Showing papers on "Photoluminescence published in 2004"

Strong coupling in a single quantum dot–semiconductor microcavity system

Abstract: Cavity quantum electrodynamics, a central research field in optics and solid-state physics, addresses properties of atom-like emitters in cavities and can be divided into a weak and a strong coupling regime. For weak coupling, the spontaneous emission can be enhanced or reduced compared with its vacuum level by tuning discrete cavity modes in and out of resonance with the emitter. However, the most striking change of emission properties occurs when the conditions for strong coupling are fulfilled. In this case there is a change from the usual irreversible spontaneous emission to a reversible exchange of energy between the emitter and the cavity mode. This coherent coupling may provide a basis for future applications in quantum information processing or schemes for coherent control. Until now, strong coupling of individual two-level systems has been observed only for atoms in large cavities. Here we report the observation of strong coupling of a single two-level solid-state system with a photon, as realized by a single quantum dot in a semiconductor microcavity. The strong coupling is manifest in photoluminescence data that display anti-crossings between the quantum dot exciton and cavity-mode dispersion relations, characterized by a vacuum Rabi splitting of about 140 microeV.

Bound exciton and donor–acceptor pair recombinations in ZnO

Abstract: The optical properties of excitonic recombinations in bulk, n-type ZnO are investigated by photoluminescence (PL) and spatially resolved cathodoluminescence (CL) measurements. At liquid helium temperature in undoped crystals the neutral donor bound excitons dominate in the PL spectrum. Two electron satellite transitions (TES) of the donor bound excitons allow to determine the donor binding energies ranging from 46 to 73 meV. These results are in line with the temperature dependent Hall effect measurements. In the as-grown crystals a shallow donor with an activation energy of 30 meV controls the conductivity. Annealing annihilates this shallow donor which has a bound exciton recombination at 3.3628 eV. Correlated by magnetic resonance experiments we attribute this particular donor to hydrogen. The Al, Ga and In donor bound exciton recombinations are identified based on doping and diffusion experiments and using secondary ion mass spectroscopy. We give a special focus on the recombination around 3.333 eV, i.e. about 50 meV below the free exciton transition. From temperature dependent measurements one obtains a small thermal activation energy for the quenching of the luminescence of 10 ± 2 meV despite the large localization energy of 50 meV. Spatially resolved CL measurements show that the 3.333 eV lines are particularly strong at crystal irregularities and occur only at certain spots hence are not homogeneously distributed within the crystal contrary to the bound exciton recombinations. We attribute them to excitons bound to structural defects (Y-line defect) very common in II–VI semiconductors. For the bound exciton lines which seem to be correlated with Li and Na doping we offer a different interpretation. Li and Na do not introduce any shallow acceptor level in ZnO which otherwise should show up in donor–acceptor pair recombinations. Nitrogen creates a shallow acceptor level in ZnO. Donor–acceptor pair recombination with the 165 meV deep N-acceptor is found in nitrogen doped and implanted ZnO samples, respectively. In the best undoped samples excited rotational states of the donor bound excitons can be seen in low temperature PL measurements. At higher temperatures we also see the appearance of the excitons bound to the B-valence band, which are approximately 4.7 meV higher in energy. (© 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

Strong coupling between surface plasmons and excitons in an organic semiconductor.

Abstract: We report on the observation of a strong coupling between a surface plasmon and an exciton. Reflectometry experiments are performed on an organic semiconductor, namely, cyanide dye J aggregates, deposited on a silver film. The dispersion lines present an anticrossing that is the signature of a strong plasmon-exciton coupling. Mixed states are formed in a similar way as microcavities polaritons. The Rabi splitting characteristic of this coupling reaches 180 meV at room temperature. The emission of the low energy plasmon-exciton mixed state has been observed and is largely shifted from the uncoupled emission.

Growth mechanism and properties of ZnO nanorods synthesized by plasma-enhanced chemical vapor deposition

Abstract: Uniformly distributed ZnO nanorods have been grown by plasma-enhanced chemical vapor deposition using a two-step process. By controlling the oxygen content in the gas mixture during the nucleation and growth steps, no catalyst is required for the formation of ZnO nanorods. High-resolution transmission electron microscopy studies show that ZnO nanorods are single crystals and that they grow along the c axis of the crystal plane. Alignment of these nanorods with respect to the substrates depends on the lattice mismatch between ZnO and the substrate, the surface electric field, and the amount of defects in the starting nuclei. Room-temperature photoluminescence measurements of these ZnO nanorods have shown ultraviolet peaks at 380 nm with a full width at half-maximum of 106 meV, which are comparable to those found in high-quality ZnO films. Photoluminescence measurements of annealed ZnO nanorods in hydrogen and oxygen atmospheres indicate that the origins of green emission are oxygen vacancies and zinc inter...

Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor

Abstract: The Ba3MgSi2O8:Eu2+, Mn2+ shows three emission colors: 442, 505, and 620 nm. The 442 and 505 nm emission originate from Eu2+ ions, while the 620 nm emission originates from Mn2+ ions. The excitation bands of three emission colors are positioned around 375 nm. Electron paramagnetic resonance measurement demonstrates that Eu2+ ions are occupied with three different Ba2+ sites. The red emission of Mn2+ ions has a long decay time of 750 ms due to persistent energy transfer from oxygen vacancies to Mn2+ ions, while the blue and green bands of Eu2+ ions have decay times of 0.32 and 0.64 μs, respectively. The fabricated white-light emitting diode using a 400-nm-emissive chip with a white-light emitting Ba3MgSi2O8:Eu2+, Mn2+ phosphor shows warm white light and higher color stability against input power in comparison with a commercial GaN-pumped (Y1−xGdx)3(Al1−yGay)5O12:Ce3+ phosphor.

Different origins of visible luminescence in ZnO nanostructures fabricated by the chemical and evaporation methods

Abstract: We prepared ZnO nanostructures using chemical and thermal evaporation methods. The properties of the fabricated nanostructures were studied using scanning electron microscopy, x-ray diffraction, photoluminescence, and electron paramagnetic resonance (EPR) spectroscopy. It was found that the luminescence in the visible region has different peak positions in samples prepared by chemical and evaporation methods. The samples fabricated by evaporation exhibited green luminescence due to surface centers, while the samples fabricated by chemical methods exhibited yellow luminescence which was not affected by the surface modification. No relationship was found between green emission and g∼1.96 EPR signal, while the sample with yellow emission exhibited strong EPR signal.

Superparamagnetic Fe2O3 Beads−CdSe/ZnS Quantum Dots Core−Shell Nanocomposite Particles for Cell Separation

Abstract: This paper describes the synthesis of new nanocomposite nanoparticles that consist of polymer coated γ-Fe2O3 superparamagnetic cores and CdSe/ZnS quantum dots (QDs) shell. A single layer of QDs was bound to the surface of thiol-modified magnetic beads through the formation of thiol−metal bonds to form luminescent/magnetic nanocomposite particles. Transmission electron microscopy (TEM) and energy disperse spectroscopy (EDS) were used to characterize the size, size distribution, and composition of the luminescent/magnetic nanoparticles. Their average diameter was 30 nm with a size variation of ±15%. The nanoparticles were modified with carboxylic groups to increase their miscibility in aqueous solution. A 3-fold decrease in the luminescence quantum yield of the luminescent/magnetic particles and a slight blue shift in their emission peaks compared to individual luminescent QDs were observed. However, the particles were bright and were easily observed using a conventional fluorescence microscope. Additionall...

Eu2+-doped Ca-α-SiAlON: A yellow phosphor for white light-emitting diodes

Abstract: In this letter, a yellow oxynitride phosphor α-SiAlON with compositions of Ca0.625EuxSi0.75−3xAl1.25+3xOxN16−x (Ca-α-SiAlON:Eu, x=0–25) was prepared by gas pressure sintering. The diffuse reflection spectrum, photoluminescence spectrum, and chromaticity of the powder phosphors were presented. It absorbs light efficiently in the UV–visible spectral region, and shows a single intense broadband emission at 583–603nm. This phosphor may become a good candidate for creating white light, typically warm white light, when coupled to a blue light-emitting diode (λem=450nm).

Photoluminescence and Electron Paramagnetic Resonance of ZnO Tetrapod Structures

Abstract: ZnO tetrapod nanostructures have been prepared by the evaporation of Zn in air (no flow), dry and humid argon flow, and dry and humid nitrogen flow. Their properties have been investigated using scanning electron microscopy (SEM), X-ray diffraction (XRD), photoluminescence (PL) and photoluminescence excitation (PLE) spectroscopies (at different temperatures), and electron paramagnetic resonance (EPR) spectroscopy at –160 °C and room temperature. It is found that the fabrication conditions significantly influence the EPR and PL spectra obtained. While a g = 1.96 EPR signal is present in some of the samples, green PL emission can be observed from all the samples. Therefore, the green emission in our samples does not originate from the commonly assumed transition between a singly charged oxygen vacancy and a photoexcited hole [K. Vanheusden, C. H. Seager, W. L. Warren, D. R. Tallant, J. A. Voigt, Appl. Phys. Lett. 1996, 68, 403]. However, the green emission can be suppressed by coating the nanostructures with a surfactant for all fabrication conditions, which indicates that this emission originates from surface defects.

Annealing effect on the property of ultraviolet and green emissions of ZnO thin films

Abstract: The mechanism of ultraviolet (UV) and green emission of ZnOthin filmsdeposited on (001) sapphire substrates by pulsed laser deposition was investigated by using postannealing treatment at various annealing temperatures after deposition.Structural, electrical, and optical properties of ZnOfilms have been also observed. As the postannealing temperature increased, the intensity of UV (380 nm) peak and the carrier concentration were decreased while the intensity of the visible (about 490–530 nm) peak and the resistivity were increased. The role of oxygen in ZnOthin film during the annealing process was important to the change of optical properties. The mechanism of the luminescence suggested that UVluminescence of ZnOthin film was related to the transition from near band edge to valence band, and green luminescence of ZnOthin film was caused by the transition from deep donor level to valence band due to oxygen vacancies. The activation energy derived by using the variation of green emission intensity was 1.19 eV.

Energy-transfer pumping of semiconductor nanocrystals using an epitaxial quantum well.

Abstract: As a result of quantum-confinement effects, the emission colour of semiconductor nanocrystals can be modified dramatically by simply changing their size1,2. Such spectral tunability, together with large photoluminescence quantum yields and high photostability, make nanocrystals attractive for use in a variety of light-emitting technologies—for example, displays, fluorescence tagging3, solid-state lighting and lasers4. An important limitation for such applications, however, is the difficulty of achieving electrical pumping, largely due to the presence of an insulating organic capping layer on the nanocrystals. Here, we describe an approach for indirect injection of electron–hole pairs (the electron–hole radiative recombination gives rise to light emission) into nanocrystals by non-contact, non-radiative energy transfer from a proximal quantum well that can in principle be pumped either electrically or optically. Our theoretical and experimental results indicate that this transfer is fast enough to compete with electron–hole recombination in the quantum well, and results in greater than 50 per cent energy-transfer efficiencies in the tested structures. Furthermore, the measured energy-transfer rates are sufficiently large to provide pumping in the stimulated emission regime, indicating the feasibility of nanocrystal-based optical amplifiers and lasers based on this approach.

Photoluminescence Properties of SnO2 Nanoparticles Synthesized by Sol−Gel Method

Abstract: Nanocrystalline SnO2 particles have been synthesized by a simple sol−gel method. The structural and optical properties of these SnO2 particles are investigated using X-ray powder diffraction, trans...

Emission Intensity Dependence and Single-Exponential Behavior In Single Colloidal Quantum Dot Fluorescence Lifetimes

Abstract: We present measurements of photoluminescence decay dynamics from single colloidal CdSe quantum dots. We find that the decays fluctuate in time with decay rates that correlate with time-averaged emission intensities. Moreover, the decays measured by selecting only those photons collected while the single quantum dot emission intensity was near its maximum yields single-exponential dynamics. We find that the “maximum-intensity” decays are nearly identical across different independently synthesized samples of nearly the same size. The combination of single-exponential kinetics and decays that are reproducible across samples leads us to speculate that it is the radiative lifetime that is measured and that the quantum yield of a single dot near its maximum emission intensity is close to unity. The variations in decay rates with time and their correlation with emission intensity indicate these intensity time trajectories primarily reflect fluctuations in nonradiative relaxation pathways.

Plasmon emission in photoexcited gold nanoparticles

Abstract: Light emission at the particle plasmon frequency is observed in optically excited spherical gold nanoparticles. We find a photoluminescence efficiency of ${10}^{\ensuremath{-}6}$, which is essentially independent of particle size and four orders of magnitude higher than the efficiencies determined from metal films. Our experimental findings are explained with a process in which excited $d$-band holes recombine nonradiatively with $\mathit{sp}$ electrons, emitting particle plasmons. These plasmons subsequently radiate, giving rise to the photoluminescence observed in the experiment. We determine the quantum efficiencies involved in this process.

Synthesis and Characterization of Colloidal CuInS2 Nanoparticles from a Molecular Single-Source Precursor

Abstract: Thermal decomposition of the molecular single-source precursor (PPh3)2CuIn(SEt)4 in the presence of hexanethiol in dioctylphthalate forms colloidal CuInS2 at 200 °C. The colloidal solution displays size-dependent quantum confinement behavior in the absorption and photoluminescence spectra. The average size of the nanocrystals can be increased from 2 to 4 nm by raising the reaction temperature from 200 °C to 250 °C. The nanoparticles are capped with hexanethiol ligands; these ligands can be exchanged with trioctylphosphine oxide or pyridine. The nature of the surface-capping ligands has a significant effect on the photoluminescence emission intensity. Investigation of the effect of synthesis parameters and postsynthesis treatments on the optical properties of the nanocrystals leads to the conclusion that the room-temperature emission originates in donor−acceptor defects.

Electrochemistry and optical absorbance and luminescence of molecule-like Au38 nanoparticles

Abstract: This paper describes electrochemical and spectroscopic properties of a well-characterized, synthetically accessible, 1.1 nm diam Au nanoparticle, Au(38)(PhC(2)S)(24), where PhC(2)S is phenylethylthiolate. Properties of other Au(38) nanoparticles made by exchanging the monolayer ligands with different thiolate ligands are also described. Voltammetry of the Au(38) nanoparticles in CH(2)Cl(2) reveals a 1.62 V energy gap between the first one-electron oxidation and the first reduction. Based on a charging energy correction of ca. 0.29 V, the indicated HOMO-LUMO gap energy is ca. 1.33 eV. At low energies, the optical absorbance spectrum includes peaks at 675 nm (1.84 eV) and 770 nm (1.61 eV) and an absorbance edge at ca. 1.33 eV that gives an optical HOMO-LUMO gap energy that is consistent with the electrochemical estimate. The absorbance at lowest energy is bleached upon electrochemical depletion of the HOMO level. The complete voltammetry contains two separated doublets of oxidation waves, indicating two distinct molecular orbitals, and two reduction steps. The ligand-exchanged nanoparticle Au(38)(PEG(135)S)(13)(PhC(2)S)(11), where PEG(135)S is -SCH(2)CH(2)OCH(2)CH(2)OCH(3), exhibits a broad (1.77-0.89 eV) near-IR photoluminescence band resolvable into maxima at 902 nm (1.38 eV) and 1025 nm (1.2 eV). Much of the photoluminescence occurs at energies less than the HOMO-LUMO gap energy. A working model of the energy level structure of the Au(38) nanoparticle is presented.

Exciton regeneration at polymeric semiconductor heterojunctions.

Abstract: Control of the band-edge offsets at heterojunctions between organic semiconductors allows efficient operation of either photovoltaic or light-emitting diodes. We investigate systems where the exciton is marginally stable against charge separation and show via E-field-dependent time-resolved photoluminescence spectroscopy that excitons that have undergone charge separation at a heterojunction can be efficiently regenerated. This is because the charge transfer produces a geminate electron-hole pair (separation 2.2 –3.1 nm) which may collapse into an exciplex and then endothermically (EA � 100–200 meV) back transfer towards the exciton. DOI: 10.1103/PhysRevLett.92.247402

Enhancement Effect of Illumination on the Photoluminescence of Water-Soluble CdTe Nanocrystals: Toward Highly Fluorescent CdTe/CdS Core−Shell Structure

Abstract: A strong photoluminescence enhancement effect of illumination on CdTe nanocrystals stabilized by thioglycolic acid (TGA) was observed. Under optimized conditions, the fluorescence quantum yield of CdTe nanocrystals in aqueous solution reached 85% at room temperature. Optical measurements indicated that the photodegradation of TGA rather than NCs was the main reason for the PL enhancement effect since sulfide ions released from TGA during illumination coordinated with cadmium ions on the surface of CdTe and formed a shell structure of CdS there. X-ray photoelectron spectroscopic results further proved the formation of CdS shell on the CdTe core during illumination. The colloidal solution of CdTe/CdS core−shell nanocrystals with photoluminescence quantum yield higher than 80% turned out to be very stable. Therefore, the current investigations not only reveal the PL enhancement effect of illumination, but also provide a useful synthetic route for producing water-soluble and highly fluorescent CdTe/CdS core−shell nanocrystals

Electrochemistry and electrogenerated chemiluminescence of CdTe nanoparticles

Abstract: Differential pulse voltammetry (DPV) of TOPO-capped CdTe nanoparticles (NPs) in dichloromethane and a mixture of benzene and acetonitrile showed two anodic and one cathodic peaks of the NPs themselves and an additional anodic peak resulting from the oxidation of reduced NPs. The electrochemical band gap (∼2.1 eV) between the first anodic and cathodic DPV peaks was close to the value (2 eV) obtained from the absorption spectrum. Electrogenerated chemiluminescence (ECL) of CdTe NPs was highly intense for scans into the negative potential region in dichloromethane. The fact that the ECL peak occurs at about the same wavelength as the band-edge photoluminescence (PL) peak indicates that, in contrast to CdSe NPs, the CdTe NPs as synthesized had no deep surface traps that can cause a substantially red shifted ECL.

Syntheses, structures, and photoluminescence of a novel class of d10 metal complexes constructed from pyridine-3,4-dicarboxylic acid with different coordination architectures.

Abstract: Two novel d10 metal coordination polymers [Zn(PDB)]n (1) and [Cd3(PDB)2(OH)2(H2O)2]n (2) (H2PDB = pyridine-3,4-dicarboxylic acid) have been synthesized under hydrothermal conditions and characterized by elemental analysis, IR, TG analysis, and single-crystal X-ray diffraction. Crystal data for 1: C7H3NO4Zn, orthorhombic Pna21, a = 8.423(17) A, b = 6.574(13) A, c = 12.899(3) A, Z = 4. Crystal data for 2: C14H12N2O12Cd3, monoclinic C2/c, a = 20.130(4) A, b = 6.692(13) A, c = 13.081(3) A, β = 102.78(3)°, Z = 4. Both compounds exhibit novel three-dimensional frameworks. Compound 1 not only possesses a one-dimensional rectangular channel but also contains infinite double-stranded helical chains. Compound 2 has two different types of channels, one being built up from pyridine rings and {CdO5N} and {CdO6} building units and the other being constructed from pyridine rings and {CdO5N} building units. Furthermore, both compounds show strong photoluminescence properties at room temperature.

Photoluminescence and polarized photodetection of single ZnO nanowires

Abstract: Single crystal ZnO nanowires are synthesized and configured as field-effect transistors. Photoluminescence and photoconductivity measurements show defect-related deep electronic states giving rise to green-red emission and absorption. Photocurrent temporal response shows that current decay time is significantly prolonged in vacuum due to a slower oxygen chemisorption process. The photoconductivity of ZnO nanowires is strongly polarization dependent. Collectively, these results demonstrate that ZnO nanowire is a remarkable optoelectronic material for nanoscale device applications.

Preparation and Luminescence Spectra of Calcium- and Rare-Earth (R = Eu, Tb, and Pr)-Codoped α-SiAlON Ceramics

Abstract: Rare-earth-doped oxynitride or nitride compounds have been reported to be luminescent and may then serve as new phosphors with good thermal and chemical stabilities. In this work, we report the photoluminescence (PL) spectra of europium-, terbium-, and praseodymium-doped Ca-α-SiAlON ceramics. The highly dense ceramics were prepared by hot pressing at 1750°C for 1 h under 20 MPa in a nitrogen atmosphere. Europium-doped Ca-α-SiAlON displayed a single broad emission band peaking at λ = 550-590 nm depending on the europium concentration. The emission bands in the spectra of europium-doped Ca-α-SiAlONs were assigned to the allowed transition of Eu 2+ from the lowest crystal field component of 4f 6 5d to 8 S 7/2 (4f 7 ) ground-state level. The emission spectra of terbium- and praseodymium-doped Ca-α-SiAlON ceramics both consisted of several sharp lines, which were attributed to the 5 D 4 → 7 F j (j = 3, 4, 5, 6) transitions of Tb 3+ and 3 P o → 3 H j (j = 3, 4, 5) transitions of Pr 3+ , respectively. In particular, the terbium-doped α-SiAlON ceramics showed a strong green emission among these phosphors.

Color Tuning in Benzo[1,2,5]thiadiazole‐Based Small Molecules by Amino Conjugation/Deconjugation: Bright Red‐Light‐Emitting Diodes

Abstract: Bipolar compounds (referred to in general as btza) containing a benzo[1,2,5]thiadiazole core and peripheral diarylamines and/or 4-tert-butylphenyl moieties have been synthesized via palladium-catalyzed cross-coupling reactions of 4,7-dibromobenzo[1,2,5]thiadiazole with appropriate stannyl compounds. These compounds are fluorescent and the emission color ranges from green to red. The fluorescence of the compounds originates from a charge-transfer process and exhibits solvatochromism. These red-light-emitting materials are amorphous and devices of different configurations were fabricated: I) ITO/btza/TPBI/Mg:Ag; II) ITO/btza/Alq3/Mg:Ag; III) ITO/btza/Mg:Ag (where ITO = indium tin oxide, TPBI = 1,3,5-tris(N-phenylbezimidazol-2-yl)benzene, and Alq3 = tris(8-hydroxyquinoline)aluminum). The performance of some of the red-light-emitting devices appears to be very promising.

Strong blue photoluminescence and ECL from OH-terminated PAMAM dendrimers in the absence of gold nanoparticles.

Abstract: A product showing strong blue photoluminescence was obtained by oxidation of OH-terminated PAMAM dendrimers, such as G4-OH, G2-OH, and G0-OH, with HAuCl4 or (NH4)2S2O8. The fluorescence emission spectrum peaked at 450 nm, while the excitation maximum was at 380 nm, independent of the generation of dendrimer. The product also shows two weak electrogenerated chemiluminescence (ECL) signals upon cycling the potential between about 1.2 and −1.7 V.

One-Pot Synthesis of High-Quality Zinc-Blende CdS Nanocrystals

Abstract: This paper reports a one-pot synthetic method for producing CdS nanocrystals. We have demonstrated that the nanocrystal nucleation and growth stages can be automatically separated in a homogeneous system with the presence of nucleation initiators. Accelerators used for more than 70 years in rubber vulcanization (i.e., tetraethylthiuram disulfides, and 2,2‘-dithiobisbenzothiazole) were found to be effective nucleation initiators for CdS nanocrystal synthesis. The as-prepared CdS nanocrystals are highly monodisperse and possess a zinc blende crystal structure. The quantum yield of the band-gap photoluminescence is up to 12% when the surface-trap emission was totally eliminated after a gentle oxidation under laboratory fluorescent light.

Unique optical properties of AlGaN alloys and related ultraviolet emitters

Abstract: Deep UV photoluminescence spectroscopy has been employed to study the optical properties of AlxGa1−xN alloys (0⩽x⩽1). The emission intensity with polarization of E⊥c and the degree of polarization were found to decrease with increasing x. This is a consequence of the fact that the dominant band edge emission in GaN (AlN) is with polarization of E⊥c(E∥c). Our experimental results suggest that the decreased emission efficiency in AlxGa1−xN alloys and related UV emitters could also be related with their unique polarization property, i.e., the intensity of light emission with polarization of E⊥c decreases with x. It is thus concluded that UV emitters with AlGaN alloys as active layers have very different properties from InGaN and other semiconductor emitters.