Browsing by Author "Mutlugun, E."
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Item Open Access AC-driven, color-and brightness-tunable organic light-emitting diodes constructed from an electron only device(2013) Zhao, Y.; Chen, R.; Gao, Y.; Leck, K.S.; Yang X.; Liu, S.; Abiyasa, A.P.; Divayana, Y.; Mutlugun, E.; Tan, S.T.; Sun H.; Demir, Hilmi Volkan; Sun X.W.In this paper, a color- and brightness-tunable organic light-emitting diode (OLED) is reported. This OLED was realized by inserting a charge generation layer into an electron only device to form an n-i-p-i-n structure. It is shown that, by changing the polarity of applied voltage, only the p-i-n junction operated under positive bias can emit light and, by applying an AC voltage, emission from both junctions was realized. It is also shown that, by using a combination of blue- and red-emiting layers in two p-i-n junctions, both the color and brightness of the resulting white OLED can be tuned independently by changing the positive and negative amplitudes of the AC voltage. © 2013 Elsevier B.V. All rights reserved.Item Open Access Anisotropic Emission from Multilayered Plasmon Resonator Nanocomposites of Isotropic Semiconductor Quantum Dots(American Chemical Society, 2011-01-19) Ozel, T.; Nizamoglu, S.; Sefunc, M.A.; Samarskaya, O.; Ozel, I. O.; Mutlugun, E.; Lesnyak, V.; Gaponik N.; Eychmuller, A.; Gaponenko, S. V.; Demir, Hilmi VolkanWe propose and demonstrate a nanocomposite localized surface plasmon resonator embedded into an artificial three-dimensional construction. Colloidal semiconductor quantum dots are assembled between layers of metal nanoparticles to create a highly strong plasmon-exciton interaction in the plasmonic cavity. In such a multilayered plasmonic resonator architecture of isotropic CdTe quantum dots, we observed polarized light emission of 80% in the vertical polarization with an enhancement factor of 4.4, resulting in a steady-state anisotropy value of 0.26 and reaching the highest quantum efficiency level of 30% ever reported for such CdTe quantum dot solids. Our electromagnetic simulation results are in good agreement with the experimental characterization data showing a significant emission enhancement in the vertical polarization, for which their fluorescence decay lifetimes are substantially shortened by consecutive replication of our unit cell architecture design. Such strongly plasmon-exciton coupling nanocomposites hold great promise for future exploitation and development of quantum dot plasmonic biophotonics and quantum dot plasmonic optoelectronics.Item Open Access Bio-nanohybrids of quantum dots and photoproteins facilitating strong nonradiative energy transfer(Royal Society of Chemistry, 2013-05-21) Seker U.O.S.; Mutlugun, E.; Hernandez-Martinez, R. L.; Sharma, V. K.; Lesnyak, V.; Gaponik N.; Eychmuller, A.; Demir, Hilmi VolkanUtilization of light is crucial for the life cycle of many organisms. Also, many organisms can create light by utilizing chemical energy emerged from biochemical reactions. Being the most important structural units of the organisms, proteins play a vital role in the formation of light in the form of bioluminescence. Such photoproteins have been isolated and identified for a long time; the exact mechanism of their bioluminescence is well established. Here we show a biomimetic approach to build a photoprotein based excitonic nanoassembly model system using colloidal quantum dots (QDs) for a new bioluminescent couple to be utilized in biotechnological and photonic applications. We concentrated on the formation mechanism of nanohybrids using a kinetic and thermodynamic approach. Finally we propose a biosensing scheme with an ON/OFF switch using the QD-GFP hybrid. The QD-GFP hybrid system promises strong exciton-exciton coupling between the protein and the quantum dot at a high efficiency level, possessing enhanced capabilities of light harvesting, which may bring new technological opportunities to mimic biophotonic events.Item Open Access Colloidal quantum dot light-emitting diodes employing phosphorescent small organic molecules as efficient exciton harvesters(American Chemical Society, 2014) Mutlugun, E.; Guzelturk, B.; Abiyasa, A. P.; Gao, Y.; Sun X. W.; Demir, Hilmi VolkanNonradiative energy transfer (NRET) is an alternative excitation mechanism in colloidal quantum dot (QD) based electroluminescent devices (QLEDs). Here, we develop hybrid highly spectrally pure QLEDs that facilitate energy transfer pumping via NRET from a phosphorescent small organic molecule-codoped charge transport layer to the adjacent QDs. A partially codoped exciton funnelling electron transport layer is proposed and optimized for enhanced QLED performance while exhibiting very high color purity of 99%. These energy transfer pumped hybrid QLEDs demonstrate a 6-fold enhancement factor in the external quantum efficiency over the conventional QLED structure, in which energy transfer pumping is intrinsically weak.Item Open Access Comparative study of optically activated nanocomposites with photocatalytic TiO2 and ZnO nanoparticles for massive environmental decontamination(S P I E - International Society for Optical Engineering, 2007) Tek, S.; Mutlugun, E.; Soganci, I. M.; Perkgoz, N. K.; Yucel, D.; Celiker, G.; Demir, Hilmi VolkanNanocomposites that incorporate TiO2 and ZnO nanoparticles separately in three-dimensional solgel matrices through full chemical integration are prepared to perform highly efficient photocatalytic activities for applications of environmental decontamination. Spectral responses of photocatalytic TiO2 and ZnO nanoparticles exposed to UV activation for self-cleaning process were obtained as also their optical relative spectral efficiency curves from 270 to 370 nm in the UV regime. Our investigations of the optimal conditions to increase their spectral photocatalytic efficiencies resulted in remarkably high levels of optical recovery and efficiency.Item Open Access Dual-color emitting quantum-dot-quantum-well CdSe-ZnS heteronanocrystals hybridized on InGaN/GaN light emitting diodes for high-quality white light generation(AIP Publishing LLC, 2008-03) Nizamoglu, S.; Mutlugun, E.; Özel, T.; Demir, Hilmi VolkanWe report white light generation by hybridizing green-red emitting (CdSeZnS/CdSe (core) shell/ shell quantum-dot-quantum-well heteronanocrystals on blue InGaN/GaN light emitting diodes with the photometric properties of tristimulus coordinates (x, y) =(0.36, 0.30), luminous efficacy of optical radiation LE= 278 lm/W, correlated color temperature CCT= 3929 K, and color-rendering index CRI= 75.1. We present the photometric analysis and the quantum mechanical design of these dual-color emitting heteronanocrystals synthesized to achieve high-quality white light when hybridized on light emitting diodes. Using such multicolor emitting heteronanocrystals facilitates simple device implementation while providing good photometric propertiesItem Open Access Excitonic enhancement of nonradiative energy transfer from a quantum well in the optical near field of energy gradient quantum dots(American Institute of Physics, 2012-06-13) Nizamoglu, S.; Hernandez-Martinez, P. L.; Mutlugun, E.; Karatay, D. U.; Demir, Hilmi VolkanWe report strong exciton migration with an efficiency of 83.3% from a violet-emitting epitaxial quantum well (QW) to an energy gradient colloidal construct of layered green-and red-emitting nanocrystal quantum dots (NQDs) at room temperature, enabled by the interplay between the exciton population and the depopulation of states in the optical near field. Based on the density matrix formalization of near-field interactions, we theoretically model and demonstrate that the energy gradient significantly boosts the QW-NQDs exciton transfer rate compared to using mono-dispersed NQDs, which is in agreement with the observed experimental results.Item Open Access Highly efficient nonradiative energy transfer mediated light harvesting in water using aqueous CdTe quantum dot antennas(Optical Society of America, 2010) Mutlugun, E.; Samarskaya, O.; Ozel, T.; Cicek, N.; Gaponik, N.; Eychmuller, A.; Demir, Hilmi VolkanWe present light harvesting of aqueous colloidal quantum dots to nonradiatively transfer their excitonic excitation energy efficiently to dye molecules in water, without requiring ligand exchange. These as-synthesized CdTe quantum dots that are used as donors to serve as light-harvesting antennas are carefully optimized to match the electronic structure of Rhodamine B molecules used as acceptors for light harvesting in aqueous medium. By varying the acceptor to donor concentration ratio, we measure the light harvesting factor, along with substantial lifetime modifications of these water-soluble quantum dots, from 25.3 ns to 7.2 ns as a result of their energy transfer with efficiency levels up to 86%. Such nonradiative energy transfer mediated light harvesting in aqueous medium holds great promise for future quantum dot multiplexed dye biodetection systems. (C) 2010 Optical Society of America.Item Open Access Highly flexible, electrically driven, top-emitting, quantum dot light-emitting stickers(American Chemical Society, 2014) Yang X.; Mutlugun, E.; Dang, C.; Dev, K.; Gao, Y.; Tan, S.T.; Sun X.W.; Demir, Hilmi VolkanFlexible information displays are key elements in future optoelectronic devices. Quantum dot light-emitting diodes (QLEDs) with advantages in color quality, stability, and cost-effectiveness are emerging as a candidate for single-material, full color light sources. Despite the recent advances in QLED technology, making high-performance flexible QLEDs still remains a big challenge due to limited choices of proper materials and device architectures as well as poor mechanical stability. Here, we show highly efficient, large-area QLED tapes emitting in red, green, and blue (RGB) colors with top-emitting design and polyimide tapes as flexible substrates. The brightness and quantum efficiency are 20 000 cd/m2 and 4.03%, respectively, the highest values reported for flexible QLEDs. Besides the excellent electroluminescence performance, these QLED films are highly flexible and mechanically robust to use as electrically driven light-emitting stickers by placing on or removing from any curved surface, facilitating versatile LED applications. Our QLED tapes present a step toward practical quantum dot based platforms for high-performance flexible displays and solid-state lighting. © 2014 American Chemical Society.Item Open Access Hyperbolic metamaterials based on quantum-dot plasmon resonator nanocomposites(Optical Society of America, 2014) Zhokovsky, S. V.; Ozel, T.; Mutlugun, E.; Gaponik, N.; Eychmuller, A.; Lavrinenko, A. V.; Demir, Hilmi Volkan; Gaponenko, S. V.We theoretically demonstrate that nanocomposites made of colloidal semiconductor quantum dot monolayers placed between metal nanoparticle monolayers can function as multilayer hyperbolic metamaterials. Depending on the thickness of the spacer between the quantum dot and nanoparticle layers, the effective permittivity tensor of the nanocomposite is shown to become indefinite, resulting in increased photonic density of states and strong enhancement of quantum dot luminescence. This explains the results of recent experiments [T. Ozel et al., ACS Nano 5, 1328 (2011)] and confirms that hyperbolic metamaterials are capable of increasing the radiative decay rate of emission centers inside them. The proposed theoretical framework can also be used to design quantum-dot/nanoplasmonic composites with optimized luminescence enhancement. (C) 2014 Optical Society of AmericaItem Open Access Large-Area (over 50 cm × 50 cm) Freestanding Films of Colloidal InP/ZnS Quantum Dots(American Chemical Society, 2012) Mutlugun, E.; Hernandez Martinez, P. L.; Eroglu, C.; Coskun, Y.; Erdem, T.; Sharma, V. K.; Unal, E.; Panda, S. K.; Hickey, S. G.; Gaponik, N.; Eychmuller, A.; Demir, Hilmi VolkanWe propose and demonstrate the fabrication of flexible, freestanding films of InP/ZnS quantum dots (QDs) using fatty acid ligands across very large areas (greater than 50 cm x 50 cm), which have been developed for remote phosphor applications in solid-state lighting. Embedded in a poly(methyl methacrylate) matrix, although the formation of stand alone films using other QDs commonly capped with trioctylphosphine oxide (TOPO) and oleic acid is not efficient, employing myristic acid as ligand in the synthesis of these QDs, which imparts a strongly hydrophobic character to the thin film, enables film formation and ease of removal even on surprisingly large areas, thereby avoiding the need for ligand exchange. When pumped by a blue LED, these Cd-free QD films allow for high color rendering, warm white light generation with a color rendering index of 89.30 and a correlated color temperature of 2298 K. In the composite film, the temperature-dependent emission kinetics and energy transfer dynamics among different-sized InP/ZnS QDs are investigated and a model is proposed. High levels of energy transfer efficiency (up to 80%) and strong donor lifetime modification (from 18 to 4 ns) are achieved. The suppression of the nonradiative channels is observed when the hybrid film is cooled to cryogenic temperatures. The lifetime changes of the donor and acceptor InP/ZnS QDs in the film as a result of the energy transfer are explained well by our theoretical model based on the exciton-exciton interactions among the dots and are in excellent agreement with the experimental results. The understanding of these excitonic interactions is essential to facilitate improvements in the fabrication of photometrically high quality nanophosphors. The ability to make such large-area, flexible, freestanding Cd-free QD films pave the way for environmentally friendly phosphor applications including flexible, surface-emitting light engines.Item Open Access Light extraction efficiency enhancement of colloidal quantum dot light-emitting diodes using large-scale nanopillar arrays(Wiley-VCH Verlag, 2014) Yang, X.; Dev, K.; Wang, J.; Mutlugun, E.; Dang, C.; Zhao Y.; Liu, S.; Tang, Y.; Tan S.T.; Sun, X. W.; Demir, Hilmi VolkanA colloidal quantum dot light-emitting diode (QLED) is reported with substantially enhanced light extraction efficiency by applying a layer of large-scale, low-cost, periodic nanopillar arrays. Zinc oxide nanopillars are grown on the glass surface of the substrate using a simple, efficient method of non-wetting templates. With the layer of ZnO nanopillar array as an optical outcoupling medium, a record high current efficiency (CE) of 26.6 cd/A is achieved for QLEDs. Consequently, the corresponding external quantum efficiency (EQE) of 9.34% reaches the highest EQE value for green-emitting QLEDs. Also, the underlying physical mechanisms enabling the enhanced light-extraction are investigated, which leads to an excellent agreement of the numerical results based on the mode theory with the experimental measurements. This study is the first account for QLEDs offering detailed insight into the light extraction efficiency enhancement of QLED devices. The method demonstrated here is intended to be useful not only for opening up a ubiquitous strategy for designing high-performance QLEDs but also with respect to fundamental research on the light extraction in QLEDs.Item Open Access Liposomal prevention of quantum dots cytotoxicity(2011) Buyuksungur, A.; Mutlugun, E.; Demir, Hilmi Volkan; Hasirci V.[No abstract available]Item Open Access Localized plasmon-engineered spontaneous emission of CdSe/ZnS nanocrystals closely-packed in the proximity of Ag nanoisland films for controlling emission linewidth, peak, and intensity(Optical Society of America, 2007) Soganci, I. M.; Nizamoglu, S.; Mutlugun, E.; Akin, O.; Demir, Hilmi VolkanUsing metallic nanoislands, we demonstrate the localized plasmonic control and modification of the spontaneous emission from closely-packed nanocrystal emitters, leading to significant changes in their collective emission characteristics tuned spectrally and spatially by plasmon coupling. Using randomly-distributed silver nanoislands, we show that the emission linewidth of proximal CdSe/ZnS core-shell quantum dots is reduced by 22% and their peak emission wavelength is shifted by 14nm, while their ensemble photoluminescence is enhanced via radiative energy transfer by 21.6 and 15.1 times compared to the control groups of CdSe/ZnS nanocrystals with identical nano-silver but no dielectric spacer and the same nanocrystals alone, respectively. (C) 2007 Optical Society of America.Item Open Access Nanocrystal hybridized scintillators for enhanced detection and imaging on Si platforms in UV(Optical Society of America, 2007) Mutlugun, E.; Sorganci, I. M.; Demir, Hilmi VolkanWe report on the conception, design, fabrication, experimental characterization, and theoretical analysis of nanocrystal scintillators hybridized on Si detectors and CCDs for enhanced detection and imaging in UV. Integrating luminescent CdSe/ZnS core-shell nanocrystals (NCs of 3.2 and 5.2 nm in diameter with 5% size distribution) to efficiently convert incident UV radiation to visible emission, we demonstrate hybrid NC-Si photodetectors that exhibit significantly improved responsivity between 200-240nm, experimentally with a two orders of magnitude peak enhancement and theoretically with a three orders of magnitude peak enhancement. Such nanocrystal based scintillators hold great promise in UV detection and imaging on Si platforms. (c) 2007 Optical Society of America.Item Open Access Nanosecond colloidal quantum dot lasers for sensing(Optical Society of America, 2014) Guilhabert, B.; Foucher, C.; Haughey, A M.; Mutlugun, E.; Gao, Y.; Herrnsdorf, J.; Sun, H. D.; Demir, Hilmi Volkan; Dawson, M. D.; Laurand, N.Low-threshold, gain switched colloidal quantum dot (CQD) distributed-feedback lasers operating in the nanosecond regime are reported and proposed for sensing applications for the first time to the authors' knowledge. The lasers are based on a mechanically-flexible polymeric, second order grating structure overcoated with a thin-film of CQD/PMMA composite. The threshold fluence of the resulting lasers is as low as 0.5 mJ=cm2 for a 610 nm emission and the typical linewidth is below 0.3 nm. The emission wavelength of the lasers can be set at the design stage and laser operation between 605 nm and 616 nm, while using the exact same CQD gain material, is shown. In addition, the potential of such CQD lasers for refractive index sensing in solution is demonstrated by immersion in water. © 2014 Optical Society of America.Item Open Access Observation of biexcitons in nanocrystal solids in the presence of photocharging(American Chemical Society, 2013) Cihan, A. F.; Martinez, P. L. H.; Kelestemur Y.; Mutlugun, E.; Demir, Hilmi VolkanT In nanocrystal quantum dots (NQDs), generating multiexcitons offers an enabling tool for enhancing NQD-based devices. However, the photocharging effect makes understanding multiexciton kinetics in NQD solids fundamentally challenging, which is critically important for solid-state devices. To date, this lack of understanding and the spectral temporal aspects of the multiexciton recombination still remain unresolved in solid NQD ensembles, which is mainly due to the confusion with recombination of carriers in charged NQDs. In this work, we reveal the spectral temporal behavior of biexcitons (BXs) in the presence of photocharging using near-unity quantum yield CdSe/CdS NQDs exhibiting substantial suppression of Auger recombination. Here, recombinations of biexcitons and single excitons (Xs) are successfully resolved in the presence of trions in the ensemble measurements of time-correlated single-photon counting at variable excitation intensities and varying emission wavelengths. The spectral behaviors of BXs and Xs are obtained for three NQD samples with different core sizes, revealing the strength tunability of the X X interaction energy in these NQDs. The extraction of spectrally resolved X, BX, and trion kinetics, which are otherwise spectrally unresolved, is enabled by our approach introducing integrated time-resolved fluorescence. The results are further experimentally verified by cross-checking excitation intensity and exposure time dependencies as well as the temporal evolutions of the photoluminescence spectra, all of which prove to be consistent. The BX and X energies are also confirmed by theoretical calculations. These findings fill an important gap in understanding the spectral dynamics of multiexcitons in such NQD solids under the influence of photocharging effects, paving the way to engineering of multiexciton kinetics in nanocrystal optoelectronics, including NQD-based lasing, photovoltaics, and photodetection.Item Open Access Observation of selective plasmon-exciton coupling in nonradiative energy transfer: donor-selective versus acceptor-selective plexcitons(American Chemical Society, 2013-06) Ozel, T.; Hernandez-Martinez, P. L.; Mutlugun, E.; Akin, O.; Nizamoglu, S.; Ozel, I. O.; Zhang, Q.; Xiong, Q.; Demir, Hilmi VolkanWe report selectively plasmon-mediated nonradiative energy transfer between quantum dot (QD) emitters interacting with each other via Forster-type resonance energy transfer (FRET) under controlled plasmon coupling either to only the donor QDs (i.e., donor-selective) or to only the acceptor QDs (i.e., acceptor-selective). Using layer-by-layer assembled colloidal QD nanocrystal solids with metal nanoparticles integrated at carefully designed spacing, we demonstrate the ability to enable/disable the coupled plasmon-exciton (plexciton) formation distinctly at the donor (exciton departing) site or at the acceptor (exciton feeding) site of our choice, while not hindering the donor exciton-acceptor exciton interaction but refraining from simultaneous coupling to both sites of the donor and the acceptor in the FRET process.. In the case of donor-selective plexciton, we observed a substantial shortening in the donor QD lifetime from 1.33 to 0.29 ns as a result of plasmon-coupling to the donors and the FRET-assisted exciton transfer from the donors to the acceptors, both of which shorten the donor lifetime. This consequently enhanced the acceptor emission by a factor of 1.93. On the other hand, in the complimentary case of acceptor-selective plexciton, we observed a 2.70-fold emission enhancement in the acceptor QDs, larger than the acceptor emission enhancement of the donor-selective plexciton, as a result of the combined effects of the acceptor plasmon coupling and the FRET-assisted exciton feeding. Here we present the comparative results of theoretical modeling of the donor- and acceptor-selective plexcitons of nonradiative energy transfer developed here for the first time, which are in excellent agreement with the systematic experimental characterization. Such an ability to modify and control energy transfer through mastering plexcitons is of fundamental importance, opening up new applications for quantum dot embedded plexciton devices along with the development of new techniques in FRET-based fluorescence microscopy.Item Open Access Photocatalytic hybrid nanocomposites of metal oxide nanoparticles enhanced towards the visible spectral range(Elsevier, 2011-04-13) Perkgoz, N. K.; Toru, R. S.; Unal, E.; Sefunc, M.A.; Tek, S.; Mutlugun, E.; Soganci, I. M.; Celiker, H.; Celiker, G.; Demir, Hilmi VolkanWe propose and demonstrate photocatalytic hybrid nanocomposites that co-integrate TiO(2) and ZnO nanoparticles in the same host resin to substantially enhance their combined photocatalytic activity in the near-UV and visible spectral ranges, where the intrinsic photocatalytic activity of TiO2 nanoparticles or that of ZnO nanoparticles is individually considerably weak For a comparative study, by embedding TiO(2) nanoparticles of ca. 6 nm and ZnO nanoparticles of ca. 40 nm in the sol-gel matrix of acrylic resin, we make thin film coatings of TiO(2)-ZnO nanoparticles (combination of TiO2 and ZnO, each with a mass ratio of 8.5%), as well as the composite films of TiO(2) nanoparticles alone (17.0%), and ZnO nanoparticles alone (17.0%), and a negative control group with no nanoparticles. For all of these thin films coated on polyvinyl chloride (PVC) polyester, we experimentally study photocatalytic activity and systematically measure spectral degradation (recovery obtained by photocatalytic reactions). This spectral characterization exhibits photodegradation levels of the contaminant at different excitation wavelengths (in the range of 310-469 nm) to distinguish different parts of optical spectrum where TiO(2) and ZnO nanopartides are individually and concurrently active. We observe that the photocatalytic activity is significantly improved towards the visible range with the use of TiO(2)-ZnO combination compared to the individual cases. Particularly for the excitation wavelengths of photochemical reactions longer than 400 nm, where the negative control group and ZnO nanoparticles alone yield no observable photodegradation level and TiO2 nanoparticles alone lead to a low photodegradation level of 14%, the synergic combination of TiO(2)-ZnO nanoparticles achieves a photodegradation level as high as 30%. Investigating their scanning electron microscopy (SEM), X-ray diffraction (XRD), and high resolution transmission electron microscopy (HRTEM), we present evidence of the heterostructure, crystallography, and chemical bonding states for the hybrid TiO(2)-ZnO nanocomposite films, in comparison to the films of only TiO(2) nanoparticles, only ZnO nanoparticles, and no nanoparticles.Item Open Access Photovoltaic nanocrystal scintillators hybridized on Si solar cells for enhanced conversion efficiency in UV(Optical Society of American (OSA), 2008) Mutlugun, E.; Soganci I.M.; Demir, Hilmi VolkanWe propose and demonstrate semiconductor nanocrystal based photovoltaic scintillators integrated on solar cells to enhance photovoltaic device parameters including spectral responsivity, open circuit voltage, short circuit current, fill factor, and solar conversion efficiency in the ultraviolet. Hybridizing (CdSe)ZnS core-shell quantum dots of 2.4 nm in diameter on multi-crystalline Si solar cells for the first time, we show that the solar conversion efficiency is enhanced 2 folds under white light illumination similar to the solar spectrum. Such nanocrystal scintillators provide the ability to extend the photovoltaic activity towards UV. © 2008 Optical Society of America.