Tailoring local density of optical states to control emission intensity and anisotropy of quantum dots in hybrid photonic-plasmonic templates

We report results of controlled tuning of the local density of states (LDOS) in versatile, flexible, and hierarchical self assembled plasmonic templates. Using 5 nm diameter gold (Au) spherical nanoantenna within a polymer template randomly dispersed with quantum dots, we show how the photoluminescence intensity and lifetime anisotropy of these dots can be significantly enhanced through LDOS tuning. Finite difference time domain simulations corroborate the experimental observations and extend the regime of enhancement to a wider range of geometric and spectral parameters bringing out the versatility of these functional plasmonic templates. It is also demonstrated how the templates act as plasmonic resonators for effectively engineer giant enhancement of the scattering efficiency of these nano antenna embedded in the templates. Our work provides an alternative method to achieve spontaneous emission intensity and anisotropy enhancement with true nanoscale plasmon resonators. (C) 2015 AIP Publishing LLC.

IMF control of cusp proton emission intensity and dayside convection: implications for component and anti-parallel reconnection

We study a brightening of the Lyman-alpha emission in the cusp which occurred in response to a short-lived southward turning of the interplanetary magnetic field (IMF) during a period of strongly enhanced solar wind plasma concentration. The cusp proton emission is detected using the SI-12 channel of the FUV imager on the IMAGE spacecraft. Analysis of the IMF observations recorded by the ACE and Wind spacecraft reveals that the assumption of a constant propagation lag from the upstream spacecraft to the Earth is not adequate for these high time-resolution studies. The variations of the southward IMF component observed by ACE and Wind allow for the calculation of the ACE-to-Earth lag as a function of time. Application of the derived propagation delays reveals that the intensity of the cusp emission varied systematically with the IMF clock angle, the relationship being particularly striking when the intensity is normalised to allow for the variation in the upstream solar wind proton concentration. The latitude of the cusp migrated equatorward while the lagged IMF pointed southward, confirming the lag calculation and indicating ongoing magnetopause reconnection. Dayside convection, as monitored by the SuperDARN network of radars, responded rapidly to the IMF changes but lagged behind the cusp proton emission response: this is shown to be as predicted by the model of flow excitation by Cowley and Lockwood (1992). We use the numerical cusp ion precipitation model of Lockwood and Davis (1996), along with modelled Lyman-_ emission efficiency and the SI-12 instrument response, to investigate the effect of the sheath field clock angle on the acceleration of ions on crossing the dayside magnetopause. This modelling reveals that the emission commences on each reconnected field line 2–2.5min after it is opened and peaks 3–5 min after it is opened. We discuss how comparison of the Lyman-alpha intensities with oxygen emissions observed simultaneously by the SI-13 channel of the FUV instrument offers an opportunity to test whether or not the clock angle dependence is consistent with the “component” or the “anti-parallel” reconnection hypothesis.

Optical emission characteristics and mode transitions in low-frequency inductively coupled plasmas

An attempt was made to investigate the optical emission spectra of atomic, molecular, and ionic species in low-frequency, high-density ICP discharges in pure nitrogen, ar con gases, and gas mixtures Ar+H2, N2+Ar, and N2+H2. The excited species were identified by in situ optical emission intensity (OEI) measurements in the discharge chamber. In general, significant results were obtained.

Role of the triplet state in the green emission peak of polyfluorene films: A time evolution study

The blue emission of ethyl-hexyl substituted polyfluorene (PF2/6) films is accompanied by a low energy green emission peak around 500 nm in inert atmosphere. The intensity of this 500 nm peak is large in electroluminescence (EL) compared to photoluminescence (PL)measurements. Furthermore, the green emission intensity reduces dramatically in the presence of molecular oxygen. To understand this, we have modeled various nonradiative processes by time dependent quantum many body methods. These are (i) intersystem crossing to study conversion of excited singlets to triplets leading to a phosphorescence emission, (ii) electron-hole recombination (e-hR) process in the presence of a paramagnetic impurity to follow the yield of triplets in a polyene system doped with paramagnetic metal atom, and (iii) quenching of excited triplet states in the presence of oxygen molecules to understand the low intensity of EL emission in ambient atmosphere, when compared with that in nitrogen atmosphere. We have employed the Pariser-Parr-Pople Hamiltonian to model the molecules and have invoked electron-electron repulsions beyond zero differential approximation while treating interactions between the organic molecule and the rest of the system. Our time evolution methods show that there is a large cross section for triplet formation in the e-hR process in the presence of paramagnetic impurity with degenerate orbitals. The triplet yield through e-hR process far exceeds that in the intersystem crossing pathway, clearly pointing to the large intensity of the 500 nm peak in EL compared to PL measurements. We have also modeled the triplet quenching process by a paramagnetic oxygen molecule which shows a sizable quenching cross section especially for systems with large sizes. These studies show that the most probable origin of the experimentally observed low energy EL emission is the triplets.

Defects induced enhancement of Eu3+Emission in yttria (Y2O3:Eu3+)

Bixbyite type Y2O3:Eu3+ apart from being the efficient red phosphor extensively used in trichromatic fluorescent lamps, it is a typical system one can apply Jorgensen's refined electron spin pairing theory. This can be used to explain the enhancement in Eu3+ emission intensity observed with the aliovalent substitution in the yttria host matrix. Results based on these are explained qualitatively by considering a simple configurational coordinate model. Futhermore, an insight into the different types of defects induced with the aliovalent substitution in the yttria lattice has become possible with EPR probe.

Room temperature synthesis of Mn2+ doped ZnS d-dots and observation of tunable dual emission: Effects of doping concentration, temperature, and ultraviolet light illumination

Mn2+ doped (0-50.0 molar %) ZnS d-dots have been synthesized in water medium by using an environment friendly low cost chemical technique. Tunable dual emission in UV and yellow-orange regions is achieved by tailoring the Mn2+ doping concentration in the host ZnS nanocrystal. The optimum doping concentration for achieving efficient photoluminescence (PL) emission is determined to be similar to 1.10 (at. %) corresponding to 40.0 (molar %) of Mn2+ doping concentration used during synthesis. The mechanism of charge transfer from the host to the dopant leading to the intensity modulated tunable (594-610 nm) yellow-orange PL emission is straightforwardly understood as no capping agent is used. The temperature dependent PL emission measurements are carried out, viz., in 1.10 at. % Mn2+ doped sample and the experimental results are explained by using a theoretical PL emission model. It is found that the ratio of non-radiative to radiative recombination rates is temperature dependent and this phenomenon has not been reported, so far, in Mn2+ doped ZnS system. The colour tuning of the emitted light from the samples are evident from the calculated chromaticity coordinates. UV light irradiation for 150 min in 40.0 (molar %) Mn2+ doped sample shows an enhancement of 33% in PL emission intensity. (C) 2013 American Institute of Physics. http://dx.doi.org/10.1063/1.4795779]

FIELD EMISSION EFFICIENCY OF A CARBON NANOTUBE ARRAY UNDER PARASITIC NONLINEARITIES

Carbon Nanotubes (CNTs) grown on substrates are potential electron sources in field emission applications. Several studies have reported the use of CNTs in field emission devices, including field emission displays, X-ray tube, electron microscopes, cathode-ray lamps, etc. Also, in recent years, conventional cold field emission cathodes have been realized in micro-fabricated arrays for medical X-ray imaging. CNTbased field emission cathode devices have potential applications in a variety of industrial and medical applications, including cancer treatment. Field emission performance of a single isolated CNT is found to be remarkable, but the situation becomes complex when an array of CNTs is used. At the same time, use of arrays of CNTs is practical and economical. Indeed, such arrays on cathode substrates can be grown easily and their collective dynamics can be utilized in a statistical sense such that the average emission intensity is high enough and the collective dynamics lead to longer emission life. The authors in their previous publications had proposed a novel approach to obtain stabilized field emission current from a stacked CNT array of pointed height distribution. A mesoscopic modeling technique was employed, which took into account electro-mechanical forces in the CNTs, as well as transport of conduction electron coupled with electron phonon induced heat generation from the CNT tips. The reported analysis of pointed arrangements of the array showed that the current density distribution was greatly localized in the middle of the array, the scatter due to electrodynamic force field was minimized, and the temperature transients were much smaller compared to those in an array with random height distribution. In the present paper we develop a method to compute the emission efficiency of the CNT array in terms of the amount of electrons hitting the anode surface using trajectory calculations. Effects of secondary electron emission and parasitic capacitive nonlinearity on the current-voltage signals are accounted. Field emission efficiency of a stacked CNT array with various pointed height distributions are compared to that of arrays with random and uniform height distributions. Effect of this parasitic nonlinearity on the emission switch-on voltage is estimated by model based simulation and Monte Carlo method.

Fine-Tuning Dual Emission and Aggregation-Induced Emission Switching in NPI-BODIPY Dyads

Three new NPI-BODIPY dyads 1-3 (NPI = 1,8-naphthalimide, BODIPY = boron-dipyrromethene) were synthesized, characterized, and studied. The NPI and BODIPY moieties in these dyads are electronically separated by oxoaryl bridges, and the compounds only differ structurally with respect to methyl substituents on the BODIPY fluorophore. The NPI and BODIPY moieties retain their optical features in molecular dyads 1-3. Dyads 1-3 show dual emission in solution originating from the two separate fluorescent units. The variations of the dual emission in these compounds are controlled by the structural flexibilities of the systems. Dyads 13, depending on their molecular flexibilities, show considerably different spectral shapes and dissimilar intensity ratios of the two emission bands. The dyads also show significant aggregation-induced emission switching (AIES) on formation of nano-aggregates in THF/H2O with changes in emission color from green to red. Whereas the flexible and aggregation-prone compound 1 shows AIES, rigid systems with less favorable intermolecular interactions (i.e., 2 and 3) show aggregation-induced quenching of emission. Correlations of the emission intensity and structural flexibility were found to be reversed in solution and aggregated states. Photophysical and structural investigations suggested that intermolecular interactions (e. g., pi-pi stacking) play a major role in controlling the emission of these compounds in the aggregated state.

Effect of thermal annealing on dual photoluminescence emission characteristics of chemically synthesized uncapped Mn2+ doped ZnS quantum dots

Dual photoluminescence (PL) emission characteristics of Mn2+ doped ZnS (ZnS:Mn) quantum dots (QDs) have drawn a lot of attention recently. However, here we report the effect of thermal annealing on the PL emission characteristics of uncapped ZnS:Mn QDs of average sizes similar to 2-3 nm, synthesized by simple chemical precipitation method by using de-ionized (DI) water at room temperature. As-synthesized samples show dual PL emissions, having one UV PL band centred at similar to 400 nm and the other in the visible region similar to 610 nm. But when the samples are isochronally annealed for 2 h at 100-600 degrees C temperature range in air, similar to 90% quenching of Mn2+ related visible PL emission intensity takes place at the annealing temperature of 600 degrees C. X-ray diffraction data show that the as-synthesized cubic ZnS has been converted to wurtzite ZnO at 600 degrees C annealing temperature. The nanostructural properties of the samples are also determined by transmission electron micrograph, electron probe micro-analyser and UV-vis spectrophotometry. The photocatalytic property of the annealed ZnS:Mn sample has been demonstrated and photo-degradation efficiency of the as-synthesized and 600 degrees C annealed ZnS:Mn sample has been found out to be similar to 35% and similar to 61%, respectively, for the degradation of methylene blue dye under visible light irradiation. The synthesized QDs may find significant applications in future optoelectronic devices. (C) 2014 Elsevier B.V. All rights reserved.

Long range emission enhancement and anisotropy in coupled quantum dots induced by aligned gold nanoantenna

Quantum dot arrays have been projected as the material of choice for next generation displays and photodetectors. Extensive ongoing research aims at improving optical and electrical efficiencies of such devices. We report experimental results on non-local long range emission intensity enhancement and anisotropy in quantum dot assemblies induced by isolated and partially aligned gold nanoantennas. Spatially resolved photoluminescence clearly demonstrate that the effect is maximum, when the longitudinal surface plasmon resonance of the nanoantenna is resonant with the emission maxima of the quantum dots. We estimated the decay length of this enhancement to be similar to 2.6 mu m, which is considerably larger than the range of near field interaction of metal nanoantenna. Numerical simulations qualitatively capture the near field behavior of the nanorods but fail to match the experimentally observed non-local effects. We have suggested how strong interactions of quantum dots in the close packed assemblies, mediated by the nanoantennas, could lead to such observed behavior. (C) 2014 AIP Publishing LLC.

Simple chemical aqueous synthesis of dahlia nanoflower consisting of finger-like ZnO nanorods and observation of stable ultraviolet photoluminescence emission

In this work, we have reported the synthesis of dahlia flower-like ZnO nanostructures consisting of human finger-like nanorods by the hydrothermal method at 120 degrees C and without using any capping agent. Optical properties of the samples, including UV-vis absorption and photoluminescence (PL) emission characteristics are determined by dispersing the samples in water as well as in ethanol media. The quenching of PL emission intensity along-with the red shifting of the PL emission peak are observed when the samples are dispersed in water in comparison to those obtained after dispersing the samples in ethanol. It has been found that PL emission characteristic, particularly the spectral nature of PL emission, of the samples remains almost unaltered (except some improvement in UV PL emission) even after thermally annealing it for 2 h at the temperature of 300 degrees C. Also the synthesized powder samples, kept in a plastic container, showed a very stable PL emission even after 15 months of synthesis. Therefore, the synthesized samples might be useful for their applications in future optoelectronics devices. (C) 2014 Elsevier Ltd. All rights reserved.

Enhancement Mechanism of Fluorescence Intensity in Presence of Plasmonic Nanoparticles

The emission intensity of fluorophore molecule may change in presence of strong plasmon field induced by nanoparticles. The enhancement intensity is optimized through selective clustering or functionalization of nanoparticles in closed vicinity of fluorophore. Our study is aimed at understanding the enhancement mechanism of fluorescence intensity in presence of gold nanoparticles to utilize it in molecular sensing and in situ imaging in the microfluidic lab-on-chip device. Related phenomena are studied in situ in a microfluidic channel via fluorescence imaging. Detailed analysis is carried out to understand the possible mechanism of enhancement of fluorescence due to nanoparticles. In the present experimental study we show that SYTO9 fluorescence intensity increased in presence of Au nanoparticles of similar to 20 nm diameter. The fluorescence intensity is 20 time more compared to that in absence of Au nanoparticles. The enhancement of fluorescence intensity is attributed to the plasmonic resonance of Au nanoparticle at around the fluorescence emission wavelength. Underlying fundamental mechanism via dipole interaction model is explored for quantitative correlation of plasmonic enhancement properties.

Cyclotron harmonic emission in a Penning discharge

Microwave noise emission at the harmonics of the electron cyclotron frequency from the magnetized plasma column of a Penning discharge is investigated experimentally. The harmonic emission spectrum is observed using oxygen gas in a variety of discharge configurations. It is found that grid stabilization of the plasma column has very little effect on the emission spectrum. Measurements of the shape and location of the harmonic emission lines are described in detail. On the basis of a microwave interferometer measurement of the electron density, it is concluded that the existence of a hybrid layer somewhere on the plasma column is a necessary condition for the observation of harmonic emission. The relaxation time and the cathode voltage dependence of the harmonic emission are investigated using a pulse modulation technique. It is found that the emission intensity increases rapidly with the magnitude of the cathode voltage and that the relaxation time decreases with increasing neutral gas pressure. High intensity nonharmonic radiation is observed and identified as resulting from a beam-plasma wave instability thereby eliminating the same instability as a possible source of the harmonic emission. It is found that the collective experimental results are in reasonable agreement with the single particle electrostatic radiation theory of Canobbio and Croci.

Upconversion emission in Er3+ doped novel bismuthate glass

Novel Er3+-doped bismuth lead strontiam glass was fabricated and characterized, and the absorption spectrum and upconversion spectrum of the glass were studied. The Judd-Ofelt intensity parameters Omega(t)(t = 2, 4, 6) were found to be Omega(2) = 3.27 x 10(-20) cm(2), Omega(4) = 1.15 x 10(-20) cm(2), and Omega(6) = 0.38 x 10(-20) cm(2). The oscillator strength, the spontaneous transition probabilities, the fluorescence branching ratios, and excited state lifetimes were also measured and calculated. The upconversion emission intensity varies with the power of infrared excitation intensity. A plot of log I-up vs log I-IR yields a straight line with slope 1.86, 1.88 and 1.85, corresponding to 525, 546, and 657 nm emission bands, respectively, which indicates that a two-photon process for the red and green emission.