Browsing by Author "Eychmuller, A."
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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 Bright White-Light Emitting Manganese and Copper Co-Doped ZnSe Quantum Dots(Wiley, 2011) Panda, S. K.; Hickey, S. G.; Demir, Hilmi Volkan; Eychmuller, A.Doubly doped quantum dots with highly efficient (17 %) white-light emission (WLE) have been directly synthesized using a one-pot hot-injection technique (see picture). The generation of WLE was due to the judicious manipulation of the synthesis strategy for the co-doping of the host material-ZnSe quantum dots-with Mn and Cu.Item Open Access Colloidal Nanocrystals Embedded in Macrocrystals: Robustness, Photostability, and Color Purity(American Chemical Society, 2012-09-14) Otto, T.; Mueller, M.; Mundra, P.; Lesnyak, V.; Demir, Hilmi Volkan; Gaponik N.; Eychmuller, A.The incorporation of colloidal quantum dots (QDs) into ionic crystals of various salts (NaCl, KCl, KBr, etc.) is demonstrated. The resulting mixed crystals of various shapes and beautiful colors preserve the strong luminescence of the incorporated QDs. Moreover, the ionic salts appear to be very tight matrices, ensuring the protection of the QDs from the environment and as a result providing them with extraordinary high photo- and chemical stability. A prototype of a white light-emitting diode (WLED) with a color conversion layer consisting of this kind of mixed crystals is demonstrated. These materials may also find applications in nonlinear optics and as luminescence standards.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 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 (> 50 cm × 50 cm), freestanding, flexible, optical membranes of Cd-free nanocrystal quantum dots(IEEE, 2012) Mutlugün, Evren; Hernandez Martinez, Pedro L.; Eroğlu, Cüneyt; Coşkun, Yasemin; Erdem, Talha; Sharma, Vijay K.; Ünal, Emre; Panda, S. K.; Hickey, S. G.; Gaponik, N.; Eychmuller, A.; Demir, Hilmi VolkanColloidal semiconductor quantum dots (QDs) have been extensively explored for numerous applications ranging from optoelectronics to biotechnology. This strong demand for the colloidal QDs arises because of their favorable optical and electronic properties. From the application points of view, QDs typically need to be used in their solid form, as opposed to their as-synthesized dispersion form. For immobilization of QDs and homogeneity of their films, various polymers have been used to host QDs within solid media. However, the integration of QDs into a polymeric medium is commonly complex, which requires a high level of understanding to provide optical quality. © 2012 IEEE.Item 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 Liquid-liquid diffusion ‐ assisted crystallization: a fast and versatile approach toward high quality mixed quantum dot ‐ salt crystals(Wiley-VCH Verlag, 2015) Adam, M.; Wang, Z.; Dubavik, A.; Stachowski, G. M.; Meerbach, C.; Soran-Erdem, Z.; Rengers, C.; Demir, Hilmi Volkan; Gaponik N.; Eychmuller, A.Here, a new, fast, and versatile method for the incorporation of colloidal quantum dots (QDs) into ionic matrices enabled by liquid-liquid diffusion is demonstrated. QDs bear a huge potential for numerous applications thanks to their unique chemical and physical properties. However, stability and processability are essential for their successful use in these applications. Incorporating QDs into a tight and chemically robust ionic matrix is one possible approach to increase both their stability and processability. With the proposed liquid-liquid diffusion-assisted crystallization (LLDC), substantially accelerated ionic crystallization of the QDs is shown, reducing the crystallization time needed by one order of magnitude. This fast process allows to incorporate even the less stable colloids including initially oil-based ligand-exchanged QDs into salt matrices. Furthermore, in a modified two-step approach, the seed-mediated LLDC provides the ability to incorporate oil-based QDs directly into ionic matrices without a prior phase transfer. Finally, making use of their processability, a proof-of-concept white light emitting diode with LLDC-based mixed QD-salt films as an excellent color-conversion layer is demonstrated. These findings suggest that the LLDC offers a robust, adaptable, and rapid technique for obtaining high quality QD-salts.Item Open Access Observation of anisotropic emission from semiconductor quantum dots in nanocomposites of metal nanoparticles(IEEE, 2010) Özel, Tuncay; Nizamoglu, Sedat; Sefunc, Mustafa A.; Samarskaya, Olga; Özel, İlkem O.; Mutlugun, Evren; Lesnyak V.; Gaponik, N.; Eychmuller, A.; Gaponenko, S.V.; Demir, Hilmi Volkan[No abstract available]Item Open Access Structural tuning of color chromaticity through nonradiative energy transfer by interspacing CdTe nanocrystal monolayers(American Institute of Physics, 2009-02-09) Cicek, N.; Nizamoglu, S.; Ozel, T.; Mutlugun, E.; Karatay, D. U.; Lesnyak, V.; Otto, T.; Gaponik N.; Eychmuller, A.; Demir, Hilmi VolkanWe proposed and demonstrated architectural tuning of color chromaticity by controlling photoluminescence decay kinetics through nonradiative Forster resonance energy transfer in the heterostructure of layer-by-layer spaced CdTe nanocrystal (NC) solids. We achieved highly sensitive tuning by precisely adjusting the energy transfer efficiency from donor NCs to acceptor NCs via controlling interspacing between them at the nanoscale. By modifying decay lifetimes of donors from 12.05 to 2.96 ns and acceptors from 3.68 to 14.57 ns, we fine-tuned chromaticity coordinates from (x,y)=(0.575,0.424) to (0.632, 0.367). This structural adjustment enabled a postsynthesis color tuning capability, alternative or additive to using the size, shape, and composition of NCs.Item Open Access Sweet plasmonics: sucrose macrocrystals of metal nanoparticles(Tsinghua University Press, 2015-03) Erdem, T.; Soran - Erdem, Z.; Hernandez - Martinez, P. L.; Sharma, V. K.; Akçalı, H.; Akçalı, I.; Gaponik N.; Eychmuller, A.; Demir, Hilmi VolkanThe realization of plasmonic structures generally necessitates expensive fabrication techniques, such as electron beam and focused ion beam lithography, allowing for the top-down fabrication of low-dimensional structures. Another approach to make plasmonic structures in a bottom-up fashion is colloidal synthesis, which is convenient for liquid-state applications or very thin solid films where aggregation problems are an important challenge. The architectures prepared using these methods are typically not robust enough for easy handling and convenient integration. Therefore, developing a new plasmonic robust platform having large-scale dimensions without adversely affecting the plasmonic features is in high demand. As a solution, here we present a new plasmonic composite structure consisting of gold nanoparticles (Au NPs) incorporated into sucrose macrocrystals on a large scale, while preserving the plasmonic nature of the Au NPs and providing robustness in handling at the same time. As a proof of concept demonstration, we present the fluorescence enhancement of green CdTe quantum dots (QDs) via plasmonic coupling with these Au NPs in the sucrose crystals. The obtained composite material exhibits centimeter scale dimensions and the resulting quantum efficiency (QE) is enhanced via the interplay between the Au NPs and CdTe QDs by 58% (from 24% to 38%). Moreover, a shortening in the photoluminescence lifetime from 11.0 to 7.40 ns, which corresponds to a field enhancement factor of 2.4, is observed upon the introduction of Au NPs into the QD incorporated macrocrystals. These results suggest that such "sweet" plasmonic crystals are promising for large-scale robust platforms to embed plasmonic nanoparticles.