitor has been widely used in clinic for diabetic therapy. In the present study, a facile and sensitive fluorescent assay based on enzyme activated inner filter effect (IFE) on nitrogen-doped carbon dots (CDs) was first developed for the detection of α-glucosidase. The N-doped CDs with green emission were prepared by a one-step hydrothermal synthesis and gave the fluorescence quantum yield of 30%, which were used as the signal output. Through α-glucosidase catalysis, 4-nitrophenol was released from 4-nitrophenyl-α-d-glucopyranoside (NGP). Interestingly, the absorption of 4-nitrophenol and the excitation of CDs were completely overlapping. Due to its great molar absorptivity, 4-nitrophenol was capable of acting as a powerful absorber to affect the fluorescent signal of CDs (i.e. IFE). By converting the absorption signals into fluorescence signals, the facile fluorescence assay strategy could be realized for α-glucosidase activity sensing, which effectively avoided the complex modification of the surface of CDs or construction of the nanoprobes. The established IFE-based sensing platform offered a low detection limit of 0.01 U/mL (S/N = 3). This proposed sensing approach has also been expanded to the inhibitor screening and showed excellent applicability. As a typical α-glucosidase inhibitor, acarbose was investigated with a low detection limit of 10 -8  M. This developed method enjoyed many merits including simplicity, lost cost, high sensitivity, good reproducibility and excellent selectivity, which also provided a new insight on the application of CDs to develop the facile and sensitive biosensor. Copyright © 2017 Elsevier B.V. All rights reserved.

Optical properties of DNA induced starch capped PbS, CdS and PbS/CdS nanocomposites

NASA Astrophysics Data System (ADS)

Das, D.; Konwar, R.; Kalita, P. K.

2015-08-01

Starch capped PbS, CdS and PbS-CdS nanocomposites are conjugated with Calf-Thymus DNA. All the materials are characterized by X-ray diffraction, high-resolution transmission electron microscopy, UV-Vis spectroscopy and photoluminescence spectroscopy. The x-ray diffraction patterns of PbS and CdS show that the materials possess polycrystalline having both cubic and hexagonal phases. High resolution transmission electron microscopic results (HRTEM) shows PbS nanoparticles of size 3 nm and that of CdS nanoparticles having average size 4 nm which exhibit tendency of agglomeration. In case of PbS/CdS, it exhibits different types of nanosheets. The UV absorption spectra of all the samples exhibit clear blue-shift with the respective bulk absorption edges. This is attributed to the strong quantum confinement in the materials. The absorption spectra also exhibit increase of the band gaps from 2.25 to 4.35 eV for PbS; 2.25-4.2 eV for CdS with decrease of molarities from 0.1 to 0.001 M as well as conjugated with DNA. The photoluminescence spectra of all PbS, CdS and PbS/CdS composites synthesized at 0.1 M molar concentration show a further blue shift and an enhancement of intensity after conjugation with DNA, but the effect is reversed i.e. occurrence of red shift and reduction of intensity for those having 0.01 M. This is due to the two competing processes of surface passivation as well as stabilization of nanocomposites governed by bio-molecules and that of Dexter energy transfer with the effective charge separation. The result shows the applicability of the materials in development of biological labels and biosensors.

Nearly Blinking-Free, High-Purity Single-Photon Emission by Colloidal InP/ZnSe Quantum Dots.

PubMed

Chandrasekaran, Vigneshwaran; Tessier, Mickaël D; Dupont, Dorian; Geiregat, Pieter; Hens, Zeger; Brainis, Edouard

2017-10-11

Colloidal core/shell InP/ZnSe quantum dots (QDs), recently produced using an improved synthesis method, have a great potential in life-science applications as well as in integrated quantum photonics and quantum information processing as single-photon emitters. Single-particle spectroscopy of 10 nm QDs with 3.2 nm cores reveals strong photon antibunching attributed to fast (70 ps) Auger recombination of multiple excitons. The QDs exhibit very good photostability under strong optical excitation. We demonstrate that the antibunching is preserved when the QDs are excited above the saturation intensity of the fundamental-exciton transition. This result paves the way toward their usage as high-purity on-demand single-photon emitters at room temperature. Unconventionally, despite the strong Auger blockade mechanism, InP/ZnSe QDs also display very little luminescence intermittency ("blinking"), with a simple on/off blinking pattern. The analysis of single-particle luminescence statistics places these InP/ZnSe QDs in the class of nearly blinking-free QDs, with emission stability comparable to state-of-the-art thick-shell and alloyed-interface CdSe/CdS, but with improved single-photon purity.

Understanding and Curing Structural Defects in Colloidal GaAs Nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Srivastava, Vishwas; Liu, Wenyong; Janke, Eric M.

2017-02-22

Nearly three decades since the first report on the synthesis of colloidal GaAs nanocrystals (NCs), the preparation and properties of this material remain highly controversial. Traditional synthetic routes either fail to produce the GaAs phase or result in materials that do not show expected optical properties such as excitonic transitions. In this work, we demonstrate a variety of synthetic routes toward crystalline GaAs NCs. By using a combination of Raman, EXAFS and transient absorption spectroscopies, we conclude that unusual optical properties of 2 colloidal GaAs NCs can be related to the presence of vacancies and lattice disorder. We introduce novelmore » molten salt based annealing approach to alleviate these structural defects and show the emergence of size-dependent excitonic transitions in colloidal GaAs quantum dots.« less

A dual spectroscopic fluorescence probe based on carbon dots for detection of 2,4,6-trinitrophenol/Fe (III) ion by fluorescence and frequency doubling scattering spectra and its analytical applications.

PubMed

Xu, Jinxia; Bai, Zhangjun; Zu, Fanlin; Yan, Fanyong; Wei, Junfu; Zhang, Saihui; Luo, Yunmei

2018-07-05

A convenient, highly sensitive and reliable assay for 2,4,6‑trinitrophenol (TNP) and Fe (III) ion (Fe 3+ ) in the dual spectroscopic manner is developed based on novel carbon dots (CDs). The CDs with highly blue emitting fluorescent were easily prepared via the one-step potassium hydroxide-assisted reflux method from dextrin. The as-synthesized CDs exhibited the high crystalline quality, the excellent fluorescence characteristics with a high quantum yield of ~13.1%, and the narrow size distribution with an average diameter of 6.3±0.5nm. Fluorescence and frequency doubling scattering (FDS) spectra of CDs show the unique changes in the presence of TNP/Fe 3+ by different mechanism. The fluorescence of CDs decreased apparently in the presence of TNP via electron-transfer. Thus, after the experimental conditions were optimized, the linear range for detection TNP is 0-50μM, the detection limit was 19.1nM. With the addition of Fe 3+ , the FDS of CDs appeared to be highly sensitive with a quick response to Fe 3+ as a result of the change concentration of the scattering particle. The emission peak for FDS at 450nm was enhanced under the excitation wavelength at 900nm. The fluorescence response changes linearly with Fe 3+ concentration in the range of 8-40μM, the detection limits were determined to be 44.1nM. The applications of CDs were extended for the detection of TNP, Fe 3+ in real water samples with a high recovery. The results reported here may become the potential tools for the fast response of TNP and Fe 3+ in the analysis of environmental pollutants. Copyright © 2018 Elsevier B.V. All rights reserved.

Evolution of oxygenated cadmium sulfide (CdS:O) during high-temperature CdTe solar cell fabrication

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meysing, Daniel M.; Reese, Matthew O.; Warren, Charles W.

Oxygenated cadmium sulfide (CdS:O) produced by reactive sputtering has emerged as a promising alternative to conventional CdS for use as the n-type window layer in CdTe solar cells. Here, complementary techniques are used to expose the window layer (CdS or CdS:O) in completed superstrate devices and combined with a suite of materials characterization to elucidate its evolution during high temperature device processing. During device fabrication amorphous CdS:O undergoes significant interdiffusion with CdTe and recrystallization, forming CdS1-yTey nanocrystals whose Te fraction approaches solubility limits. Significant oxygen remains after processing, concentrated in sulfate clusters dispersed among the CdS1-yTey alloy phase, accounting formore » ~30% of the post-processed window layer based on cross-sectional microscopy. Interdiffusion and recrystallization are observed in devices with un-oxygenated CdS, but to a much lesser extent. Etching experiments suggest that the CdS thickness is minimally changed during processing, but the CdS:O window layer is reduced from 100 nm to 60-80 nm, which is confirmed by microscopy. Alloying reduces the band gap of the CdS:O window layer to 2.15 eV, but reductions in thickness and areal density improve its transmission spectrum, which is well matched to device quantum efficiency. The changes to the window layer in the reactive environments of device fabrication are profoundly different than what occurs by thermal annealing in an inert environment, which produced films with a band gap of 2.4 eV for both CdS and CdS:O. These results illustrate for the first time the significant changes that occur to the window layer during processing that are critical to the performance of CdTe solar cells.« less

Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation

DOE PAGES

Wilker, Molly B.; Utterback, James K.; Greene, Sophie; ...

2017-12-08

Complexes of CdS nanorods and [FeFe] hydrogenase from Clostridium acetobutylicum have been shown to photochemically produce H 2. This study examines the role of the ligands that passivate the nanocrystal surfaces in the electron transfer from photoexcited CdS to hydrogenase and the H 2 generation that follows. We functionalized CdS nanorods with a series of mercaptocarboxylate surface-capping ligands of varying lengths and measured their photoexcited electron relaxation by transient absorption (TA) spectroscopy before and after hydrogenase adsorption. Rate constants for electron transfer from the nanocrystals to the enzyme, extracted by modeling of TA kinetics, decrease exponentially with ligand length, suggestingmore » that the ligand layer acts as a barrier to charge transfer and controls the degree of electronic coupling. Relative light-driven H 2 production efficiencies follow the relative quantum efficiencies of electron transfer, revealing the critical role of surface-capping ligands in determining the photochemical activity of these nanocrystal-enzyme complexes. Our results suggest that the H 2 production in this system could be maximized with a choice of a surface-capping ligand that decreases the distance between the nanocrystal surface and the electron injection site of the enzyme.« less

Ultrasensitive electrochemical detection of tumor cells based on multiple layer CdS quantum dots-functionalized polystyrene microspheres and graphene oxide - polyaniline composite.

PubMed

Wang, Jidong; Wang, Xiaoyu; Tang, Hengshan; Gao, Zehua; He, Shengquan; Li, Jian; Han, Shumin

2018-02-15

In this work, a novel ultrasensitive electrochemical biosensor was developed for the detection of K562 cell by a signal amplification strategy based on multiple layer CdS QDs functionalized polystyrene microspheres(PS) as bioprobe and graphene oxide(GO) -polyaniline(PANI) composite as modified materials of capture electrode. Due to electrostatic force of different charge, CdS QDs were decorated on the surface of PS by PDDA (poly(diallyldimethyl-ammonium chloride)) through a layer-by-layer(LBL) assemble technology, in which the structure of multiple layer CdS QDs increased the detection signal intensity. Moreover, GO-PANI composite not only enhanced the electron transfer rate, but also increased tumor cells load ratio. The resulting electrochemical biosensor was used to detect K562 cells with a lower detection limit of 3 cellsmL -1 (S/N = 3) and a wider linear range from 10 to 1.0 × 10 7 cellsmL -1 . This sensor was also used for mannosyl groups on HeLa cells and Hct116 cells, which showed high specificity and sensitivity. This signal amplification strategy would provide a novel approach for detection, diagnosis and treatment for tumor cells. Copyright © 2017 Elsevier B.V. All rights reserved.

Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilker, Molly B.; Utterback, James K.; Greene, Sophie

Complexes of CdS nanorods and [FeFe] hydrogenase from Clostridium acetobutylicum have been shown to photochemically produce H 2. This study examines the role of the ligands that passivate the nanocrystal surfaces in the electron transfer from photoexcited CdS to hydrogenase and the H 2 generation that follows. We functionalized CdS nanorods with a series of mercaptocarboxylate surface-capping ligands of varying lengths and measured their photoexcited electron relaxation by transient absorption (TA) spectroscopy before and after hydrogenase adsorption. Rate constants for electron transfer from the nanocrystals to the enzyme, extracted by modeling of TA kinetics, decrease exponentially with ligand length, suggestingmore » that the ligand layer acts as a barrier to charge transfer and controls the degree of electronic coupling. Relative light-driven H 2 production efficiencies follow the relative quantum efficiencies of electron transfer, revealing the critical role of surface-capping ligands in determining the photochemical activity of these nanocrystal-enzyme complexes. Our results suggest that the H 2 production in this system could be maximized with a choice of a surface-capping ligand that decreases the distance between the nanocrystal surface and the electron injection site of the enzyme.« less

ZnS, CdS and HgS nanoparticles via alkyl-phenyl dithiocarbamate complexes as single source precursors.

PubMed

Onwudiwe, Damian C; Ajibade, Peter A

2011-01-01

The synthesis of II-VI semiconductor nanoparticles obtained by the thermolysis of certain group 12 metal complexes as precursors is reported. Thermogravimetric analysis of the single source precursors showed sharp decomposition leading to their respective metal sulfides. The structural and optical properties of the prepared nanoparticles were characterized by means of X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) UV-Vis and photoluminescence spectroscopy. The X-ray diffraction pattern showed that the prepared ZnS nanoparticles have a cubic sphalerite structure; the CdS indicates a hexagonal phase and the HgS show the presence of metacinnabar phase. The TEM image demonstrates that the ZnS nanoparticles are dot-shaped, the CdS and the HgS clearly showed a rice and spherical morphology respectively. The UV-Vis spectra exhibited a blue-shift with respect to that of the bulk samples which is attributed to the quantum size effect. The band gap of the samples have been calculated from absorption spectra and werefound to be about 4.33 eV (286 nm), 2.91 eV (426 nm) and 4.27 eV (290 nm) for the ZnS, CdS and HgS samples respectively.

ZnS, CdS and HgS Nanoparticles via Alkyl-Phenyl Dithiocarbamate Complexes as Single Source Precursors

PubMed Central

Onwudiwe, Damian C.; Ajibade, Peter A.

2011-01-01

The synthesis of II-VI semiconductor nanoparticles obtained by the thermolysis of certain group 12 metal complexes as precursors is reported. Thermogravimetric analysis of the single source precursors showed sharp decomposition leading to their respective metal sulfides. The structural and optical properties of the prepared nanoparticles were characterized by means of X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) UV-Vis and photoluminescence spectroscopy. The X-ray diffraction pattern showed that the prepared ZnS nanoparticles have a cubic sphalerite structure; the CdS indicates a hexagonal phase and the HgS show the presence of metacinnabar phase. The TEM image demonstrates that the ZnS nanoparticles are dot-shaped, the CdS and the HgS clearly showed a rice and spherical morphology respectively. The UV-Vis spectra exhibited a blue-shift with respect to that of the bulk samples which is attributed to the quantum size effect. The band gap of the samples have been calculated from absorption spectra and werefound to be about 4.33 eV (286 nm), 2.91 eV (426 nm) and 4.27 eV (290 nm) for the ZnS, CdS and HgS samples respectively. PMID:22016607

Whispering gallery modes in photoluminescence and Raman spectra of a spherical microcavity with CdTe quantum dots: anti-Stokes emission and interference effects

PubMed Central

Gaponik, Nikolai; Gerlach, Matthias; Donegan, John F; Savateeva, Diana; Rogach, Andrey L

2006-01-01

We have studied the photoluminescence and Raman spectra of a system consisting of a polystyrene latex microsphere coated by CdTe colloidal quantum dots. The cavity-induced enhancement of the Raman scattering allows the observation of Raman spectra from only a monolayer of CdTe quantum dots. Periodic structure with very narrow peaks in the photoluminescence spectra of a single microsphere was detected both in the Stokes and anti-Stokes spectral regions, arising from the coupling between the emission of quantum dots and spherical cavity modes.

Quantum dots/silica/polymer nanocomposite films with high visible light transmission and UV shielding properties

NASA Astrophysics Data System (ADS)

Mumin, Md Abdul; Xu, William Z.; Charpentier, Paul A.

2015-08-01

The dispersion of light-absorbing inorganic nanomaterials in transparent plastics such as poly(ethylene-co-vinyl acetate) (PEVA) is of enormous current interest in emerging solar materials, including photovoltaic (PV) modules and commercial greenhouse films. Nanocrystalline semiconductor or quantum dots (QDs) have the potential to absorb UV light and selectively emit visible light, which can control plant growth in greenhouses or enhance PV panel efficiencies. This work provides a new and simple approach for loading mesoporous silica-encapsulated QDs into PEVA. Highly luminescent CdS and CdS-ZnS core-shell QDs with 5 nm size were synthesized using a modified facile approach based on pyrolysis of the single-molecule precursors and capping the CdS QDs with a thin layer of ZnS. To make both the bare and core-shell structure QDs more resistant against photochemical reactions, a mesoporous silica layer was grown on the QDs through a reverse microemulsion technique based on hydrophobic interactions. By careful experimental tuning, this encapsulation technique enhanced the quantum yield (˜65%) and photostability compared to the bare QDs. Both the encapsulated bare and core-shell QDs were then melt-mixed with EVA pellets using a mini twin-screw extruder and pressed into thin films with controlled thickness. The results demonstrated for the first time that mesoporous silica not only enhanced the quantum yield and photostability of the QDs but also improved the compatibility and dispersibility of QDs throughout the PEVA films. The novel light selective films show high visible light transmission (˜90%) and decreased UV transmission (˜75%).

Quantum dots/silica/polymer nanocomposite films with high visible light transmission and UV shielding properties.

PubMed

Mumin, Md Abdul; Xu, William Z; Charpentier, Paul A

2015-08-07

The dispersion of light-absorbing inorganic nanomaterials in transparent plastics such as poly(ethylene-co-vinyl acetate) (PEVA) is of enormous current interest in emerging solar materials, including photovoltaic (PV) modules and commercial greenhouse films. Nanocrystalline semiconductor or quantum dots (QDs) have the potential to absorb UV light and selectively emit visible light, which can control plant growth in greenhouses or enhance PV panel efficiencies. This work provides a new and simple approach for loading mesoporous silica-encapsulated QDs into PEVA. Highly luminescent CdS and CdS-ZnS core-shell QDs with 5 nm size were synthesized using a modified facile approach based on pyrolysis of the single-molecule precursors and capping the CdS QDs with a thin layer of ZnS. To make both the bare and core-shell structure QDs more resistant against photochemical reactions, a mesoporous silica layer was grown on the QDs through a reverse microemulsion technique based on hydrophobic interactions. By careful experimental tuning, this encapsulation technique enhanced the quantum yield (∼65%) and photostability compared to the bare QDs. Both the encapsulated bare and core-shell QDs were then melt-mixed with EVA pellets using a mini twin-screw extruder and pressed into thin films with controlled thickness. The results demonstrated for the first time that mesoporous silica not only enhanced the quantum yield and photostability of the QDs but also improved the compatibility and dispersibility of QDs throughout the PEVA films. The novel light selective films show high visible light transmission (∼90%) and decreased UV transmission (∼75%).

Study of the self-organization processes in lead sulfide quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tarasov, S. A., E-mail: SATarasov@mail.ru; Aleksandrova, O. A.; Maksimov, A. I.

A procedure is described for the synthesis of nanoparticles based on lead chalcogenides. The procedure combines the synthesis of colloidal quantum dots (QDs) in aqueous solutions with simultaneous organization of the QDs into ordered arrays. The processes of the self-organization of QDs are analyzed at the nano- and microscopic levels by the photoluminescence method, atomic-force microscopy, and optical microscopy.

Determination of the electronic energy levels of colloidal nanocrystals using field-effect transistors and Ab-initio calculations.

PubMed

Bisri, Satria Zulkarnaen; Degoli, Elena; Spallanzani, Nicola; Krishnan, Gopi; Kooi, Bart Jan; Ghica, Corneliu; Yarema, Maksym; Heiss, Wolfgang; Pulci, Olivia; Ossicini, Stefano; Loi, Maria Antonietta

2014-08-27

Colloidal nanocrystals electronic energy levels are determined by strong size-dependent quantum confinement. Understanding the configuration of the energy levels of nanocrystal superlattices is vital in order to use them in heterostructures with other materials. A powerful method is reported to determine the energy levels of PbS nanocrystal assemblies by combining the utilization of electric-double-layer-gated transistors and advanced ab-initio theory. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tuning light emission of PbS nanocrystals from infrared to visible range by cation exchange

PubMed Central

Binetti, Enrico; Striccoli, Marinella; Sibillano, Teresa; Giannini, Cinzia; Brescia, Rosaria; Falqui, Andrea; Comparelli, Roberto; Corricelli, Michela; Tommasi, Raffaele; Agostiano, Angela; Curri, M Lucia

2015-01-01

Colloidal semiconductor nanocrystals, with intense and sharp-line emission between red and near-infrared spectral regions, are of great interest for optoelectronic and bio-imaging applications. The growth of an inorganic passivation layer on nanocrystal surfaces is a common strategy to improve their chemical and optical stability and their photoluminescence quantum yield. In particular, cation exchange is a suitable approach for shell growth at the expense of the nanocrystal core size. Here, the cation exchange process is used to promote the formation of a CdS passivation layer on the surface of very small PbS nanocrystals (2.3 nm in diameter), blue shifting their optical spectra and yielding luminescent and stable nanostructures emitting in the range of 700–850 nm. Structural, morphological and compositional investigation confirms the nanocrystal size contraction after the cation-exchange process, while the PbS rock-salt crystalline phase is retained. Absorption and photoluminescence spectroscopy demonstrate the growth of a passivation layer with a decrease of the PbS core size, as inferred by the blue-shift of the excitonic peaks. The surface passivation strongly increases the photoluminescence intensity and the excited state lifetime. In addition, the nanocrystals reveal increased stability against oxidation over time. Thanks to their absorption and emission spectral range and the slow recombination dynamics, such highly luminescent nano-objects can find interesting applications in sensitized photovoltaic cells and light-emitting devices. PMID:27877842

A Colloidal-Quantum-Dot-Based Self-Charging System via the Near-Infrared Band.

PubMed

Baek, Se-Woong; Cho, Jungmin; Kim, Joo-Seong; Kim, Changjo; Na, Kwangmin; Lee, Sang-Hoon; Jun, Sunhong; Song, Jung Hoon; Jeong, Sohee; Choi, Jang Wook; Lee, Jung-Yong

2018-05-11

A novel self-charging platform is proposed using colloidal-quantum-dot (CQD) photovoltaics (PVs) via the near-infrared (NIR) band for low-power electronics. Low-bandgap CQDs can convert invisible NIR light sources to electrical energy more efficiently than wider spectra because of reduced thermalization loss. This energy-conversion strategy via NIR photons ensures an enhanced photostability of the CQD devices. Furthermore, the NIR wireless charging system can be concealed using various colored and NIR-transparent fabric or films, providing aesthetic freedom. Finally, an NIR-driven wireless charging system is demonstrated for a wearable healthcare bracelet by integrating a CQD PVs receiver with a flexible lithium-ion battery and entirely embedding them into a flexible strap, enabling permanent self-charging without detachment. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A differential dielectric spectroscopy setup to measure the electric dipole moment and net charge of colloidal quantum dots.

PubMed

Kortschot, R J; Bakelaar, I A; Erné, B H; Kuipers, B W M

2014-03-01

A sensitive dielectric spectroscopy setup is built to measure the response of nanoparticles dispersed in a liquid to an alternating electric field over a frequency range from 10(-2) to 10(7) Hz. The measured complex permittivity spectrum records both the rotational dynamics due to a permanent electric dipole moment and the translational dynamics due to net charges. The setup consists of a half-transparent capacitor connected in a bridge circuit, which is balanced on pure solvent only, using a software-controlled compensating voltage. In this way, the measured signal is dominated by the contributions of the nanoparticles rather than by the solvent. We demonstrate the performance of the setup with measurements on a dispersion of colloidal CdSe quantum dots in the apolar liquid decalin.

Building devices from colloidal quantum dots.

PubMed

Kagan, Cherie R; Lifshitz, Efrat; Sargent, Edward H; Talapin, Dmitri V

2016-08-26

The continued growth of mobile and interactive computing requires devices manufactured with low-cost processes, compatible with large-area and flexible form factors, and with additional functionality. We review recent advances in the design of electronic and optoelectronic devices that use colloidal semiconductor quantum dots (QDs). The properties of materials assembled of QDs may be tailored not only by the atomic composition but also by the size, shape, and surface functionalization of the individual QDs and by the communication among these QDs. The chemical and physical properties of QD surfaces and the interfaces in QD devices are of particular importance, and these enable the solution-based fabrication of low-cost, large-area, flexible, and functional devices. We discuss challenges that must be addressed in the move to solution-processed functional optoelectronic nanomaterials. Copyright © 2016, American Association for the Advancement of Science.

Electrophoretic properties of BSA-coated quantum dots.

PubMed

Bücking, Wendelin; Massadeh, Salam; Merkulov, Alexei; Xu, Shu; Nann, Thomas

2010-02-01

Low toxic InP/ZnS quantum dots (QDs), ZnS:Mn(2+)/ZnS nanocrystals and CdSe/ZnS nanoparticles were rendered water-dispersible by different ligand-exchange methods. Eventually, they were coated with bovine serum albumin (BSA) as a model protein. All particles were characterised by isotachophoresis (ITP), laser Doppler velocimetry (LDV) and agarose gel electrophoresis. It was found that the electrophoretic mobility and colloidal stability of ZnS:Mn(2+)/ZnS and CdSe/ZnS nanoparticles, which bore short-chain surface ligands, was primarily governed by charges on the nanoparticles, whereas InP/ZnS nanocrystals were not charged per se. BSA-coated nanoparticles showed lower electrophoretic mobility, which was attributed to their larger size and smaller overall charge. However, these particles were colloidally stable. This stability was probably caused by steric stabilisation of the BSA coating.

Statistical interpretation of transient current power-law decay in colloidal quantum dot arrays

NASA Astrophysics Data System (ADS)

Sibatov, R. T.

2011-08-01

A new statistical model of the charge transport in colloidal quantum dot arrays is proposed. It takes into account Coulomb blockade forbidding multiple occupancy of nanocrystals and the influence of energetic disorder of interdot space. The model explains power-law current transients and the presence of the memory effect. The fractional differential analogue of the Ohm law is found phenomenologically for nanocrystal arrays. The model combines ideas that were considered as conflicting by other authors: the Scher-Montroll idea about the power-law distribution of waiting times in localized states for disordered semiconductors is applied taking into account Coulomb blockade; Novikov's condition about the asymptotic power-law distribution of time intervals between successful current pulses in conduction channels is fulfilled; and the carrier injection blocking predicted by Ginger and Greenham (2000 J. Appl. Phys. 87 1361) takes place.

Application of DNA Aptamers and Quantum Dots to Lateral Flow Test Strips for Detection of Foodborne Pathogens with Improved Sensitivity versus Colloidal Gold

PubMed Central

Bruno, John G.

2014-01-01

Preliminary studies aimed at improving the sensitivity of foodborne pathogen detection via lateral flow (LF) test strips by use of high affinity DNA aptamers for capture and reporter functions when coupled to red-emitting quantum dots (Qdot 655) are reported. A variety of DNA aptamers developed against Escherichia coli, Listeria monocytogenes, and Salmonella enterica were paired in capture and reporter combinations to determine which yielded the strongest detection of their cognate bacteria using a colloidal gold screening system. Several promising sandwich combinations were identified for each of the three bacterial LF strip systems. The best E. coli aptamer-LF system was further studied and yielded a visible limit of detection (LOD) of ~3,000 E. coli 8739 and ~6,000 E. coli O157:H7 in buffer. These LODs were reduced to ~300–600 bacterial cells per test respectively by switching to a Qdot 655 aptamer-LF system. Novel aspects of these assays such as the use of high levels of detergents to avoid quantum dot agglutination and enhance migration in analytical membranes, identification of optimal analytical membrane types, UV-immobilization of capture aptamers, and novel dual biotin/digoxigenin-end labeled aptamer streptavidin-colloidal gold or -Qdot 655 conjugates plus anti-digoxigenin antibody control lines are also discussed. In general, this work provides proof-of-principle for highly sensitive aptamer-Qdot LF strip assays for rapid foodborne pathogen detection. PMID:25437803

Band-gap engineering by molecular mechanical strain-induced giant tuning of the luminescence in colloidal amorphous porous silicon nanostructures.

PubMed

Mughal, A; El Demellawi, J K; Chaieb, Sahraoui

2014-12-14

Nano-silicon is a nanostructured material in which quantum or spatial confinement is the origin of the material's luminescence. When nano-silicon is broken into colloidal crystalline nanoparticles, its luminescence can be tuned across the visible spectrum only when the sizes of the nanoparticles, which are obtained via painstaking filtration methods that are difficult to scale up because of low yield, vary. Bright and tunable colloidal amorphous porous silicon nanostructures have not yet been reported. In this letter, we report on a 100 nm modulation in the emission of freestanding colloidal amorphous porous silicon nanostructures via band-gap engineering. The mechanism responsible for this tunable modulation, which is independent of the size of the individual particles and their distribution, is the distortion of the molecular orbitals by a strained silicon-silicon bond angle. This mechanism is also responsible for the amorphous-to-crystalline transformation of silicon.

Hypervalent surface interactions for colloidal stability and doping of silicon nanocrystals

PubMed Central

Wheeler, Lance M.; Neale, Nathan R.; Chen, Ting; Kortshagen, Uwe R.

2013-01-01

Colloidal semiconductor nanocrystals have attracted attention for cost-effective, solution-based deposition of quantum-confined thin films for optoelectronics. However, two significant challenges must be addressed before practical nanocrystal-based devices can be realized. The first is coping with the ligands that terminate the nanocrystal surfaces. Though ligands provide the colloidal stability needed to cast thin films from solution, these ligands dramatically hinder charge carrier transport in the resulting film. Second, after a conductive film is achieved, doping has proven difficult for further control of the optoelectronic properties of the film. Here we report the ability to confront both of these challenges by exploiting the ability of silicon to engage in hypervalent interactions with hard donor molecules. For the first time, we demonstrate the significant potential of applying the interaction to the nanocrystal surface. In this study, hypervalent interactions are shown to provide colloidal stability as well as doping of silicon nanocrystals. PMID:23893292

High-resolution of particle contacts via fluorophore exclusion in deep-imaging of jammed colloidal packings

NASA Astrophysics Data System (ADS)

Kyeyune-Nyombi, Eru; Morone, Flaviano; Liu, Wenwei; Li, Shuiqing; Gilchrist, M. Lane; Makse, Hernán A.

2018-01-01

Understanding the structural properties of random packings of jammed colloids requires an unprecedented high-resolution determination of the contact network providing mechanical stability to the packing. Here, we address the determination of the contact network by a novel strategy based on fluorophore signal exclusion of quantum dot nanoparticles from the contact points. We use fluorescence labeling schemes on particles inspired by biology and biointerface science in conjunction with fluorophore exclusion at the contact region. The method provides high-resolution contact network data that allows us to measure structural properties of the colloidal packing near marginal stability. We determine scaling laws of force distributions, soft modes, correlation functions, coordination number and free volume that define the universality class of jammed colloidal packings and can be compared with theoretical predictions. The contact detection method opens up further experimental testing at the interface of jamming and glass physics.

Highly Luminescent Phase-Stable CsPbI3 Perovskite Quantum Dots Achieving Near 100% Absolute Photoluminescence Quantum Yield.

PubMed

Liu, Feng; Zhang, Yaohong; Ding, Chao; Kobayashi, Syuusuke; Izuishi, Takuya; Nakazawa, Naoki; Toyoda, Taro; Ohta, Tsuyoshi; Hayase, Shuzi; Minemoto, Takashi; Yoshino, Kenji; Dai, Songyuan; Shen, Qing

2017-10-24

Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems such as CdSe and PbS, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental nonradiative recombination centers and thus quenching luminescence. In this paper, we show that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI 3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine-PbI 2 (TOP-PbI 2 ) as the reactive precursor, which also leads to a significantly improved stability for the resulting CsPbI 3 QD solutions. Ultrafast kinetic analysis with time-resolved transient absorption spectroscopy evidence the negligible electron or hole-trapping pathways in our QDs, which explains such a high quantum efficiency. We expect the successful synthesis of the "ideal" perovskite QDs will exert profound influence on their applications to both QD-based light-harvesting and -emitting devices.

Role of Precursor-Conversion Chemistry in the Crystal-Phase Control of Catalytically Grown Colloidal Semiconductor Quantum Wires.

PubMed

Wang, Fudong; Buhro, William E

2017-12-26

Crystal-phase control is one of the most challenging problems in nanowire growth. We demonstrate that, in the solution-phase catalyzed growth of colloidal cadmium telluride (CdTe) quantum wires (QWs), the crystal phase can be controlled by manipulating the reaction chemistry of the Cd precursors and tri-n-octylphosphine telluride (TOPTe) to favor the production of either a CdTe solute or Te, which consequently determines the composition and (liquid or solid) state of the Bi x Cd y Te z catalyst nanoparticles. Growth of single-phase (e.g., wurtzite) QWs is achieved only from solid catalysts (y ≪ z) that enable the solution-solid-solid growth of the QWs, whereas the liquid catalysts (y ≈ z) fulfill the solution-liquid-solid growth of the polytypic QWs. Factors that affect the precursor-conversion chemistry are systematically accounted for, which are correlated with a kinetic study of the composition and state of the catalyst nanoparticles to understand the mechanism. This work reveals the role of the precursor-reaction chemistry in the crystal-phase control of catalytically grown colloidal QWs, opening the possibility of growing phase-pure QWs of other compositions.

Upconversion fluorescence tyrosine doped LaF3:Dy quantum dots useful in biolabeling and biotagging

NASA Astrophysics Data System (ADS)

Singh, Amit T.; Khandpekar, M. M.

2018-04-01

Water soluble hexahedral colloidal quantum dots (QDOTs) of Tyrosine doped LaF3:Dy have been synthesized by wet chemical route. The nanoparticles have been irradiated by microwave during synthesis for drying and also to reduce agglomeration. The coating of the LaF3:Dy nanoparticles by the amino acid tyrosine results in colloidal quantum dots. XRD studies indicates hexagonal lattice and confirms JCPDS data. The average particle size obtained by XRD and SEM are 22.89nm and 25.5nm respectively. The average sizes of nanorods obtained from TEM are 55 nm. The presence of elements has been verified with EDAX and ICP-AES technique. The SAED pattern of the samples shows sharp concentric rings indicating the crystalline nature of the synthesized nanoparticles. The FTIR spectra have been used to study the surface modification of the nanoparticles. The optical studies have been done using UV-visible and PL spectra. The PL spectra showed upconversion nature of the synthesized nanoparticles with sharp emission at 618 nm. The nanoparticles synthesized have potential application as biomaterials in bio imaging and biotagging.

Conformal fabrication of colloidal quantum dot solids for optically enhanced photovoltaics.

PubMed

Labelle, André J; Thon, Susanna M; Kim, Jin Young; Lan, Xinzheng; Zhitomirsky, David; Kemp, Kyle W; Sargent, Edward H

2015-05-26

Colloidal quantum dots (CQD) are an attractive thin-film material for photovoltaic applications due to low material costs, ease of fabrication, and size-tunable band gap. Unfortunately, today they suffer from a compromise between light absorption and photocarrier extraction, a fact that currently prevents the complete harvest of incoming above-band-gap solar photons. We have investigated the use of structured substrates and/or electrodes to increase the effective light path through the active material and found that these designs require highly conformal application of the light-absorbing films to achieve the greatest enhancement. This conformality requirement derives from the need for maximal absorption enhancement combined with shortest-distance charge transport. Here we report on a means of processing highly conformal layer-by-layer deposited CQD absorber films onto microstructured, light-recycling electrodes. Specifically, we engineer surface hydrophilicity to achieve conformal deposition of upper layers atop underlying ones. We show that only with the application of conformal coating can we achieve optimal quantum efficiency and enhanced power conversion efficiency in structured-electrode CQD cells.

Single-step colloidal quantum dot films for infrared solar harvesting

NASA Astrophysics Data System (ADS)

Kiani, Amirreza; Sutherland, Brandon R.; Kim, Younghoon; Ouellette, Olivier; Levina, Larissa; Walters, Grant; Dinh, Cao-Thang; Liu, Mengxia; Voznyy, Oleksandr; Lan, Xinzheng; Labelle, Andre J.; Ip, Alexander H.; Proppe, Andrew; Ahmed, Ghada H.; Mohammed, Omar F.; Hoogland, Sjoerd; Sargent, Edward H.

2016-10-01

Semiconductors with bandgaps in the near- to mid-infrared can harvest solar light that is otherwise wasted by conventional single-junction solar cell architectures. In particular, colloidal quantum dots (CQDs) are promising materials since they are cost-effective, processed from solution, and have a bandgap that can be tuned into the infrared (IR) via the quantum size effect. These characteristics enable them to harvest the infrared portion of the solar spectrum to which silicon is transparent. To date, IR CQD solar cells have been made using a wasteful and complex sequential layer-by-layer process. Here, we demonstrate ˜1 eV bandgap solar-harvesting CQD films deposited in a single step. By engineering a fast-drying solvent mixture for metal iodide-capped CQDs, we deposited active layers greater than 200 nm in thickness having a mean roughness less than 1 nm. We integrated these films into infrared solar cells that are stable in air and exhibit power conversion efficiencies of 3.5% under illumination by the full solar spectrum, and 0.4% through a simulated silicon solar cell filter.

Understanding chemically processed solar cells based on quantum dots

PubMed Central

Malgras, Victor; Nattestad, Andrew; Kim, Jung Ho; Dou, Shi Xue; Yamauchi, Yusuke

2017-01-01

Abstract Photovoltaic energy conversion is one of the best alternatives to fossil fuel combustion. Petroleum resources are now close to depletion and their combustion is known to be responsible for the release of a considerable amount of greenhouse gases and carcinogenic airborne particles. Novel third-generation solar cells include a vast range of device designs and materials aiming to overcome the factors limiting the current technologies. Among them, quantum dot-based devices showed promising potential both as sensitizers and as colloidal nanoparticle films. A good example is the p-type PbS colloidal quantum dots (CQDs) forming a heterojunction with a n-type wide-band-gap semiconductor such as TiO2 or ZnO. The confinement in these nanostructures is also expected to result in marginal mechanisms, such as the collection of hot carriers and generation of multiple excitons, which would increase the theoretical conversion efficiency limit. Ultimately, this technology could also lead to the assembly of a tandem-type cell with CQD films absorbing in different regions of the solar spectrum. PMID:28567179

Synthesis and Use of [Cd(Detu)2(OOCCH3)2]·H2O as Single Molecule Precursor for Cds Nanoparticles

PubMed Central

Ajibade, Peter A.

2013-01-01

Substituted thiourea ligands are of interest because they possess various donor sites for metal ions and their application in separation of metal ions and as antimicrobial agents. The coordination of the sulfur donor atom led to interest in them as precursor for semiconductor nanoparticles. In this study, cadmium(II) complex of diethylthiourea was synthesized and characterized by elemental analysis, FTIR, and X-ray crystallography. Single crystal X-ray structure of the complex showed that the octahedral geometry around the Cd ion consists of two molecules of diethylthiourea acting as monodentate ligands and two chelating acetate ions. The thermal decomposition of the compound showed that it decomposed to give CdS. The compound was thermolysed in hexadecylamine (HDA) to prepare HDA-capped CdS nanoparticles. The absorption spectrum showed blue shifts in its absorption band edges which clearly indicated quantum confinement effect, and the emission spectrum showed characteristic band edge luminescence. The broad diffraction peaks of the XRD pattern showed the materials to be of the nanometric size. PMID:24294141

Carbon dots in zeolites: A new class of thermally activated delayed fluorescence materials with ultralong lifetimes

PubMed Central

Liu, Jiancong; Wang, Ning; Yu, Yue; Yan, Yan; Zhang, Hongyue; Li, Jiyang; Yu, Jihong

2017-01-01

Thermally activated delayed fluorescence (TADF) materials are inspiring intensive research in optoelectronic applications. To date, most of the TADF materials are limited to metal-organic complexes and organic molecules with lifetimes of several microseconds/milliseconds that are sensitive to oxygen. We report a facial and general “dots-in-zeolites” strategy to in situ confine carbon dots (CDs) in zeolitic matrices during hydrothermal/solvothermal crystallization to generate high-efficient TADF materials with ultralong lifetimes. The resultant CDs@zeolite composites exhibit high quantum yields up to 52.14% and ultralong lifetimes up to 350 ms at ambient temperature and atmosphere. This intriguing TADF phenomenon is due to the fact that nanoconfined space of zeolites can efficiently stabilize the triplet states of CDs, thus enabling the reverse intersystem crossing process for TADF. Meanwhile, zeolite frameworks can also hinder oxygen quenching to present TADF behavior at air atmosphere. This design concept introduces a new perspective to develop materials with unique TADF performance and various novel delayed fluorescence–based applications. PMID:28560347

Nanoscale Interfaces in Colloidal Quantum Dot Solar Cells: Physical Insights and Materials Engineering Strategies

NASA Astrophysics Data System (ADS)

Kemp, Kyle Wayne

With growing global energy demand there will be an increased need for sources of renewable energy such as solar cells. To make these photovoltaic technologies more competitive with conventional energy sources such as coal and natural gas requires further reduction in manufacturing costs that can be realized by solution processing and roll-to-roll printing. Colloidal quantum dots are a bandgap tunable, solution processible, semiconductor material which may offer a path forward to efficient, inexpensive photovoltaics. Despite impressive progress in performance with these materials, there remain limitations in photocarrier collection that must be overcome. This dissertation focuses on the characterization of charge recombination and transport in colloidal quantum dot photovoltaics, and the application of this knowledge to the development of new and better materials. Core-shell, PbS-CdS, quantum dots were investigated in an attempt to achieve better surface passivation and reduce electronic defects which can limit performance. Optimization of this material led to improved open circuit voltage, exceeding 0.6 V for the first time, and record published performance of 6% efficiency. Using temperature-dependent and transient photovoltage measurements we explored the significance of interface recombination on the operation of these devices. Careful engineering of the electrode using atomic layer deposition of ZnO helped lead to better TiO2 substrate materials and allowed us to realize a nearly two-fold reduction in recombination rate and an enhancement upwards of 50 mV in open circuit voltage. Carrier extraction efficiency was studied in these devices using intensity dependent current-voltage data of an operational solar cell. By developing an analytical model to describe recombination loss within the active layer of the device we were able to accurately determine transport lengths ranging up to 90 nm. Transient absorption and photoconductivity techniques were used to study charge dynamics by identifying states in these quantum dot materials which facilitate carrier transport. Thermal activation energies for transport of 60 meV or lower were measured for different PbS quantum dot bandgaps, representing a relatively small barrier for carrier transport. From these measurements a dark, quantum confined energy level was attributed to the electronic bandedge of these materials which serves to govern their optoelectronic behavior.

Detection of CdSe quantum dot photoluminescence for security label on paper

DOE Office of Scientific and Technical Information (OSTI.GOV)

Isnaeni,, E-mail: isnaeni@lipi.go.id; Sugiarto, Iyon Titok; Bilqis, Ratu

CdSe quantum dot has great potential in various applications especially for emitting devices. One example potential application of CdSe quantum dot is security label for anti-counterfeiting. In this work, we present a practical approach of security label on paper using one and two colors of colloidal CdSe quantum dot, which is used as stamping ink on various types of paper. Under ambient condition, quantum dot is almost invisible. The quantum dot security label can be revealed by detecting emission of quantum dot using photoluminescence and cnc machine. The recorded quantum dot emission intensity is then analyzed using home-made program tomore » reveal quantum dot pattern stamp having the word ’RAHASIA’. We found that security label using quantum dot works well on several types of paper. The quantum dot patterns can survive several days and further treatment is required to protect the quantum dot. Oxidation of quantum dot that occurred during this experiment reduced the emission intensity of quantum dot patterns.« less

Overview of Stabilizing Ligands for Biocompatible Quantum Dot Nanocrystals

PubMed Central

Zhang, Yanjie; Clapp, Aaron

2011-01-01

Luminescent colloidal quantum dots (QDs) possess numerous advantages as fluorophores in biological applications. However, a principal challenge is how to retain the desirable optical properties of quantum dots in aqueous media while maintaining biocompatibility. Because QD photophysical properties are directly related to surface states, it is critical to control the surface chemistry that renders QDs biocompatible while maintaining electronic passivation. For more than a decade, investigators have used diverse strategies for altering the QD surface. This review summarizes the most successful approaches for preparing biocompatible QDs using various chemical ligands. PMID:22247651

Fluorescence enhancement by a dark plasmon mode

NASA Astrophysics Data System (ADS)

Peter, Manuel; Werra, Julia F. M.; Friesen, Cody; Achnitz, Doreen; Busch, Kurt; Linden, Stefan

2018-05-01

We investigate the fluorescence properties of colloidal quantum dots coupled to gold nanowire antennas. By varying the wire length, the plasmon modes of the nanoantennas are successively tuned through the emission band of the quantum dots. We observe a pronounced fluorescence enhancement both for short and long nanoantennas. These findings can be attributed to the coupling of the quantum dots to the bright dipole plasmon mode and the dark quadrupol plasmon mode, respectively. This interpretation is supported by numerical calculations of the far-field scattering spectra and the radiation rates.

Hybrid zinc oxide/graphene electrodes for depleted heterojunction colloidal quantum-dot solar cells.

PubMed

Tavakoli, Mohammad Mahdi; Aashuri, Hossein; Simchi, Abdolreza; Fan, Zhiyong

2015-10-07

Recently, hybrid nanocomposites consisting of graphene/nanomaterial heterostructures have emerged as promising candidates for the fabrication of optoelectronic devices. In this work, we have employed a facile and in situ solution-based process to prepare zinc oxide/graphene quantum dots (ZnO/G QDs) in a hybrid structure. The prepared hybrid dots are composed of a ZnO core, with an average size of 5 nm, warped with graphene nanosheets. Spectroscopic studies show that the graphene shell quenches the photoluminescence intensity of the ZnO nanocrystals by about 72%, primarily due to charge transfer reactions and static quenching. A red shift in the absorption peak is also observed. Raman spectroscopy determines G-band splitting of the graphene shell into two separated sub-bands (G(+), G(-)) caused by the strain induced symmetry breaking. It is shown that the hybrid ZnO/G QDs can be used as a counter-electrode for heterojunction colloidal quantum-dot solar cells for efficient charge-carrier collection, as evidenced by the external quantum efficiency measurement. Under the solar simulated spectrum (AM 1.5G), we report enhanced power conversion efficiency (35%) with higher short current circuit (80%) for lead sulfide-based solar cells as compared to devices prepared by pristine ZnO nanocrystals.

A High Power, Frequency Tunable Colloidal Quantum Dot (CdSe/ZnS) Laser

PubMed Central

Prasad, Saradh; Saleh AlHesseny, Hanan; AlSalhi, Mohamad S.; Devaraj, Durairaj; Masilamai, Vadivel

2017-01-01

Tunable lasers are essential for medical, engineering and basic science research studies. Most conventional solid-state lasers are capable of producing a few million laser shots, but limited to specific wavelengths, which are bulky and very expensive. Dye lasers are continuously tunable, but exhibit very poor chemical stability. As new tunable, efficient lasers are always in demand, one such laser is designed with various sized CdSe/ZnS quantum dots. They were used as a colloid in tetrahydrofuran to produce a fluorescent broadband emission from 520 nm to 630 nm. The second (532 nm) and/or third harmonic (355 nm) of the Nd:YAG laser (10 ns, 10 Hz) were used together as the pump source. In this study, different sized quantum dots were independently optically pumped to produce amplified spontaneous emission (ASE) with 4 nm to 7 nm of full width at half-maximum (FWHM), when the pump power and focusing were carefully optimized. The beam was directional with a 7 mrad divergence. Subsequently, these quantum dots were combined together, and the solution was placed in a resonator cavity to obtain a laser with a spectral width of 1 nm and tunable from 510 to 630 nm, with a conversion efficiency of about 0.1%. PMID:28336863

Measuring charge carrier diffusion in coupled colloidal quantum dot solids.

PubMed

Zhitomirsky, David; Voznyy, Oleksandr; Hoogland, Sjoerd; Sargent, Edward H

2013-06-25

Colloidal quantum dots (CQDs) are attractive materials for inexpensive, room-temperature-, and solution-processed optoelectronic devices. A high carrier diffusion length is desirable for many CQD device applications. In this work we develop two new experimental methods to investigate charge carrier diffusion in coupled CQD solids under charge-neutral, i.e., undepleted, conditions. The methods take advantage of the quantum-size-effect tunability of our materials, utilizing a smaller-bandgap population of quantum dots as a reporter system. We develop analytical models of diffusion in 1D and 3D structures that allow direct extraction of diffusion length from convenient parametric plots and purely optical measurements. We measure several CQD solids fabricated using a number of distinct methods and having significantly different doping and surface ligand treatments. We find that CQD materials recently reported to achieve a certified power conversion efficiency of 7% with hybrid organic-inorganic passivation have a diffusion length of 80 ± 10 nm. The model further allows us to extract the lifetime, trap density, mobility, and diffusion coefficient independently in each material system. This work will facilitate further progress in extending the diffusion length, ultimately leading to high-quality CQD solid semiconducting materials and improved CQD optoelectronic devices, including CQD solar cells.

A High Power, Frequency Tunable Colloidal Quantum Dot (CdSe/ZnS) Laser.

PubMed

Prasad, Saradh; AlHesseny, Hanan Saleh; AlSalhi, Mohamad S; Devaraj, Durairaj; Masilamai, Vadivel

2017-01-30

Tunable lasers are essential for medical, engineering and basic science research studies. Most conventional solid-state lasers are capable of producing a few million laser shots, but limited to specific wavelengths, which are bulky and very expensive. Dye lasers are continuously tunable, but exhibit very poor chemical stability. As new tunable, efficient lasers are always in demand, one such laser is designed with various sized CdSe/ZnS quantum dots. They were used as a colloid in tetrahydrofuran to produce a fluorescent broadband emission from 520 nm to 630 nm. The second (532 nm) and/or third harmonic (355 nm) of the Nd:YAG laser (10 ns, 10 Hz) were used together as the pump source. In this study, different sized quantum dots were independently optically pumped to produce amplified spontaneous emission (ASE) with 4 nm to 7 nm of full width at half-maximum (FWHM), when the pump power and focusing were carefully optimized. The beam was directional with a 7 mrad divergence. Subsequently, these quantum dots were combined together, and the solution was placed in a resonator cavity to obtain a laser with a spectral width of 1 nm and tunable from 510 to 630 nm, with a conversion efficiency of about 0.1%.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mumin, Md Abdul, E-mail: pcharpentier@eng.uwo.ca; Akhter, Kazi Farida, E-mail: pcharpentier@eng.uwo.ca; Charpentier, Paul A., E-mail: pcharpentier@eng.uwo.ca

Semiconductor nanocrystals (NCs) (also known as quantum dots, QDs) have attracted immense attention for their size-tunable optical properties that makes them impressive candidates for solar cells, light emitting devices, lasers, as well as biomedical imaging. However monodispersity, high and consistent photoluminescence, photostability, and biocompatibility are still major challenges. This work focuses on optimizing the photophysical properties and biocompatibility of QDs by forming core-shell nanostructures and their encapsulation by a carrier. Highly luminescent CdS and CdS-ZnS core-shell QDs with 5 nm sizes were synthesized using a facile approach based on pyrolysis of the single molecule precursors. After capping the CdS QDsmore » with a thin layer of ZnS to reduce toxicity, the photoluminescence and photostability of the core-shell QDs was significantly enhanced. To make both the bare and core/shell structure QDs more resistant against photochemical reactions, a mesoporous silica layer was grown on the QDs through a reverse microemulsion technique based on hydrophobic interaction. This encapsulation enhanced the quantum yield and photostability compared to the bare QDs by providing much stronger resistance to oxidation and Oswald ripening of QDs. Encapsulation also improved biocompatibility of QDs that was evaluated with human umbilical vein endothelial cell lines (HUVEC)« less

The Proteomic Response of Arabidopsis thaliana to Cadmium Sulfide Quantum Dots, and Its Correlation with the Transcriptomic Response

PubMed Central

Marmiroli, Marta; Imperiale, Davide; Pagano, Luca; Villani, Marco; Zappettini, Andrea; Marmiroli, Nelson

2015-01-01

A fuller understanding of the interaction between plants and engineered nanomaterials is of topical relevance because the latter are beginning to find applications in agriculture and the food industry. There is a growing need to establish objective safety criteria for their use. The recognition of two independent Arabidopsis thaliana mutants displaying a greater level of tolerance than the wild type plant to exposure to cadmium sulfide quantum dots (CdS QDs) has offered the opportunity to characterize the tolerance response at the physiological, transcriptomic, and proteomic levels. Here, a proteomics-based comparison confirmed the conclusions drawn from an earlier transcriptomic analysis that the two mutants responded to CdS QD exposure differently both to the wild type and to each other. Just over half of the proteomic changes mirrored documented changes at the level of gene transcription, but a substantial number of transcript/gene product pairs were altered in the opposite direction. An interpretation of the discrepancies is given, along with some considerations regarding the use and significance of -omics when monitoring the potential toxicity of ENMs for health and environment. PMID:26732871

Programmable Colloidal Approach to Hierarchical Structures of Methylammonium Lead Bromide Perovskite Nanocrystals with Bright Photoluminescent Properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Teunis, Meghan B.; Johnson, Merrell A.; Muhoberac, Barry B.

Here, systematic tailoring of nanocrystal architecture could provide unprecedented control over their electronic, photophysical, and charge transport properties for a variety of applications. However, at present, manipulation of the shape of perovskite nanocrystals is done mostly by trial-and-error-based experimental approaches. Here, we report systematic colloidal synthetic strategies to prepare methylammonium lead bromide quantum platelets and quantum cubes. In order to control the nucleation and growth processes of these nano crystals, we appropriately manipulate the solvent system, surface ligand chemistry, and reaction temperature causing syntheses into anisotropic shapes. We demonstrate that both the presence of chlorinated solvent and a long chainmore » aliphatic amine in the reaction mixture are crucial for the formation of ultrathin quantum platelets (similar to 1.5 nm in thickness), which is driven by mesoscale-assisted growth of spherical seed nanocrystals (similar to 1.6 nm in diameter) through attachment of monomers onto selective crystal facets. A combined surface and structural characterization, along with small-angle X-ray scattering analysis, confirm that the long hydrocarbon of the aliphatic amine is responsible for the well ordered hierarchical stacking of the quantum platelets of 3.5 nm separation. In contrast, the formation of similar to 12 nm edge-length quantum cubes is a kinetically driven process in which a high flux of monomers is achieved by supplying thermal energy. The photoluminescence quantum yield of our quantum platelets (similar to 52%) is nearly 2-fold higher than quantum cubes. Moreover, the quantum platelets display a lower nonradiative rate constant than that found with quantum cubes, which suggests less surface trap states. Together, our research has the potential both to improve the design of synthetic methods for programmable control of shape and assembly and to provide insight into optoelectronic properties of these materials for solid-state device fabrication, e.g., light-emitting diodes, solar cells, and lasing materials.« less

Programmable Colloidal Approach to Hierarchical Structures of Methylammonium Lead Bromide Perovskite Nanocrystals with Bright Photoluminescent Properties

DOE PAGES

Teunis, Meghan B.; Johnson, Merrell A.; Muhoberac, Barry B.; ...

2017-04-05

Here, systematic tailoring of nanocrystal architecture could provide unprecedented control over their electronic, photophysical, and charge transport properties for a variety of applications. However, at present, manipulation of the shape of perovskite nanocrystals is done mostly by trial-and-error-based experimental approaches. Here, we report systematic colloidal synthetic strategies to prepare methylammonium lead bromide quantum platelets and quantum cubes. In order to control the nucleation and growth processes of these nano crystals, we appropriately manipulate the solvent system, surface ligand chemistry, and reaction temperature causing syntheses into anisotropic shapes. We demonstrate that both the presence of chlorinated solvent and a long chainmore » aliphatic amine in the reaction mixture are crucial for the formation of ultrathin quantum platelets (similar to 1.5 nm in thickness), which is driven by mesoscale-assisted growth of spherical seed nanocrystals (similar to 1.6 nm in diameter) through attachment of monomers onto selective crystal facets. A combined surface and structural characterization, along with small-angle X-ray scattering analysis, confirm that the long hydrocarbon of the aliphatic amine is responsible for the well ordered hierarchical stacking of the quantum platelets of 3.5 nm separation. In contrast, the formation of similar to 12 nm edge-length quantum cubes is a kinetically driven process in which a high flux of monomers is achieved by supplying thermal energy. The photoluminescence quantum yield of our quantum platelets (similar to 52%) is nearly 2-fold higher than quantum cubes. Moreover, the quantum platelets display a lower nonradiative rate constant than that found with quantum cubes, which suggests less surface trap states. Together, our research has the potential both to improve the design of synthetic methods for programmable control of shape and assembly and to provide insight into optoelectronic properties of these materials for solid-state device fabrication, e.g., light-emitting diodes, solar cells, and lasing materials.« less

Temperature-assisted photochemical construction of CdS-based ordered porous films with photocatalytic activities on solution surfaces.

PubMed

Huang, Zhenxun; Sun, Fengqiang; Zhang, Yu; Gu, Kaiyuan; Zou, Xueqiong; Huang, Yuying; Wu, Qingsong; Zhang, Zihe

2011-04-15

Taking a colloidal monolayer floating on the surface of a precursor solution as template, free-standing CdS/Cd composites and pure CdS (CdS-based) ordered porous films had been prepared by a temperature-assisted photochemical strategy. After irradiation with UV-light and heat treatment, the films formed hemi-spherical pores due to the preferable deposition of CdS and Cd onto the PS spheres during the photochemical and interfacial reactions. When the temperature increased from 15 to 60°C, the air/water interface gradually changed into a vapor/water interface on the surface of the solution, resulting in variations of the final compositions. The optical properties of the films were hence changed. Because of the free-standing characteristic, the ordered porous films were first transferred on surface of polluted solutions as photocatalysts, which was a new mode in application of photocatalysts. The photocatalytic activities of films showed regular variations with the compositions in photodegradation of Rhodamine B. This method provides a simple route for tuning the properties of porous films through control of its composition and a flexible application of films on any surface. Copyright © 2011 Elsevier Inc. All rights reserved.

Preparation of manganese doped cadmium sulfide nanoparticles in zincblende phase and their magnetic properties.

PubMed

Nakaya, Masafumi; Tanaka, Itaru; Muramatsu, Atsushi

2012-12-01

In this study, the random dope of Mn into CdS nanoparticles in zincblende phase has been carried out under the mild reaction condition. The resulting nanoparticles were characterized by energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), X-ray diffractometer (XRD), UV-Vis spectrometer, PL spectrometer, and SQUID. EDX showed that the compositions of Mn doped CdS nanoparticles were readily controlled. TEM showed the particle sizes were not significantly affected by the compositions, retaining to be ca. 3 nm with a narrow size distribution. UV-Vis and PL spectra of the resulting nanoparticles showed the intra-Mn level may be affected by the quantum size effect. SQUID measurement showed that the resulting nanoparticles showed diamagnetism, paramagnetism and superparamagnetism dependent on Mn content.

Potentiometric Titrations for Measuring the Capacitance of Colloidal Photodoped ZnO Nanocrystals.

PubMed

Brozek, Carl K; Hartstein, Kimberly H; Gamelin, Daniel R

2016-08-24

Colloidal semiconductor nanocrystals offer a unique opportunity to bridge molecular and bulk semiconductor redox phenomena. Here, potentiometric titration is demonstrated as a method for quantifying the Fermi levels and charging potentials of free-standing colloidal n-type ZnO nanocrystals possessing between 0 and 20 conduction-band electrons per nanocrystal, corresponding to carrier densities between 0 and 1.2 × 10(20) cm(-3). Potentiometric titration of colloidal semiconductor nanocrystals has not been described previously, and little precedent exists for analogous potentiometric titration of any soluble reductants involving so many electrons. Linear changes in Fermi level vs charge-carrier density are observed for each ensemble of nanocrystals, with slopes that depend on the nanocrystal size. Analysis indicates that the ensemble nanocrystal capacitance is governed by classical surface electrical double layers, showing no evidence of quantum contributions. Systematic shifts in the Fermi level are also observed with specific changes in the identity of the charge-compensating countercation. As a simple and contactless alternative to more common thin-film-based voltammetric techniques, potentiometric titration offers a powerful new approach for quantifying the redox properties of colloidal semiconductor nanocrystals.

Optimization of the Photoanode of CdS Quantum Dot-Sensitized Solar Cells Using Light-Scattering TiO2 Hollow Spheres

NASA Astrophysics Data System (ADS)

Marandi, Maziar; Rahmani, Elham; Ahangarani Farahani, Farzaneh

2017-12-01

CdS quantum dot-sensitized solar cells (QDSCs) have been fabricated and their photoanode optimized by altering the thickness of the photoelectrode and CdS deposition conditions and applying a ZnS electron-blocking layer and TiO2 hollow spheres. Hydrothermally grown TiO2 nanocrystals (NCs) with dominant size of 20 nm were deposited as a sublayer in the photoanode with thickness in the range from 5 μm to 10 μm using a successive ionic layer adsorption and reaction (SILAR) method. The number of deposition cycles was altered over a wide range to obtain optimized sensitization. Photoanode thickness and number of CdS sensitization cycles around the optimum values were selected and used for ZnS deposition. ZnS overlayers were also deposited on the surface of the photoanodes using different numbers of cycles of the SILAR process. The best QDSC with the optimized photoelectrode demonstrated a 153% increase in efficiency compared with a similar cell with ZnS-free photoanode. Such bilayer photoelectrodes were also fabricated with different thicknesses of TiO2 sublayers and one overlayer of TiO2 hollow spheres (HSs) with external diameter of 500 nm fabricated by liquid-phase deposition with carbon spheres as template. The optimization was performed by changing the photoanode thickness using a wide range of CdS sensitizing cycles. The maximum energy conversion efficiency was increased by about 77% compared with a similar cell with HS-free photoelectrode. The reason was considered to be the longer path length of the incident light inside the photoanode and greater light absorption. A ZnS blocking layer was overcoated on the surface of the bilayer photoanode with optimized thickness. The number of CdS sensitization cycles was also changed around the optimized value to obtain the best QDSC performance. The number of ZnS deposition cycles was also altered in a wide range for optimization of the photovoltaic performance. It was shown that the maximum efficiency was increased by about 55% compared with a similar QDSC with ZnS-free bilayer photoanode. The final improvement was carried out by applying methanol-based Cd precursor solution in the SILAR deposition process. The best photoanodes from the previous stages were selected and used in this sensitizing process. Besides, nanocrystalline TiO2 sublayers with different thicknesses were applied for further optimization. The results revealed that maximum power conversion efficiency of 3.7% was achieved as a result of such improvement, for a QDSC with optimized double-layer photoanode including TiO2 HSs and NCs and ZnS blocking layer.

Enhanced photovoltaic performance of CdS-sensitized inverted organic solar cells prepared via a successive ionic layer adsorption and reaction method

NASA Astrophysics Data System (ADS)

Oleiwi, Hind Fadhil; Zakaria, Azmi; Yap, Chi Chin; Abbas, Haidr Abdulzahra; Tan, Sin Tee; Lee, Hock Beng; Tan, Chun Hui; Ginting, Riski Titian; Alshanableh, Abdelelah; Talib, Zainal Abidin

2017-05-01

One-dimensional ZnO nanorods (ZNRs) synthesized on fluorine-doped tin oxide (FTO) glass by hydrothermal method were modified with cadmium sulfide quantum dots (CdS QDs) as an electron transport layer (ETL) in order to enhance the photovoltaic performance of inverted organic solar cell (IOSC). In present study, CdS QDs were deposited on ZNRs using a Successive Ionic Layer Adsorption and Reaction method (SILAR) method. In typical procedures, IOSCs were fabricated by spin-coating the P3HT:PC61BM photoactive layer onto the as-prepared ZNRs/CdS QDs. The results of current-voltage (I-V) measurement under illumination shows that the FTO/ZNRs/CdS QDs/ P3HT:PC61BM/ PEDOT: PSS/Ag IOSC achieved a higher power conversion efficiency (4.06 %) in comparison to FTO/ZNRs/P3HT:PC61BM/PEDOT: PSS/Ag (3.6 %). Our findings suggest that the improved open circuit voltage (Voc) and short circuit current density (Jsc) of ZNRs/CdS QDs devices could be attributed to enhanced electron selectivity and reduced interfacial charge carrier recombination between ZNRs and P3HT:PC61BM after the deposition of CdS QDs. The CdS QDs sensitized ZNRs reported herein exhibit great potential for advanced optoelectronic application.

Theoretical investigation of the structural, electronic, and thermodynamic properties of CdS1-xSex alloys

NASA Astrophysics Data System (ADS)

Long, Debing; Li, Mingkai; Meng, Dongxue; Ahuja, Rajeev; He, Yunbin

2018-03-01

In this work, the structural, electronic, and thermodynamic properties of wurtzite (WZ) and zincblende (ZB) CdS1-xSex alloys are investigated using the density functional theory (DFT) and the cluster expansion method. A special quasirandom structure containing 16 atoms is constructed to calculate the band structures of random alloys. The band gaps of CdS1-xSex alloys are direct and decrease as the Se content increases. The delta self-consistent-field method is applied to correct band gaps that are underestimated by DFT. The band offsets clearly reflect the variation in valence band maxima and conduction band minima, thus providing information useful to the design of relevant quantum well structures. The positive formation enthalpies of both phases imply that CdS1-xSex is an immiscible system and tends to phase separate. The influence of lattice vibrations on the phase diagram is investigated by calculating the phonon density of states. Lattice vibration effects can reduce the critical temperature Tc and increase alloy solid solubilities. This influence is especially significant in the ZB structure. When only chemical interactions are present, the Tc values for WZ- and ZB-CdS1-xSex are 260 K and 249 K, respectively. The lattice vibration enthalpy and entropy lower the Tc to 255 K and 233 K, respectively.

Garry Rumbles | NREL

Science.gov Websites

, colloidal quantum dots, and single-walled carbon nanotubes. Laser-based experiments (time-resolved fluorescence spectroscopy; time-resolved resonance Raman spectroscopy; laser-induced fluorescence spectroscopy ; time-resolved evanescent wave-induced fluorescence spectroscopy; picosecond coherent anti-Stokes Raman

Evaluation of the dielectric function of colloidal Cd1 - xHgxTe quantum dot films by spectroscopic ellipsometry

NASA Astrophysics Data System (ADS)

Bejaoui, A.; Alonso, M. I.; Garriga, M.; Campoy-Quiles, M.; Goñi, A. R.; Hetsch, F.; Kershaw, S. V.; Rogach, A. L.; To, C. H.; Foo, Y.; Zapien, J. A.

2017-11-01

We report on the investigation by spectroscopic ellipsometry of films containing Cd1 - xHgxTe alloy quantum dots (QDs). The alloy QDs were fabricated from colloidal CdTe QDs grown by an aqueous synthesis process followed by an ion-exchange step in which Hg2+ ions progressively replace Cd2+. For ellipsometric studies, several films were prepared on glass substrates using layer-by-layer (LBL) deposition. The contribution of the QDs to the measured ellipsometric spectra is extracted from a multi-sample, transmission and multi- angle-of-incidence ellipsometric data analysis fitted using standard multilayer and effective medium models that include surface roughness effects, modeled by an effective medium approximation. The relationship of the dielectric function of the QDs retrieved from these studies to that of the corresponding II-VI bulk material counterparts is presented and discussed.

Composite Supraparticles with Tunable Light Emission

PubMed Central

2017-01-01

Robust luminophores emitting light with broadly tunable colors are desirable in many applications such as light-emitting diode (LED)-based lighting, displays, integrated optoelectronics and biology. Nanocrystalline quantum dots with multicolor emission, from core- and shell-localized excitons, as well as solid layers of mixed quantum dots that emit different colors have been proposed. Here, we report on colloidal supraparticles that are composed of three types of Cd(Se,ZnS) core/(Cd,Zn)S shell nanocrystals with emission in the red, green, and blue. The emission of the supraparticles can be varied from pure to composite colors over the entire visible region and fine-tuned into variable shades of white light by mixing the nanocrystals in controlled proportions. Our approach results in supraparticles with sizes spanning the colloidal domain and beyond that combine versatility and processability with a broad, stable, and tunable emission, promising applications in lighting devices and biological research. PMID:28787121

Aggregation control of quantum dots through ion-mediated hydrogen bonding shielding.

PubMed

Liu, Jianbo; Yang, Xiaohai; Wang, Kemin; He, Xiaoxiao; Wang, Qing; Huang, Jin; Liu, Yan

2012-06-26

Nanoparticle stabilization against detrimental aggregation is a critical parameter that needs to be well controlled. Herein, we present a facile and rapid ion-mediated dispersing technique that leads to hydrophilic aggregate-free quantum dots (QDs). Because of the shielding of the hydrogen bonds between cysteamine-capped QDs, the presence of F(-) ions disassembled the aggregates of QDs and afforded their high colloidal stability. The F(-) ions also greatly eliminated the nonspecific adsorption of the QDs on glass slides and cells. Unlike the conventional colloidal stabilized method that requires the use of any organic ligand and/or polymer for the passivation of the nanoparticle surface, the proposed approach adopts the small size and large diffusion coefficient of inorganic ions as dispersant, which offers the disaggregation a fast reaction dynamics and negligible influence on their intrinsic surface functional properties. Therefore, the ion-mediated dispersing strategy showed great potential in chemosensing and biomedical applications.

Detecting trap states in planar PbS colloidal quantum dot solar cells

PubMed Central

Jin, Zhiwen; Wang, Aiji; Zhou, Qing; Wang, Yinshu; Wang, Jizheng

2016-01-01

The recently developed planar architecture (ITO/ZnO/PbS-TBAI/PbS-EDT/Au) has greatly improved the power conversion efficiency of colloidal quantum dot photovoltaics (QDPVs). However, the performance is still far below the theoretical expectations and trap states in the PbS-TBAI film are believed to be the major origin, characterization and understanding of the traps are highly demanded to develop strategies for continued performance improvement. Here employing impedance spectroscopy we detect trap states in the planar PbS QDPVs. We determined a trap state of about 0.34 eV below the conduction band with a density of around 3.2 × 1016 cm−3 eV−1. Temperature dependent open-circuit voltage analysis, temperature dependent diode property analysis and temperature dependent build-in potential analysis consistently denotes an below-bandgap activation energy of about 1.17–1.20 eV. PMID:27845392

Nanoimprint-Transfer-Patterned Solids Enhance Light Absorption in Colloidal Quantum Dot Solar Cells.

PubMed

Kim, Younghoon; Bicanic, Kristopher; Tan, Hairen; Ouellette, Olivier; Sutherland, Brandon R; García de Arquer, F Pelayo; Jo, Jea Woong; Liu, Mengxia; Sun, Bin; Liu, Min; Hoogland, Sjoerd; Sargent, Edward H

2017-04-12

Colloidal quantum dot (CQD) materials are of interest in thin-film solar cells due to their size-tunable bandgap and low-cost solution-processing. However, CQD solar cells suffer from inefficient charge extraction over the film thicknesses required for complete absorption of solar light. Here we show a new strategy to enhance light absorption in CQD solar cells by nanostructuring the CQD film itself at the back interface. We use two-dimensional finite-difference time-domain (FDTD) simulations to study quantitatively the light absorption enhancement in nanostructured back interfaces in CQD solar cells. We implement this experimentally by demonstrating a nanoimprint-transfer-patterning (NTP) process for the fabrication of nanostructured CQD solids with highly ordered patterns. We show that this approach enables a boost in the power conversion efficiency in CQD solar cells primarily due to an increase in short-circuit current density as a result of enhanced absorption through light-trapping.

Cyclic voltammetry as a sensitive method for in situ probing of chemical transformations in quantum dots.

PubMed

Osipovich, Nikolai P; Poznyak, Sergei K; Lesnyak, Vladimir; Gaponik, Nikolai

2016-04-21

The application of electrochemical methods for the characterization of colloidal quantum dots (QDs) attracts considerable attention as these methods may allow for monitoring of some crucial parameters, such as energetic levels of conduction and valence bands as well as surface traps and ligands under real conditions of colloidal solution. In the present work we extend the applications of cyclic voltammetry (CV) to in situ monitoring of degradation processes of water-soluble CdTe QDs. This degradation occurs under lowering of pH to the values around 5, i.e. under conditions relevant to bioimaging applications of these QDs, and is accompanied by pronounced changes of their photoluminescence. Observed correlations between characteristic features of CV diagrams and the fluorescence spectra allowed us to propose mechanisms responsible for evolution of the photoluminescence properties as well as degradation pathway of CdTe QDs at low pH.

10.6% Certified Colloidal Quantum Dot Solar Cells via Solvent-Polarity-Engineered Halide Passivation.

PubMed

Lan, Xinzheng; Voznyy, Oleksandr; García de Arquer, F Pelayo; Liu, Mengxia; Xu, Jixian; Proppe, Andrew H; Walters, Grant; Fan, Fengjia; Tan, Hairen; Liu, Min; Yang, Zhenyu; Hoogland, Sjoerd; Sargent, Edward H

2016-07-13

Colloidal quantum dot (CQD) solar cells are solution-processed photovoltaics with broad spectral absorption tunability. Major advances in their efficiency have been made via improved CQD surface passivation and device architectures with enhanced charge carrier collection. Herein, we demonstrate a new strategy to improve further the passivation of CQDs starting from the solution phase. A cosolvent system is employed to tune the solvent polarity in order to achieve the solvation of methylammonium iodide (MAI) and the dispersion of hydrophobic PbS CQDs simultaneously in a homogeneous phase, otherwise not achieved in a single solvent. This process enables MAI to access the CQDs to confer improved passivation. This, in turn, allows for efficient charge extraction from a thicker photoactive layer device, leading to a certified solar cell power conversion efficiency of 10.6%, a new certified record in CQD photovoltaics.

Empirical, thermodynamic and quantum-chemical investigations of inclusion complexation between flavanones and (2-hydroxypropyl)-cyclodextrins.

PubMed

Liu, Benguo; Li, Wei; Nguyen, Tien An; Zhao, Jian

2012-09-15

The inclusion complexation of (2-hydroxypropyl)-cyclodextrins with flavanones was investigated by phase solubility measurements, as well as thermodynamic and quantum chemical methods. Inclusion complexes were formed between (2-hydroxypropyl)-α-cyclodextrin (HP-α-CD), (2-hydroxypropyl)-β-cyclodextrin (HP-β-CD), (2-hydroxypropyl)-γ-cyclodextrin (HP-γ-CD) and β-cyclodextrin (β-CD) and four flavanones (naringenin, naringin, hesperetin and dihydromyricetin) in aqueous solutions and their phase solubility was determined. For all the flavanones, the stability constants of their complexes formed with different CDs followed the rank order: HP-β-CD (MW 1540)>HP-β-CD (MW 1460)>HP-β-CD (MW 1380)>β-CD>HP-γ-CD>HP-α-CD. Experimental results and quantum chemical calculations showed that the ability of flavanones to form inclusion complex with (2-hydroxypropyl)-cyclodextrins was determined by both the steric effect and hydrophobicity of the flavanones. For flavanones that have similar molecular volumes, the hydrophobicity of the molecule was the main determining factor of its ability to form inclusion complexes with HP-β-CD, and the hydrophobicity parameter Log P is highly correlated with the stability constant of the complexes. Results of thermodynamic study demonstrated that hydrophobic interaction is the main driving force for the formation process of the flavanone-CD inclusion complexes. Quantum chemical analysis of the most active hydroxyl groups and HOMO (the highest occupied molecular orbital) showed that the B ring of the flavanones was most likely involved in hydrogen bonding with the side groups in the cavity of the CDs, through which the inclusion complex was stabilised. Copyright © 2012 Elsevier Ltd. All rights reserved.

A triple quantum dot based nano-electromechanical memory device

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pozner, R.; Lifshitz, E.; Solid State Institute, Technion-Israel Institute of Technology, Haifa 32000

Colloidal quantum dots (CQDs) are free-standing nano-structures with chemically tunable electronic properties. This tunability offers intriguing possibilities for nano-electromechanical devices. In this work, we consider a nano-electromechanical nonvolatile memory (NVM) device incorporating a triple quantum dot (TQD) cluster. The device operation is based on a bias induced motion of a floating quantum dot (FQD) located between two bound quantum dots (BQDs). The mechanical motion is used for switching between two stable states, “ON” and “OFF” states, where ligand-mediated effective interdot forces between the BQDs and the FQD serve to hold the FQD in each stable position under zero bias. Consideringmore » realistic microscopic parameters, our quantum-classical theoretical treatment of the TQD reveals the characteristics of the NVM.« less

Using of Quantum Dots in Biology and Medicine.

PubMed

Pleskova, Svetlana; Mikheeva, Elza; Gornostaeva, Ekaterina

2018-01-01

Quantum dots are nanoparticles, which due to their unique physical and chemical (first of all optical) properties, are promising in biology and medicine. There are many ways for quantum dots synthesis, both in the form of nanoislands self-forming on the surfaces, which can be used as single-photon emitters in electronics for storing information, and in the form of colloidal quantum dots for diagnostic and therapeutic purposes in living systems. The paper describes the main methods of quantum dots synthesis and summarizes medical and biological ways of their use. The main emphasis is laid on the ways of quantum dots surface modification. Influence of the size and form of nanoparticles, charge on the surfaces of quantum dots, and cover type on the efficiency of internalization by cells and cell compartments is shown. The main mechanisms of penetration are considered.

Aqueous synthesis of highly luminescent AgInS2-ZnS quantum dots and their biological applications

NASA Astrophysics Data System (ADS)

Regulacio, Michelle D.; Win, Khin Yin; Lo, Seong Loong; Zhang, Shuang-Yuan; Zhang, Xinhai; Wang, Shu; Han, Ming-Yong; Zheng, Yuangang

2013-02-01

Highly emissive and air-stable AgInS2-ZnS quantum dots (ZAIS QDs) with quantum yields of up to 20% have been successfully synthesized directly in aqueous media in the presence of polyacrylic acid (PAA) and mercaptoacetic acid (MAA) as stabilizing and reactivity-controlling agents. The as-prepared water-dispersible ZAIS QDs are around 3 nm in size, possess the tetragonal chalcopyrite crystal structure, and exhibit long fluorescence lifetimes (>100 ns). In addition, these ZAIS QDs are found to exhibit excellent optical and colloidal stability in physiologically relevant pH values as well as very low cytotoxicity, which render them particularly suitable for biological applications. Their potential use in biological labelling of baculoviral vectors is demonstrated.Highly emissive and air-stable AgInS2-ZnS quantum dots (ZAIS QDs) with quantum yields of up to 20% have been successfully synthesized directly in aqueous media in the presence of polyacrylic acid (PAA) and mercaptoacetic acid (MAA) as stabilizing and reactivity-controlling agents. The as-prepared water-dispersible ZAIS QDs are around 3 nm in size, possess the tetragonal chalcopyrite crystal structure, and exhibit long fluorescence lifetimes (>100 ns). In addition, these ZAIS QDs are found to exhibit excellent optical and colloidal stability in physiologically relevant pH values as well as very low cytotoxicity, which render them particularly suitable for biological applications. Their potential use in biological labelling of baculoviral vectors is demonstrated. Electronic supplementary information (ESI) available: Quantum yields, EDX spectrum and photoluminescence decay curves. See DOI: 10.1039/c3nr34159c

Organic-inorganic nanostructures for luminescent indication in the near-infrared range

NASA Astrophysics Data System (ADS)

Kondratenko, T. S.; Ovchinnikov, O. V.; Grevtseva, I. G.; Smirnov, M. S.

2016-04-01

Amplifying and quenching of IR luminescence of colloidal Ag2S quantum dots were revealed to take place when they couple to organic dye molecules of 3,3'-di-(γ-sulfopropyl)-9-ethyl-4,5,4',5'-dibenzothiacarbocyanine betaine and erytrosine pyridinium salts, respectively. The observed effects are explained as due to the formation of organic-inorganic heterostructures with different mutual arrangement of electronic states of the dyes and the quantum dots.

Photoelectric performance of TiO2 nanotube array photoelectrodes sensitized with CdS0.54Se0.46 quantum dots

NASA Astrophysics Data System (ADS)

Gakhar, Ruchi; Smith, York R.; Misra, Mano; Chidambaram, Dev

2015-11-01

The photoelectrochemical performance of CdSSe quantum dots tethered to a framework of vertically oriented titania (TiO2) nanotubes was studied. The TiO2/CdSSe framework demonstrated improved charge transfer due to its unique band edge structure, thus validating the higher photocurrent generation. The composite film led to an 11-fold enhancement in comparison to the control TiO2 film, implying that the ternary quantum dots and the nanotubular structure of TiO2 work in tandem to promote charge separation and favorably impact photoelectrochemical performance. Further, the results also suggest that structural and optoelectronic properties of TiO2 films are significantly affected by the thicknesses of the CdSSe layer.

Sample-averaged biexciton quantum yield measured by solution-phase photon correlation.

PubMed

Beyler, Andrew P; Bischof, Thomas S; Cui, Jian; Coropceanu, Igor; Harris, Daniel K; Bawendi, Moungi G

2014-12-10

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.

Effect of lateral size and thickness on the electronic structure and optical properties of quasi two-dimensional CdSe and CdS nanoplatelets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bose, Sumanta; Fan, W. J., E-mail: ewjfan@ntu.edu.sg; Zhang, D. H.

2016-04-14

The effect of lateral size and vertical thickness of CdSe and CdS nanoplatelets (NPLs) on their electronic structure and optical properties are investigated using an effective-mass envelope function theory based on the 8-band k ⋅ p model with valence force field considerations. Volumetrically larger NPLs have lower photon emission energy due to limited quantum confinement, but a greater transition matrix element (TME) due to larger electron-hole wavefunction overlap. The optical gain characteristics depend on several factors such as TME, Fermi factor, carrier density, NPL dimensions, material composition, and dephasing rate. There is a red shift in the peak position, moremore » so with an increase in thickness than lateral size. For an increasing carrier density, the gain spectrum undergoes a slight blue shift due to band filling effect. For a fixed carrier density, the Fermi factor is higher for volumetrically larger NPLs and so is the difference between the quasi-Fermi level separation and the effective bandgap. The transparency injection carrier density (and thus input current density threshold) is dimension dependent and falls for volumetrically larger NPLs, as they can attain the requisite exciton count for transparency with a relatively lower density. Between CdSe and CdS, CdSe has lower emission energy due to smaller bandgap, but a higher TME due to lower effective mass. CdS, however, has a higher so hole contribution due to a lower spin-orbit splitting energy. Both CdSe and CdS NPLs are suitable candidates for short-wavelength LEDs and lasers in the visible spectrum, but CdSe is expected to exhibit better optical performance.« less

Continuous distribution of emission states from single CdSe/ZnS quantum dots.

PubMed

Zhang, Kai; Chang, Hauyee; Fu, Aihua; Alivisatos, A Paul; Yang, Haw

2006-04-01

The photoluminescence dynamics of colloidal CdSe/ZnS/streptavidin quantum dots were studied using time-resolved single-molecule spectroscopy. Statistical tests of the photon-counting data suggested that the simple "on/off" discrete state model is inconsistent with experimental results. Instead, a continuous emission state distribution model was found to be more appropriate. Autocorrelation analysis of lifetime and intensity fluctuations showed a nonlinear correlation between them. These results were consistent with the model that charged quantum dots were also emissive, and that time-dependent charge migration gave rise to the observed photoluminescence dynamics.

AgCl-doped CdSe quantum dots with near-IR photoluminescence.

PubMed

Kotin, Pavel Aleksandrovich; Bubenov, Sergey Sergeevich; Mordvinova, Natalia Evgenievna; Dorofeev, Sergey Gennadievich

2017-01-01

We report the synthesis of colloidal CdSe quantum dots doped with a novel Ag precursor: AgCl. The addition of AgCl causes dramatic changes in the morphology of synthesized nanocrystals from spherical nanoparticles to tetrapods and finally to large ellipsoidal nanoparticles. Ellipsoidal nanoparticles possess an intensive near-IR photoluminescence ranging up to 0.9 eV (ca. 1400 nm). In this article, we explain the reasons for the formation of the ellipsoidal nanoparticles as well as the peculiarities of the process. The structure, Ag content, and optical properties of quantum dots are also investigated. The optimal conditions for maximizing both the reaction yield and IR photoluminescence quantum yield are found.

Interactions between colloidal silver and photosynthetic pigments located in cyanobacteria fragments and in solution.

PubMed

Siejak, Przemysław; Frackowiak, Danuta

2007-09-25

Changes in the yield of the fluorescence emitted by pigments of photosynthetic organisms could be used for the establishment of the presence of some toxic substances. The presence of colloidal metals can be indicated by enhancement of pigments' emission as a result of plasmons generation. The spectra of the pigments of cyanobacterium Synechocystis located in the bacterium fragments and in solutions with and without colloidal silver additions have been measured. The quantum yield of the pigments' fluorescence in solution has been observed to increase at some wavelength of excitation, while the fluorescence of the pigments in the bacteria fragments has been only quenched as a consequence of interactions with colloidal silver particles. Close contact between pigment molecules located in bacteria fragments and silver particles is probably not possible. We plan in future to investigate the influence of other, more typical metal pollutants of water, using similar spectral methods and several other photosynthetic bacteria pigments, in solution, in cell fragments and in the whole bacteria organisms.

Design of cadmium-free colloidal II-VI semiconductor quantum dots exhibiting RGB emission

NASA Astrophysics Data System (ADS)

Asano, Hiroshi; Omata, Takahisa

2017-04-01

The size and composition dependence of the optical gap of colloidal alloyed quantum dots (QDs) of Zn(Te1-xSex) and Zn(Te1-xSx) were calculated by the finite-depth-well effective mass approximation method. QDs that exhibited red, green and blue emission were explored to develop cadmium-free II-VI chalcogenide-based QD-phosphors. We considered that highly monodisperse colloidal QDs with diameters of 3-6 nm are easy to synthesize and II-VI semiconductor QDs usually exhibit a Stokes shift ranging between 50 and 150 meV. We showed that Zn(Te1-xSex) QDs with 0.02≤x≤0.68, and 0≤x≤0.06, and 0.66≤x≤0.9 may be expected to exhibit green, and blue emission, respectively. Zn(Te1-xSx) QDs with 0.26≤x≤0.37, 0.01≤x≤0.2 and 0.45≤x≤0.61, 0≤x≤0.02, and 0.63≤x≤0.72, should give red, green and blue emission respectively. On the basis of our calculations, we showed that Zn(Te,Se) and Zn(Te,S) QDs are very promising cadmium-free II-VI chalcogenide semiconductor QD phosphors.

Mode-locked Er-doped fiber laser based on PbS/CdS core/shell quantum dots as saturable absorber.

PubMed

Ming, Na; Tao, Shina; Yang, Wenqing; Chen, Qingyun; Sun, Ruyi; Wang, Chang; Wang, Shuyun; Man, Baoyuan; Zhang, Huanian

2018-04-02

Previously, PbS/CdS core/shell quantum dots with excellent optical properties have been widely used as light-harvesting materials in solar cell and biomarkers in bio-medicine. However, the nonlinear absorption characteristics of PbS/CdS core/shell quantum dots have been rarely investigated. In this work, PbS/CdS core/shell quantum dots were successfully employed as nonlinear saturable absorber (SA) for demonstrating a mode-locked Er-doped fiber laser. Based on a film-type SA, which was prepared by incorporating the quantum dots with the polyvinyl alcohol (PVA), mode-locked Er-doped operation with a pulse width of 54 ps and a maximum average output power of 2.71 mW at the repetition rate of 3.302 MHz was obtained. Our long-time stable results indicate that the CdS shell can effectively protect the PbS core from the effect of photo-oxidation and PbS/CdS core/shell quantum dots were efficient SA candidates for demonstrating pulse fiber lasers due to its tunable absorption peak and excellent saturable absorption properties.

Quantum Dot Solar Cell Fabrication Protocols

DOE PAGES

Chernomordik, Boris D.; Marshall, Ashley R.; Pach, Gregory F.; ...

2016-09-26

Colloidally synthesized quantum-confined semiconducting spherical nanocrystals, often referred to as quantum dots (QDs), offer a high degree of chemical, optical, and electronic tunability. As a result, there is an increasing interest in employing colloidal QDs for electronic and optical applications that is reflected in a growing number of publications. In this protocol we provide detailed procedures for the fabrication of QD solar cells specifically employing PbSe and PbS QDs. Here we include details that are learned through experience, beyond those in typical methodology sections, and include example pictures and videos to aid in fabricating QD solar cells. Although successful solarmore » cell fabrication is ultimately learned through experience, this protocol is intended to accelerate that process. The protocol developed here is intended to be a general starting point for developing PbS and PbSe QD test bed solar cells. We include steps for forming conductive QD films via dip coating as well as spin coating. Finally, we provide protocols that detail the synthesis of PbS and PbSe QDs through a unique cation exchange reaction and discuss how different QD synthetic routes could impact the resulting solar cell performance.« less

Dry-Deposited Transparent Carbon Nanotube Film as Front Electrode in Colloidal Quantum Dot Solar Cells.

PubMed

Zhang, Xiaoliang; Aitola, Kerttu; Hägglund, Carl; Kaskela, Antti; Johansson, Malin B; Sveinbjörnsson, Kári; Kauppinen, Esko I; Johansson, Erik M J

2017-01-20

Single-walled carbon nanotubes (SWCNTs) show great potential as an alternative material for front electrodes in photovoltaic applications, especially for flexible devices. In this work, a press-transferred transparent SWCNT film was utilized as front electrode for colloidal quantum dot solar cells (CQDSCs). The solar cells were fabricated on both glass and flexible substrates, and maximum power conversion efficiencies of 5.5 and 5.6 %, respectively, were achieved, which corresponds to 90 and 92 % of an indium-doped tin oxide (ITO)-based device (6.1 %). The SWCNTs are therefore a very good alternative to the ITO-based electrodes especially for flexible solar cells. The optical electric field distribution and optical losses within the devices were simulated theoretically and the results agree with the experimental results. With the optical simulations that were performed it may also be possible to enhance the photovoltaic performance of SWCNT-based solar cells even further by optimizing the device configuration or by using additional optical active layers, thus reducing light reflection of the device and increasing light absorption in the quantum dot layer. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tapping the potential of trioctylphosphine (TOP) in the realization of highly luminescent blue-emitting colloidal indium phosphide (InP) quantum dots

NASA Astrophysics Data System (ADS)

Singh, Akanksha; Chawla, Parul; Jain, Shefali; Sharma, Shailesh Narain

2017-06-01

In this work, extremely small blue emitting colloidal InP-based quantum dots (size 2-5 nm) have been synthesized using trioctylphosphine (TOP) as a source of phosphorus. The method reported here is unconventional, quite rapid ( 90 min), more viable, less expensive and relatively greener as compared to other conventional methods that employ tristrimethylsilyylphosphine(P(SiMe3)3) which is scarce, expensive, flammable, highly toxic and even banned in a few countries. Highly luminescent InP QDs having bluish-green emission (λ 490 nm) can be synthesized using this method without resorting to any post-synthesis etching to tune the emission to the blue region. Besides being the source of phosphorus and the particle size regulating agent, the efficacy of TOP is further realized during synthesis via its reduction of indium salt, which aids in the formation of indium metal and then subsequently in the development of InP QDs. The PL intensity of as-synthesized InP QDs is further enhanced by growing a shell of wide band gap material, i.e. ZnS resulting in a concurrent increment in quantum yield from 25% to 38% respectively.

All-solution-processed, multilayered CuInS₂/ZnS colloidal quantum-dot-based electroluminescent device.

PubMed

Kim, Jong-Hoon; Yang, Heesun

2014-09-01

While significant progress of electroluminescent (EL) quantum dot light-emitting diodes (QD-LEDs) that rely exclusively on Cd-containing II-VI quantum dots (QDs) has been reported over the past two decades with respect to device processing and performance, devices based on non-Cd QDs as an active emissive layer (EML) remain at the early stage of development. In this work, utilizing highly luminescent colloidal CuInS2 (CIS)/ZnS QDs, all-solution-processed multilayered QD-LEDs are fabricated by sequentially spin depositing a hole transport layer of poly(9-vinlycarbazole), an EML of CIS/ZnS QDs, and an electron transport layer of ZnO nanoparticles. Our focus in device fabrication is to vary the thickness of the QD EML, which is one of the primary determinants in EL performance but has not been addressed in earlier reports. The device with an optimal EML thickness exhibits a peak luminance of 1564  cd/m2 and current efficiency of 2.52  cd/A. This record value in efficiency is higher by 3-4 times that of CIS QD-LEDs reported previously.

Structural, optical, electrochemical and photovoltaic studies of spider web like Silver Indium Diselenide Quantum dots synthesized by ligand mediated colloidal sol-gel approach

NASA Astrophysics Data System (ADS)

Adhikari, Tham; Pathak, Dinesh; Wagner, Tomas; Jambor, Roman; Jabeen, Uzma; Aamir, Muhammad; Nunzi, Jean-Michel

2017-11-01

Silver indium diselenide quantum dots were successively synthesized by colloidal sol-gel method by chelating with organic ligand oleylamine (OLA). The particle size was studied by transmission electron microscopy (TEM) and the size was found about 10 nm. X-ray diffraction (XRD) was used to study crystalline structure of the nanocrystals. The grain size and morphology were further studied by scanning electron microscopy (SEM) and atomic force microscopy (AFM). The elemental composition was studied by X-ray photon electron spectroscopy (XPS) and energy dispersive x-ray spectroscopy (EDAX). The capping property of OLA in nanocrystal was also demonstrated by Fourier Transform Infrared spectroscopy (FTIR). The band gap was calculated from both cyclic voltammetry and optical absorption and suggest quantum confinement. The solution processed bilayer thin film solar cells were fabricated with n-type Zinc oxide using doctor blading/spin coating method and their photovoltaic performance was studied. The best device sintered at 450 °C showed an efficiency 0.75% with current density of 4.54 mAcm-2, open-circuit voltage 0.44 V and fill factor 39.4%.

Cyto-molecular Tuning of Quantum Dots

NASA Astrophysics Data System (ADS)

Lee, Bong; Suresh, Sindhuja; Ekpenyong, Andrew

Quantum dots (QDs) are semiconductor nanoparticles composed of groups II-VI or III-V elements, with physical dimensions smaller than the exciton Bohr radius, and between 1-10 nm. Their applications and promising myriad applications in photovoltaic cells, biomedical imaging, targeted drug delivery, quantum computing, etc, have led to much research on their interactions with other systems. For biological systems, research has focused on biocompatibility and cytotoxicity of QDs in the context of imaging/therapy. However, there is a paucity of work on how biological systems might be used to tune QDs. Here, we hypothesize that the photo-electronic properties of QDs can be tuned by biological macromolecules following controlled changes in cellular activities. Using CdSe/ZnS core-shell QDs, we perform spectroscopic analysis of optically excited colloidal QDs with and without promyelocytic HL60 cells. Preliminary results show shifts in the emission spectra of the colloidal dispersions with and without cells. We will present results for activated HL60-derived cells where specific macromolecules produced by these cells perturb the electric dipole moments of the excited QDs and the associated electric fields, in ways that constitute what we describe as cyto-molecular tuning. Startup funds from the College of Arts and Sciences, Creighton University (to AEE).

Quantum Dot Solar Cell Fabrication Protocols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chernomordik, Boris D.; Marshall, Ashley R.; Pach, Gregory F.

Colloidally synthesized quantum-confined semiconducting spherical nanocrystals, often referred to as quantum dots (QDs), offer a high degree of chemical, optical, and electronic tunability. As a result, there is an increasing interest in employing colloidal QDs for electronic and optical applications that is reflected in a growing number of publications. In this protocol we provide detailed procedures for the fabrication of QD solar cells specifically employing PbSe and PbS QDs. Here we include details that are learned through experience, beyond those in typical methodology sections, and include example pictures and videos to aid in fabricating QD solar cells. Although successful solarmore » cell fabrication is ultimately learned through experience, this protocol is intended to accelerate that process. The protocol developed here is intended to be a general starting point for developing PbS and PbSe QD test bed solar cells. We include steps for forming conductive QD films via dip coating as well as spin coating. Finally, we provide protocols that detail the synthesis of PbS and PbSe QDs through a unique cation exchange reaction and discuss how different QD synthetic routes could impact the resulting solar cell performance.« less

Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna

DOE PAGES

Matsuzaki, Korenobu; Vassant, Simon; Liu, Hsuan-Wei; ...

2017-02-14

Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other nonradiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons and biexcitons by 109 and 100 folds at quantum efficiencies of 60 and 70%, respectively, in very good agreement withmore » the outcome of numerical calculations. We discuss the implications of our work for future fundamental and applied research in nano-optics.« less

Eco-friendly carbon-nanodot-based fluorescent paints for advanced photocatalytic systems

PubMed Central

Young Park, So; Uk Lee, Hyun; Lee, Young-Chul; Choi, Saehae; Hyun Cho, Dae; Sik Kim, Hee; Bang, Sunghee; Seo, Soonjoo; Chang Lee, Soon; Won, Jonghan; Son, Byung-Chul; Yang, Mino; Lee, Jouhahn

2015-01-01

Fluorescent carbon nanomaterials, especially zero-dimensional (0D) carbon nanodots (CDs), are widely used in broad biological and optoelectronic applications. CDs have unique characteristics such as strong fluorescence, biocompatibility, sun-light response, and capability of mass-production. Beyond the previous green CD obtained from harmful natural substances, we report a new type of fluid-based fluorescent CD paints (C-paints) derived from polyethylene glycol (PEG; via simple ultrasound irradiation at room temperatures) and produced in quantum yields of up to ~14%. Additionally, C-paints possess a strong, UV- and visible-light-responsive photoluminescent (PL) property. Most especially, C-paints, by incorporation into a photocatalytic system, show additional roles in the emission of fluorescent light for activation of TiO2 nanoparticles (NPs) and the resultant detoxification of most organic dyes, thus further enabling embarkation in advanced water purification. PMID:26201431

Eco-friendly carbon-nanodot-based fluorescent paints for advanced photocatalytic systems.

PubMed

Park, So Young; Lee, Hyun Uk; Lee, Young-Chul; Choi, Saehae; Cho, Dae Hyun; Kim, Hee Sik; Bang, Sunghee; Seo, Soonjoo; Lee, Soon Chang; Won, Jonghan; Son, Byung-Chul; Yang, Mino; Lee, Jouhahn

2015-07-23

Fluorescent carbon nanomaterials, especially zero-dimensional (0D) carbon nanodots (CDs), are widely used in broad biological and optoelectronic applications. CDs have unique characteristics such as strong fluorescence, biocompatibility, sun-light response, and capability of mass-production. Beyond the previous green CD obtained from harmful natural substances, we report a new type of fluid-based fluorescent CD paints (C-paints) derived from polyethylene glycol (PEG; via simple ultrasound irradiation at room temperatures) and produced in quantum yields of up to ~14%. Additionally, C-paints possess a strong, UV- and visible-light-responsive photoluminescent (PL) property. Most especially, C-paints, by incorporation into a photocatalytic system, show additional roles in the emission of fluorescent light for activation of TiO2 nanoparticles (NPs) and the resultant detoxification of most organic dyes, thus further enabling embarkation in advanced water purification.

Nanocrystals of Cesium Lead Halide Perovskites (CsPbX₃, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut.

PubMed

Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I; Krieg, Franziska; Caputo, Riccarda; Hendon, Christopher H; Yang, Ruo Xi; Walsh, Aron; Kovalenko, Maksym V

2015-06-10

Metal halides perovskites, such as hybrid organic-inorganic CH3NH3PbI3, are newcomer optoelectronic materials that have attracted enormous attention as solution-deposited absorbing layers in solar cells with power conversion efficiencies reaching 20%. Herein we demonstrate a new avenue for halide perovskites by designing highly luminescent perovskite-based colloidal quantum dot materials. We have synthesized monodisperse colloidal nanocubes (4-15 nm edge lengths) of fully inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I or mixed halide systems Cl/Br and Br/I) using inexpensive commercial precursors. Through compositional modulations and quantum size-effects, the bandgap energies and emission spectra are readily tunable over the entire visible spectral region of 410-700 nm. The photoluminescence of CsPbX3 nanocrystals is characterized by narrow emission line-widths of 12-42 nm, wide color gamut covering up to 140% of the NTSC color standard, high quantum yields of up to 90%, and radiative lifetimes in the range of 1-29 ns. The compelling combination of enhanced optical properties and chemical robustness makes CsPbX3 nanocrystals appealing for optoelectronic applications, particularly for blue and green spectral regions (410-530 nm), where typical metal chalcogenide-based quantum dots suffer from photodegradation.

Efficient PbS/CdS co-sensitized solar cells based on TiO2 nanorod arrays

PubMed Central

2013-01-01

Narrow bandgap PbS nanoparticles, which may expand the light absorption range to the near-infrared region, were deposited on TiO2 nanorod arrays by successive ionic layer adsorption and reaction method to make a photoanode for quantum dot-sensitized solar cells (QDSCs). The thicknesses of PbS nanoparticles were optimized to enhance the photovoltaic performance of PbS QDSCs. A uniform CdS layer was directly coated on previously grown PbS-TiO2 photoanode to protect the PbS from the chemical attack of polysulfide electrolytes. A remarkable short-circuit photocurrent density (approximately 10.4 mA/cm2) for PbS/CdS co-sensitized solar cell was recorded while the photocurrent density of only PbS-sensitized solar cells was lower than 3 mA/cm2. The power conversion efficiency of the PbS/CdS co-sensitized solar cell reached 1.3%, which was beyond the arithmetic addition of the efficiencies of single constituents (PbS and CdS). These results indicate that the synergistic combination of PbS with CdS may provide a stable and effective sensitizer for practical solar cell applications. PMID:23394609

Ultrafast Room-Temperature Single Photon Emission from Quantum Dots Coupled to Plasmonic Nanocavities.

PubMed

Hoang, Thang B; Akselrod, Gleb M; Mikkelsen, Maiken H

2016-01-13

Efficient and bright single photon sources at room temperature are critical components for quantum information systems such as quantum key distribution, quantum state teleportation, and quantum computation. However, the intrinsic radiative lifetime of quantum emitters is typically ∼10 ns, which severely limits the maximum single photon emission rate and thus entanglement rates. Here, we demonstrate the regime of ultrafast spontaneous emission (∼10 ps) from a single quantum emitter coupled to a plasmonic nanocavity at room temperature. The nanocavity integrated with a single colloidal semiconductor quantum dot produces a 540-fold decrease in the emission lifetime and a simultaneous 1900-fold increase in the total emission intensity. At the same time, the nanocavity acts as a highly efficient optical antenna directing the emission into a single lobe normal to the surface. This plasmonic platform is a versatile geometry into which a variety of other quantum emitters, such as crystal color centers, can be integrated for directional, room-temperature single photon emission rates exceeding 80 GHz.

Directed assembly of colloidal particles for micro/nano photonics (Conference Presentation)

NASA Astrophysics Data System (ADS)

Zheng, Yuebing

2017-02-01

Bottom-up fabrication of complex structures with chemically synthesized colloidal particles as building blocks pave an efficient and cost-effective way towards micro/nano photonics with unprecedented functionality and tunability. Novel properties can arise from quantum effects of colloidal particles, as well as inter-particle interactions and spatial arrangement in particle assemblies. Herein, I discuss our recent developments and applications of three types of techniques for directed assembly of colloidal particles: moiré nanosphere lithography (MNSL), bubble-pen lithography (BPL), and optothermal tweezers (OTTs). Specifically, MNSL provides an efficient approach towards creating moiré metasurface with tunable and multiband optical responses from visible to mid-infrared regime. Au moiré metasurfaces have been applied for surface-enhanced infrared spectroscopy, optical capture and patterning of bacteria, and photothermal denaturation of proteins. BPL is developed to pattern a variety of colloidal particles on plasmonic substrates and two-dimensional atomic-layer materials in an arbitrary manner. The laser-directed microbubble captures and immobilizes nanoparticles through coordinated actions of Marangoni convection, surface tension, gas pressure, and substrate adhesion. OTTs are developed to create dynamic nanoparticle assemblies at low optical power. Such nanoparticle assemblies have been used for surface-enhanced Raman spectroscopy for molecular analysis in their native environments.

Two-dimensional colloidal metal chalcogenides semiconductors: synthesis, spectroscopy, and applications.

PubMed

Lhuillier, Emmanuel; Pedetti, Silvia; Ithurria, Sandrine; Nadal, Brice; Heuclin, Hadrien; Dubertret, Benoit

2015-01-20

CONSPECTUS: Semiconductors are at the basis of electronics. Up to now, most devices that contain semiconductors use materials obtained from a top down approach with semiconductors grown by molecular beam epitaxy or chemical vapor deposition. Colloidal semiconductor nanoparticles have been synthesized for more than 30 years now, and their synthesis is becoming mature enough that these nanoparticles have started to be incorporated into devices. An important development that recently took place in the field of colloidal quantum dots is the synthesis of two-dimensional (2D) semiconductor nanoplatelets that appear as free-standing nanosheets. These 2D colloidal systems are the newborn in the family of shaped-controlled nanoparticles that started with spheres, was extended with rods and wires, continued with tetrapods, and now ends with platelets. From a physical point of view, these objects bring 1D-confined particles into the colloidal family. It is a notable addition, since these platelets can have a thickness that is controlled with atomic precision, so that no inhomogeneous broadening is observed. Because they have two large free interfaces, mirror charges play an important role, and the binding energy of the exciton is extremely large. These two effects almost perfectly compensate each other, it results in particles with unique spectroscopic properties such as fast fluorescent lifetimes and extreme color purity (narrow full width at half-maximum of their emission spectra). These nanoplatelets with extremely large confinement but very simple and well-defined chemistry are model systems to check and further develop, notably with the incorporation in the models of the organic/inorganic interface, various theoretical approaches used for colloidal particles. From a chemical point of view, these colloidal particles are a model system to study the role of ligands since they have precisely defined facets. In addition, the synthesis of these highly anisotropic objects triggered new research to understand at a mechanistic level how this strong anisotropy could be generated. Luckily, some of the chemical know-how built with the spherical and rod-shaped particles is being transferred, with some adaptation, to 2D systems, so that 2D core/shell and core/crown heterostructures have recently been introduced. These objects are very interesting because they suggest that multiple quantum wells could be grown in solution. From the application point of view, 2D colloidal nanoplatelets offer interesting perspectives when color purity, charge conductivity, or field tunable absorption are required. In this Account, we review the chemical synthesis, the physical properties, and the applications of colloidal semiconductor nanoplatelets with an emphasis on the zinc-blende nanoplatelets that were developed more specifically in our group.

A real-time spectrum acquisition system design based on quantum dots-quantum well detector

NASA Astrophysics Data System (ADS)

Zhang, S. H.; Guo, F. M.

2016-01-01

In this paper, we studied the structure characteristics of quantum dots-quantum well photodetector with response wavelength range from 400 nm to 1000 nm. It has the characteristics of high sensitivity, low dark current and the high conductance gain. According to the properties of the quantum dots-quantum well photodetectors, we designed a new type of capacitive transimpedence amplifier (CTIA) readout circuit structure with the advantages of adjustable gain, wide bandwidth and high driving ability. We have implemented the chip packaging between CTIA-CDS structure readout circuit and quantum dots detector and tested the readout response characteristics. According to the timing signals requirements of our readout circuit, we designed a real-time spectral data acquisition system based on FPGA and ARM. Parallel processing mode of programmable devices makes the system has high sensitivity and high transmission rate. In addition, we realized blind pixel compensation and smoothing filter algorithm processing to the real time spectrum data by using C++. Through the fluorescence spectrum measurement of carbon quantum dots and the signal acquisition system and computer software system to realize the collection of the spectrum signal processing and analysis, we verified the excellent characteristics of detector. It meets the design requirements of quantum dot spectrum acquisition system with the characteristics of short integration time, real-time and portability.

Novel Photovoltaic Devices Using Ferroelectric Material and Colloidal Quantum Dots

NASA Astrophysics Data System (ADS)

Paik, Young Hun

As the global concern for the financial and environmental costs of traditional energy resources increases, research on renewable energy, most notably solar energy, has taken center stage. Many alternative photovoltaic (PV) technologies for 'the next generation solar cell' have been extensively studied to overcome the Shockley-Queisser 31% efficiency limit as well as tackle the efficiency vs. cost issues. This dissertation focuses on the novel photovoltaic mechanism for the next generation solar cells using two inorganic nanomaterials, nanocrystal quantum dots and ferroelectric nanoparticles. Lead zirconate titanate (PZT) materials are widely studied and easy to synthesize using solution based chemistry. One of the fascinating properties of the PZT material is a Bulk Photovoltaic effect (BPVE). This property has been spotlighted because it can produce very high open circuit voltage regardless of the electrical bandgap of the materials. However, the poor optical absorption of the PZT materials and the required high temperature to form the ferroelectric crystalline structure have been obstacles to fabricate efficient photovoltaic devices. Colloidal quantum dots also have fascinating optical and electrical properties such as tailored absorption spectrum, capability of the bandgap engineering due to the wide range of material selection and quantum confinement, and very efficient carrier dynamics called multiple exciton generations. In order to utilize these properties, many researchers have put numerous efforts in colloidal quantum dot photovoltaic research and there has been remarkable progress in the past decade. However, several drawbacks are still remaining to achieve highly efficient photovoltaic device. Traps created on the large surface area, low carrier mobility, and lower open circuit voltage while increasing the absorption of the solar spectrum is main issues of the nanocrystal based photovoltaic effect. To address these issues and to take the advantages of the two materials, this dissertation focused on material synthesis for low cost solution process for both materials, fabrication of various device structures and electrical/optical characterization to understand the underlying physics. We successfully demonstrated lead sulfide quantum dots (PbS QDs) and lead zirconate titanate nanoparticles (PZT NPs) in an aqueous solution and fabricated a photosensitive device. Solution based low-temperature process was used to fabricate a PbS QD and a PZT NP device. We exhibited a superior photoresponse and ferroelectric photovoltaic properties with the novel PZT NP device and studied the physics on domain wall effect and internal polarity effect. PZT NP was mainly investigated because PZT NP device is the first report as a photosensitive device with a successful property demonstration, as we know of. PZT's crystalline structure and the size of the nanocrystals were studied using X-ray diffraction and TEM (Transmission electron microscopy) respectively. We observed < 100 nm of PZT NPs and this result matched with DLS (dynamic light scattering) measurement. We fabricated ferroelectric devices using the PZT NPs for the various optical and electrical characterizations and verified ferroelectric properties including ferroelectric hysteresis loop. We also observed a typical ferroelectric photovoltaic effect from a PZT NP based device which was fabricated on an ITO substrate. We synthesized colloidal quantum dots (CQD) with the inexpensive soluble process. Fabricated PbS QD was used for the hybrid device with PZT thin films. J-V measured and the result shows superior open circuit voltage characteristics compared to conventional PbS QD PV devices, and resulting the improvement of the solar cell efficiency. This Ferroelectrics and Quantum Dots (FE-QDs) device also the first trial and the success as we know of.

Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals

NASA Astrophysics Data System (ADS)

Akkerman, Quinten A.; Rainò, Gabriele; Kovalenko, Maksym V.; Manna, Liberato

2018-05-01

Lead halide perovskites (LHPs) in the form of nanometre-sized colloidal crystals, or nanocrystals (NCs), have attracted the attention of diverse materials scientists due to their unique optical versatility, high photoluminescence quantum yields and facile synthesis. LHP NCs have a `soft' and predominantly ionic lattice, and their optical and electronic properties are highly tolerant to structural defects and surface states. Therefore, they cannot be approached with the same experimental mindset and theoretical framework as conventional semiconductor NCs. In this Review, we discuss LHP NCs historical and current research pursuits, challenges in applications, and the related present and future mitigation strategies explored.

Hybrid systems of AlInP microdisks and colloidal CdSe nanocrystals showing whispering-gallery modes at room temperature

DOE Office of Scientific and Technical Information (OSTI.GOV)

Strelow, Christian; Weising, Simon; Bonatz, Dennis

2014-09-01

We report on the realization of hybrid systems composed of passive optical microdisk resonators prepared from epitaxial layer systems and nanocrystal quantum emitters synthesized by colloidal chemistry. The AlInP disk material allows for the operation in the visible range, as probed by CdSe-based nanocrystals. Photoluminescence spectra at room temperature reveal sets of whispering-gallery modes consistent with finite-difference time-domain simulations. In the experiments, a special sample geometry renders it possible to detect resonant optical modes perpendicular to the disk plane.

Tunable infrared absorption and visible transparency of colloidal aluminum-doped zinc oxide nanocrystals.

PubMed

Buonsanti, Raffaella; Llordes, Anna; Aloni, Shaul; Helms, Brett A; Milliron, Delia J

2011-11-09

Plasmonic nanocrystals have been attracting a lot of attention both for fundamental studies and different applications, from sensing to imaging and optoelectronic devices. Transparent conductive oxides represent an interesting class of plasmonic materials in addition to metals and vacancy-doped semiconductor quantum dots. Herein, we report a rational synthetic strategy of high-quality colloidal aluminum-doped zinc oxide nanocrystals. The presence of substitutional aluminum in the zinc oxide lattice accompanied by the generation of free electrons is proved for the first time by tunable surface plasmon absorption in the infrared region both in solution and in thin films.

Enhanced chemiluminescence of carminic acid-permanganate by CdS quantum dots and its application for sensitive quenchometric flow injection assays of cloxacillin.

PubMed

Khataee, Alireza; Hasanzadeh, Aliyeh; Lotfi, Roya; Joo, Sang Woo

2016-05-15

A novel chemiluminescence (CL) system is introduced based on the oxidation of carminic acid by KMnO4 in acidic conditions. CdS quantum dots (QDs) were synthesized using a facile hydrothermal method which efficiently enhanced the intensity of the CL system. A possible mechanism for the proposed system is presented using the kinetic curves, CL spectra, photoluminescence (PL), and ultraviolet-visible (UV-Vis) analysis. The emission intensity of the KMnO4-carminic acid-CdS QDs system was quenched in the presence of a trace level of cloxacillin. Based on this quenching effect, a novel and sensitive flow injection CL method was developed for determining cloxacillin concentrations. At optimal experimental conditions, the decreased CL intensity had a good linear relation with the cloxacillin concentration in the range of 0.008 to 22.0 mg L(-1). The detection limit (3σ) was 5.8 µg L(-1). The precision of the method was calculated by analyzing samples containing 4.0 mg L(-1) of cloxacillin (n=11), and the relative standard deviations (RSD%) were 2.08%. The feasibility of the method is also demonstrated for determining cloxacillin concentrations in environmental water samples and a pharmaceutical formulation. Copyright © 2016 Elsevier B.V. All rights reserved.

Optically active quantum dots

NASA Astrophysics Data System (ADS)

Gerard, Valerie; Govan, Joseph; Loudon, Alexander; Baranov, Alexander V.; Fedorov, Anatoly V.; Gun'ko, Yurii K.

2015-10-01

The main goal of our research is to develop new types of technologically important optically active quantum dot (QD) based materials, study their properties and explore their biological applications. For the first time chiral II-VI QDs have been prepared by us using microwave induced heating with the racemic (Rac), D- and L-enantiomeric forms of penicillamine as stabilisers. Circular dichroism (CD) studies of these QDs have shown that D- and L-penicillamine stabilised particles produced mirror image CD spectra, while the particles prepared with a Rac mixture showed only a weak signal. It was also demonstrated that these QDs show very broad emission bands between 400 and 700 nm due to defects or trap states on the surfaces of the nanocrystals. These QDs have demonstrated highly specific chiral recognition of various biological species including aminoacids. The utilisation of chiral stabilisers also allowed the preparation of new water soluble white emitting CdS nano-tetrapods, which demonstrated circular dichroism in the band-edge region of the spectrum. Biological testing of chiral CdS nanotetrapods displayed a chiral bias for an uptake of the D- penicillamine stabilised nano-tetrapods by cancer cells. It is expected that this research will open new horizons in the chemistry of chiral nanomaterials and their application in nanobiotechnology, medicine and optical chemo- and bio-sensing.

A novel approach for the fabrication of all-inorganic nanocrystal solids: Semiconductor matrix encapsulated nanocrystal arrays

NASA Astrophysics Data System (ADS)

Moroz, Pavel

Growing fossil fuels consumption compels researchers to find new alternative pathways to produce energy. Along with new materials for the conversion of different types of energy into electricity innovative methods for efficient processing of energy sources are also introduced. The main criteria for the success of such materials and methods are the low cost and compelling performance. Among different types of materials semiconductor nanocrystals are considered as promising candidates for the role of the efficient and cheap absorbers for solar energy applications. In addition to the anticipated cost reduction, the integration of nanocrystals (NC) into device architectures is inspired by the possibility of tuning the energy of electrical charges in NCs via nanoparticle size. However, the stability of nanocrystals in photovoltaic devices is limited by the stability of organic ligands which passivate the surface of semiconductors to preserve quantum confinement. The present work introduces a new strategy for low-temperature processing of colloidal nanocrystals into all-inorganic films: semiconductor matrix encapsulated nanocrystal arrays (SMENA). This methodology goes beyond the traditional ligand-interlinking scheme and relies on the encapsulation of morphologically-defined nanocrystal arrays into a matrix of a wide-band gap semiconductor, which preserves optoelectronic properties of individual nanoparticles. Fabricated solids exhibit excellent thermal stability, which is attributed to the heteroepitaxial structure of nanocrystal-matrix interfaces. The main characteristics and properties of these solids were investigated and compared with ones of traditionally fabricated nanocrystal films using standard spectroscopic, optoelectronic and electronic techniques. As a proof of concept, we. We also characterized electron transport phenomena in different types of nanocrystal films using all-optical approach. By measuring excited carrier lifetimes in either ligand-linked or matrix-encapsulated PbS nanocrystal films containing a tunable fraction of insulating ZnS domains, we uniquely distinguish the dynamics of charge scattering on defects from other processes of exciton dissociation. The measured times are subsequently used to estimate the diffusion length and the carrier mobility for each film type within hopping transport regime. It is demonstrated that nanocrystal films encapsulated into semiconductor matrices exhibit a lower probability of charge scattering than nanocrystal solids cross-linked with either 3-mercaptopropionic acid or 1,2-ethanedithiol molecular linkers. The suppression of carrier scattering in matrix-encapsulated nanocrystal films is attributed to a relatively low density of surface defects at nanocrystal/matrix interfaces. High stability and low density of defects made it possible to fabricate infrared-emitting nanocrystal solids. Presently, an important challenge facing the development of nanocrystal infrared emitters concerns the fact that both the emission quantum yield and the stability of colloidal nanoparticles become compromised when nanoparticle solutions are processed into solids. Here, we address this issue by developing an assembly technique that encapsulates infrared-emitting PbS NCs into crystalline CdS matrices, designed to preserve NC emission characteristics upon film processing. Here, the morphology of these matrices was designed to suppress the nonradiative carrier decay, whereby increasing the exciton lifetime up to 1 mus, and boosting the emission quantum yield to an unprecedented 3.7% for inorganically encapsulated PbS NC solids.

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

DOE PAGES

Beyler, Andrew P.; Bischof, Thomas S.; Cui, Jian; ...

2014-11-19

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here in this study, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS andmore » InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.« less

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

PubMed Central

Beyler, Andrew P.; Bischof, Thomas S.; Cui, Jian; Coropceanu, Igor; Harris, Daniel K.; Bawendi, Moungi G.

2015-01-01

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals. PMID:25409496

Chemical nature and structure of organic coating of quantum dots is crucial for their application in imaging diagnostics

PubMed Central

Bakalova, Rumiana; Zhelev, Zhivko; Kokuryo, Daisuke; Spasov, Lubomir; Aoki, Ichio; Saga, Tsuneo

2011-01-01

Background: One of the most attractive properties of quantum dots is their potential to extend the opportunities for fluorescent and multimodal imaging in vivo. The aim of the present study was to clarify whether the composition and structure of organic coating of nanoparticles are crucial for their application in vivo. Methods: We compared quantum dots coated with non-crosslinked amino-functionalized polyamidoamine (PAMAM) dendrimers, quantum dots encapsulated in crosslinked carboxyl-functionalized PAMAM dendrimers, and silica-shelled amino-functionalized quantum dots. A multimodal fluorescent and paramagnetic quantum dot probe was also developed and analyzed. The probes were applied intravenously in anesthetized animals for visualization of brain vasculature using two-photon excited fluorescent microscopy and visualization of tumors using fluorescent IVIS® imaging (Caliper Life Sciences, Hopkinton, MA) and magnetic resonance imaging. Results: Quantum dots coated with non-crosslinked dendrimers were cytotoxic. They induced side effects in vivo, including vasodilatation with a decrease in mean arterial blood pressure and heart rate. The quantum dots penetrated the vessels, which caused the quality of fluorescent imaging to deteriorate. Quantum dots encapsulated in crosslinked dendrimers had low cytotoxicity and were biocompatible. In concentrations <0.3 nmol quantum dots/kg bodyweight, these nanoparticles did not affect blood pressure and heart rate, and did not induce vasodilatation or vasoconstriction. PEGylation (PEG [polyethylene glycol]) was an indispensable step in development of a quantum dot probe for in vivo imaging, based on silica-shelled quantum dots. The non-PEGylated silica-shelled quantum dots possessed low colloidal stability in high-salt physiological fluids, accompanied by rapid aggregation in vivo. The conjugation of silica-shelled quantum dots with PEG1100 increased their stability and half-life in the circulation without significant enhancement of their size. In concentrations <2.5 nmol/kg bodyweight, these quantum dots did not affect the main physiological variables. It was possible to visualize capillaries, which makes this quantum dot probe appropriate for investigation of mediators of vasoconstriction, vasodilatation, and brain circulation in intact animals in vivo. The multimodal silica-shelled quantum dots allowed visualization of tumor tissue in an early stage of its development, using magnetic resonance imaging. Conclusion: The present study shows that the type and structure of organic/bioorganic shells of quantum dots determine their biocompatibility and are crucial for their application in imaging in vivo, due to the effects of the shell on the following properties: colloidal stability, solubility in physiological fluids, influence of the basic physiological parameters, and cytotoxicity. PMID:21980235

Optical parameters of ITO/TPD/Alq3/Al luminescent structures, containing arrays of CdSe/ZnS colloidal quantum dots

NASA Astrophysics Data System (ADS)

Mikhailov, I. I.; Tarasov, S. A.; Lamkin, I. A.; Tadtaev, P. O.; Kozlovich, L. I.; Solomonov, A. V.; Stepanov, E. M.

2016-08-01

The luminescent organic ITO/TPD/Alq3/Al structures and CdSe/ZnS quantum dots (QD) arrays were created. Electrical and optical properties of the samples were examined. The luminescence of the layers and QD arrays was shown in the range of wavelengths from 400 to 680 nm. Luminescent structures with phosphors corresponding to the emission standards with CRI>98 and with color temperature of 5500 K and 6504 K were created.

Passivation Using Molecular Halides Increases Quantum Dot Solar Cell Performance.

PubMed

Lan, Xinzheng; Voznyy, Oleksandr; Kiani, Amirreza; García de Arquer, F Pelayo; Abbas, Abdullah Saud; Kim, Gi-Hwan; Liu, Mengxia; Yang, Zhenyu; Walters, Grant; Xu, Jixian; Yuan, Mingjian; Ning, Zhijun; Fan, Fengjia; Kanjanaboos, Pongsakorn; Kramer, Illan; Zhitomirsky, David; Lee, Philip; Perelgut, Alexander; Hoogland, Sjoerd; Sargent, Edward H

2016-01-13

A solution-based passivation scheme is developed featuring the use of molecular iodine and PbS colloidal quantum dots (CQDs). The improved passivation translates into a longer carrier diffusion length in the solid film. This allows thicker solar-cell devices to be built while preserving efficient charge collection, leading to a certified power conversion efficiency of 9.9%, which is a new record in CQD solar cells. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Aqueous Exfoliation of Graphite into Graphene Assisted by Sulfonyl Graphene Quantum Dots for Photonic Crystal Applications.

PubMed

Zeng, Minxiang; Shah, Smit A; Huang, Dali; Parviz, Dorsa; Yu, Yi-Hsien; Wang, Xuezhen; Green, Micah J; Cheng, Zhengdong

2017-09-13

We investigate the π-π stacking of polyaromatic hydrocarbons (PAHs) with graphene surfaces, showing that such interactions are general across a wide range of PAH sizes and species, including graphene quantum dots. We synthesized a series of graphene quantum dots with sulfonyl, amino, and carboxylic functional groups and employed them to exfoliate and disperse pristine graphene in water. We observed that sulfonyl-functionalized graphene quantum dots were able to stabilize the highest concentration of graphene in comparison to other functional groups; this is consistent with prior findings by pyrene. The graphene nanosheets prepared showed excellent colloidal stability, indicating great potential for applications in electronics, solar cells, and photonic displays which was demonstrated in this work.

Experimental observation of Fano effect in Ag nanoparticle-CdTe quantum dot hybrid system

NASA Astrophysics Data System (ADS)

Gurung, Sabina; Jayabalan, J.; Singh, Asha; Khan, Salahuddin; Chari, Rama

2018-04-01

We have experimentally measured the optical properties of Ag nanoparticle-CdTe quantum dot hybrid system and compared it with that of bare CdTe quantum dot colloid. It has been shown that the photoluminescence line shape of CdTe quantum dots becomes asymmetric in presence of Ag nanoparticles. The observed changes in the PL spectrum closely match the expected changes in the line shape due to Fano interaction between discrete level and continuum levels. Our experiment shows that a very small fraction of metal nanoparticles in the metal-semiconductor hybrid is sufficient to induce such changes in line shape which is in contrary to the earlier reported theoretical prediction on metal-semiconductor hybrid.

Optical gain in colloidal quantum dots achieved with direct-current electrical pumping

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lim, Jaehoon; Park, Young-Shin; Klimov, Victor Ivanovich

Chemically synthesized semiconductor quantum dots (QDs) can potentially enable solution-processable laser diodes with a wide range of operational wavelengths, yet demonstrations of lasing from the QDs are still at the laboratory stage. An important challenge—realization of lasing with electrical injection—remains unresolved, largely due to fast nonradiative Auger recombination of multicarrier states that represent gain-active species in the QDs. Here in this paper, we present population inversion and optical gain in colloidal nanocrystals realized with direct-current electrical pumping. Using continuously graded QDs, we achieve a considerable suppression of Auger decay such that it can be outpaced by electrical injection. Further, wemore » apply a special current-focusing device architecture, which allows us to produce high current densities (j) up to ~18 A cm -2 without damaging either the QDs or the injection layers. The quantitative analysis of electroluminescence and current-modulated transmission spectra indicates that with j = 3-4 A cm -2 we achieve the population inversion of the band-edge states.« less

Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots.

PubMed

Bertolotti, Federica; Dirin, Dmitry N; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H; Kovalenko, Maksym V; Guagliardi, Antonietta; Masciocchi, Norberto

2016-09-01

Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found.

Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots

NASA Astrophysics Data System (ADS)

Bertolotti, Federica; Dirin, Dmitry N.; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H.; Kovalenko, Maksym V.; Guagliardi, Antonietta; Masciocchi, Norberto

2016-09-01

Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found.

Passively mode-locked Yb fiber laser with PbSe colloidal quantum dots as saturable absorber.

PubMed

Wei, Kaihua; Fan, Shanhui; Chen, Qingguang; Lai, Xiaomin

2017-10-16

A passively mode-locked Yb fiber laser using PbSe colloidal quantum dots (CQDs) as saturable absorber (SA) is experimentally demonstrated. An all-fiber experimental scheme was designed to understand the SA property of PbSe CQDs. The non-saturable loss, modulation depth, and saturable intensity of SA measured were 23%, 7%, and 12 MW/cm 2 , respectively. The PbSe CQDs were sandwiched in a fiber connector, which was further inserted into the Yb fiber laser for mode-locking. As the pump power up to 110 mW, the self-starting mode-locking pulses were observed. Under the pump power of 285 mW, a maximum average laser power with fundamental mode-locking operation was obtained to be 21.3 mW. In this situation, the pulse full width at half maximum (FWHM), pulse repetition rate, and spectral FWHM were measured to be 70 ps, 8.3 MHz, and 4.5 nm, respectively.

Optical gain in colloidal quantum dots achieved with direct-current electrical pumping

NASA Astrophysics Data System (ADS)

Lim, Jaehoon; Park, Young-Shin; Klimov, Victor I.

2018-01-01

Chemically synthesized semiconductor quantum dots (QDs) can potentially enable solution-processable laser diodes with a wide range of operational wavelengths, yet demonstrations of lasing from the QDs are still at the laboratory stage. An important challenge--realization of lasing with electrical injection--remains unresolved, largely due to fast nonradiative Auger recombination of multicarrier states that represent gain-active species in the QDs. Here we present population inversion and optical gain in colloidal nanocrystals realized with direct-current electrical pumping. Using continuously graded QDs, we achieve a considerable suppression of Auger decay such that it can be outpaced by electrical injection. Further, we apply a special current-focusing device architecture, which allows us to produce high current densities (j) up to ~18 A cm-2 without damaging either the QDs or the injection layers. The quantitative analysis of electroluminescence and current-modulated transmission spectra indicates that with j = 3-4 A cm-2 we achieve the population inversion of the band-edge states.

Field-effect enhanced triboelectric colloidal quantum dot flexible sensor

NASA Astrophysics Data System (ADS)

Meng, Lingju; Xu, Qiwei; Fan, Shicheng; Dick, Carson R.; Wang, Xihua

2017-10-01

Flexible electronics, which is of great importance as fundamental sensor and communication technologies for many internet-of-things applications, has established a huge market encroaching into the trillion-dollar market of solid state electronics. For the capability of being processed by printing or spraying, colloidal quantum dots (CQDs) play an increasingly important role in flexible electronics. Although the electrical properties of CQD thin-films are expected to be stable on flexible substrates, their electrical performance could be tuned for applications in flexible touch sensors. Here, we report CQD touch sensors employing polydimethylsiloxane (PDMS) triboelectric films. The electrical response of touching activity is enhanced by incorporating CQD field-effect transistors into the device architecture. Thanks to the use of the CQD thin film as a current amplifier, the field-effect CQD touch sensor shows a fast response to various touching materials, even being bent to a large curvature. It also shows a much higher output current density compared to a PDMS triboelectric touch sensor.

Optical gain in colloidal quantum dots achieved with direct-current electrical pumping

DOE PAGES

Lim, Jaehoon; Park, Young-Shin; Klimov, Victor Ivanovich

2017-11-20

Chemically synthesized semiconductor quantum dots (QDs) can potentially enable solution-processable laser diodes with a wide range of operational wavelengths, yet demonstrations of lasing from the QDs are still at the laboratory stage. An important challenge—realization of lasing with electrical injection—remains unresolved, largely due to fast nonradiative Auger recombination of multicarrier states that represent gain-active species in the QDs. Here in this paper, we present population inversion and optical gain in colloidal nanocrystals realized with direct-current electrical pumping. Using continuously graded QDs, we achieve a considerable suppression of Auger decay such that it can be outpaced by electrical injection. Further, wemore » apply a special current-focusing device architecture, which allows us to produce high current densities (j) up to ~18 A cm -2 without damaging either the QDs or the injection layers. The quantitative analysis of electroluminescence and current-modulated transmission spectra indicates that with j = 3-4 A cm -2 we achieve the population inversion of the band-edge states.« less

Hybrid organic-inorganic inks flatten the energy landscape in colloidal quantum dot solids

NASA Astrophysics Data System (ADS)

Liu, Mengxia; Voznyy, Oleksandr; Sabatini, Randy; García de Arquer, F. Pelayo; Munir, Rahim; Balawi, Ahmed Hesham; Lan, Xinzheng; Fan, Fengjia; Walters, Grant; Kirmani, Ahmad R.; Hoogland, Sjoerd; Laquai, Frédéric; Amassian, Aram; Sargent, Edward H.

2017-02-01

Bandtail states in disordered semiconductor materials result in losses in open-circuit voltage (Voc) and inhibit carrier transport in photovoltaics. For colloidal quantum dot (CQD) films that promise low-cost, large-area, air-stable photovoltaics, bandtails are determined by CQD synthetic polydispersity and inhomogeneous aggregation during the ligand-exchange process. Here we introduce a new method for the synthesis of solution-phase ligand-exchanged CQD inks that enable a flat energy landscape and an advantageously high packing density. In the solid state, these materials exhibit a sharper bandtail and reduced energy funnelling compared with the previous best CQD thin films for photovoltaics. Consequently, we demonstrate solar cells with higher Voc and more efficient charge injection into the electron acceptor, allowing the use of a closer-to-optimum bandgap to absorb more light. These enable the fabrication of CQD solar cells made via a solution-phase ligand exchange, with a certified power conversion efficiency of 11.28%. The devices are stable when stored in air, unencapsulated, for over 1,000 h.

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

DOE PAGES

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.; ...

2017-05-16

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the bandmore » edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. As a result, we expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.« less

Continuous-wave infrared optical gain and amplified spontaneous emission at ultralow threshold by colloidal HgTe quantum dots.

PubMed

Geiregat, Pieter; Houtepen, Arjan J; Sagar, Laxmi Kishore; Infante, Ivan; Zapata, Felipe; Grigel, Valeriia; Allan, Guy; Delerue, Christophe; Van Thourhout, Dries; Hens, Zeger

2018-01-01

Colloidal quantum dots (QDs) raise more and more interest as solution-processable and tunable optical gain materials. However, especially for infrared active QDs, optical gain remains inefficient. Since stimulated emission involves multifold degenerate band-edge states, population inversion can be attained only at high pump power and must compete with efficient multi-exciton recombination. Here, we show that mercury telluride (HgTe) QDs exhibit size-tunable stimulated emission throughout the near-infrared telecom window at thresholds unmatched by any QD studied before. We attribute this unique behaviour to surface-localized states in the bandgap that turn HgTe QDs into 4-level systems. The resulting long-lived population inversion induces amplified spontaneous emission under continuous-wave optical pumping at power levels compatible with solar irradiation and direct current electrical pumping. These results introduce an alternative approach for low-threshold QD-based gain media based on intentional trap states that paves the way for solution-processed infrared QD lasers and amplifiers.

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the bandmore » edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. As a result, we expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.« less

Continuous-wave infrared optical gain and amplified spontaneous emission at ultralow threshold by colloidal HgTe quantum dots

NASA Astrophysics Data System (ADS)

Geiregat, Pieter; Houtepen, Arjan J.; Sagar, Laxmi Kishore; Infante, Ivan; Zapata, Felipe; Grigel, Valeriia; Allan, Guy; Delerue, Christophe; van Thourhout, Dries; Hens, Zeger

2018-01-01

Colloidal quantum dots (QDs) raise more and more interest as solution-processable and tunable optical gain materials. However, especially for infrared active QDs, optical gain remains inefficient. Since stimulated emission involves multifold degenerate band-edge states, population inversion can be attained only at high pump power and must compete with efficient multi-exciton recombination. Here, we show that mercury telluride (HgTe) QDs exhibit size-tunable stimulated emission throughout the near-infrared telecom window at thresholds unmatched by any QD studied before. We attribute this unique behaviour to surface-localized states in the bandgap that turn HgTe QDs into 4-level systems. The resulting long-lived population inversion induces amplified spontaneous emission under continuous-wave optical pumping at power levels compatible with solar irradiation and direct current electrical pumping. These results introduce an alternative approach for low-threshold QD-based gain media based on intentional trap states that paves the way for solution-processed infrared QD lasers and amplifiers.

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

PubMed Central

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.; McNichols, Brett W.; Miller, Elisa M.; Gu, Jing; Nozik, Arthur J.; Sellinger, Alan; Galli, Giulia; Beard, Matthew C.

2017-01-01

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the band edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. We expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications. PMID:28508866

Energy-saving quality road lighting with colloidal quantum dot nanophosphors

NASA Astrophysics Data System (ADS)

Erdem, Talha; Kelestemur, Yusuf; Soran-Erdem, Zeliha; Ji, Yun; Demir, Hilmi Volkan

2014-12-01

Here the first photometric study of road-lighting white light-emitting diodes (WLEDs) integrated with semiconductor colloidal quantum dots (QDs) is reported enabling higher luminance than conventional light sources, specifically in mesopic vision regimes essential to street lighting. Investigating over 100 million designs uncovers that quality road-lighting QD-WLEDs, with a color quality scale and color rendering index ≥85, enables 13-35% higher mesopic luminance than the sources commonly used in street lighting. Furthermore, these QD-WLEDs were shown to be electrically more efficient than conventional sources with power conversion efficiencies ≥16-29%. Considering this fact, an experimental proof-of-concept QD-WLED was demonstrated, which is the first account of QD based color conversion custom designed for street lighting applications. The obtained white LED achieved the targeted mesopic luminance levels in accordance with the road lighting standards of the USA and the UK. These results indicate that road-lighting QD-WLEDs are strongly promising for energy-saving quality road lighting.

Enhanced emission of charged-exciton polaritons from colloidal quantum dots on a SiN/SiO2 slab waveguide

PubMed Central

Xu, Xingsheng; Li, Xingyun

2015-01-01

We investigate the photoluminescence (PL) spectra and the time-resolved PL decay process from colloidal quantum dots on SiN/SiO2 wet etched via BOE (HF:NH4F:H2O). The spectrum displays multi-peak shapes that vary with irradiation time. The evolution of the spectral peaks with irradiation time and collection angle demonstrates that the strong coupling of the charged-exciton emission to the leaky modes of the SiN/SiO2 slab waveguide predominantly produces short-wavelength spectral peaks, resulting in multi-peak spectra. We conclude that BOE etching enhances the charged-exciton emission efficiency and its contribution to the total emission compared with the unetched case. BOE etching smoothes the electron confinement potential, thus decreasing the Auger recombination rate. Therefore, the charged-exciton emission efficiency is high, and the charged-exciton-polariton emission can be further enhanced through strong coupling to the leaky mode of the slab waveguide. PMID:25988709

Coupling effects in the modal emission of colloidal quantum dot microdisk lasers.

NASA Astrophysics Data System (ADS)

Lafalce, Evan; Zheng, Qingji; Lin, Chunhao; Smith, Marcus; Malak, Sidney; Jung, Jaehan; Yoon, Young; Lin, Zhiqun; Tsukruk, Vladimir; Vardeny, Z. Valy

Solution-processed semiconductors such as colloidal quantum dots (CQD) are particularly suited materials for monolithic fabrication of laser microstructures because of their ease of fabrication and compatibility with conventional lithographic techniques. We use the functionality of core/alloyed-shell CQDs to fabricate microdisk lasers of variable size and study the resulting whispering-gallery mode laser emission. In particular we study the effects of near-field coupling on resonant modes of pairs of these lasers with sub-micrometer spacing. We demonstrate the occurrence of lasing modes that originate from the interaction between two such microdisks by means of varying the spatial distribution and magnitude of the gain and loss in the coupled-pair. The transition from emission of modes localized on a single disk to those of the interacting pair is accompanied by coalescence of eigen-frequencies and pump-induced turn-off of lasing, highlighting the role of parity-time symmetry and exceptional point physics. This work was funded by AFOSR through MURI Grant RA 9550-14-1-0037.