Browsing by Author "Kelestemur, Y."
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Item Open Access Amplified Spontaneous Emission and Lasing in Colloidal Nanoplatelets(American Chemical Society, 2014-07) Guzelturk, B.; Kelestemur, Y.; Olutas, M.; Delikanli, S.; Demir, Hilmi VolkanColloidal nanoplatelets (NPLs) have recently emerged as favorable light-emitting materials, which also show great potential as optical gain media due to their remarkable optical properties. In this work, we systematically investigate the optical gain performance of CdSe core and CdSe/CdS core/crown NPLs having different CdS crown size with one- and two-photon absorption pumping. The core/crown NPLs exhibit enhanced gain performance as compared to the core-only NPLs due to increased absorption cross section and the efficient interexciton funneling, which is from the CdS crown to the CdSe core. One- and two-photon absorption pumped amplified spontaneous emission thresholds are found as low as 41 μJ/cm2 and 4.48 mJ/cm2 , respectively. These thresholds surpass the best reported optical gain performance of the state-of-the-art colloidal nanocrystals (i.e., quantum dots, nanorods,etc.) emitting in the same spectral range as the NPLs. Moreover, gain coefficient of the NPLs is measured as high as 650 cm 1 , which is 4-fold larger than the best reported gain coefficient of the colloidal quantum dots. Finally, we demonstrate a two-photon absorption pumped vertical cavity surface emitting laser of the NPLs with a lasing threshold as low as 2.49 mJ/cm2 . These excellent results are attributed to the superior properties of the NPLs as optical gain media.Item Open Access Attractive versus repulsive excitonic interactions of colloidal quantum dots control blue-to red-shifting (and non-shifting) amplified spontaneous emission(American Chemical Society, 2013-11-21) Cihan, A. F.; Kelestemur, Y.; Guzelturk, B.; Yerli, O.; Kurum, U.; Yaglioglu, H. G.; Elmali, A.; Demir, Hilmi VolkanTunable, high-performance, two-photon absorption (TPA)-based amplified spontaneous emission (ASE) from near-unity quantum efficiency colloidal quantum dots (CQDs) is reported. Besides the absolute spectral tuning of ASE, the relative spectral tuning of ASE peak with respect to spontaneous emission was shown through engineering excitonic interactions in quasi-type-II CdSe/CdS core/shell CQDs. With core shell size adjustments, it was revealed that Coulombic exciton-exciton interactions can be tuned to be attractive (type-I-like) or repulsive (type-II-like) leading to red- or blue-shifted ASE peak, respectively, and that nonshifting ASE can be achieved with the right core shell combinations. The possibility of obtaining ASE at a specific wavelength from both type-I-like and type-II-like CQDs was also demonstrated. The experimental observations were supported by parametric quantum-mechanical modeling, shedding light on the type-tunability. These excitonically engineered CQD-solids exhibited TPA-based ASE threshold as low as 6.5 mJ/cm(2) under 800 nm excitation, displaying one of the highest values of TPA cross-section of 44 660 GM.Item Open Access Energy-saving quality road lighting with colloidal quantum dot nanophosphors(Walter de Gruyter GmbH, 2014) Erdem, T.; Kelestemur, Y.; Soran-Erdem, Z.; Ji, Y.; Demir, Hilmi VolkanHere 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. © 2014 Science Wise Publishing & De Gruyter 2014.Item Open Access Evidence for Nonradiative Energy Transfer in Graphene-Oxide-Based Hybrid Structures(American Chemical Society, 2013-11-13) Yeltik, A.; Kucukayan-Dogu, G.; Guzelturk, B.; Fardindoost, S.; Kelestemur, Y.; Demir, Hilmi VolkanSolution processed graphene variants including graphene oxide (GO) and reduced graphene oxide (RGO) are promising materials for potential optoelectronic applications. To date, efficiency of the excitation energy transfer into GO and RGO thin layers has not been investigated in terms of donor-acceptor separation distance. In the present work, we study nonradiative energy transfer (NRET) from CdSe/CdS quantum dots into single and/or double layer GO or RGO using time-resolved fluorescence spectroscopy. We observe shorter lifetimes as the separation distance between the QDs and GO or RGO decreases. In accordance with these lifetimes, the rates reveal the presence of two different mechanisms dominating the NRET. Here we show that excitonic NRET is predominant at longer intervals while both excitonic and nonexcitonic NRET exist at shorter distances. In addition, we find the NRET rate behavior to be strongly dependent on the reduction degree of the GO-based layers. We obtain high NRET efficiency levels of similar to 97 and similar to 89% for the closest separation of the QD-RGO pair and the QD-GO pair, respectively. These results indicate that strong NRET from QDs into thin layer GO and RGO makes these solution-processable thin films promising candidates for light harvesting and detection systems.Item Open Access Excitonic improvement of colloidal nanocrystals in salt powder matrix for quality lighting and color enrichment(OSA - The Optical Society, 2016) Erdem, T.; Soran-Erdem, Z.; Kelestemur, Y.; Gaponik, N.; Demir, Hilmi VolkanHere we report excitonic improvement in color-converting colloidal nanocrystal powders enabled by co-integrating nonpolar greenand red-emitting nanocrystal energy transfer pairs into a single LiCl salt matrix. This leads to nonradiative energy transfer (NRET) between the cointegrated nanocrystals in the host matrix. Here we systematically studied the resulting NRET process by varying donor and acceptor concentrations in the powders. We observed that NRET is a strong function of both of the nanocrystal concentrations and that NRET efficiency increases with increasing acceptor concentration. Nevertheless, with increasing donor concentration in the powders, NRET efficiency was found to first increase (up to a maximum level of 53.9%) but then to decrease. As a device demonstrator, we employed these NRET-improved nanocrystal powders as color-converters on blue light-emitting diodes (LEDs), with the resulting hybrid LED exhibiting a luminous efficiency >70 lm/Welect . The proposed excitonic nanocrystal powders potentially hold great promise for quality lighting and color enrichment applications.Item Open Access Implementation of graphene multilayer electrodes in quantum dot light-emitting devices(Springer Verlag, 2015) Wolff, S.; Jansen, D.; Terlinden H.; Kelestemur, Y.; Mertin W.; Demir, Hilmi Volkan; Bacher G.; Nannen, E.Graphene is a highly attractive candidate for implementation as electrodes in next-generation large-area optoelectronic devices thanks to its high electrical conductivity and high optical transparency. In this study, we show all-solution-processed quantum dot-based light-emitting devices (QD-LEDs) using graphene mono- and multilayers as transparent electrodes. Here, the effect of the number of graphene layers (up to three) on the QD-LEDs performance was studied. While the implementation of a second graphene layer was found to reduce the turn-on voltage from 2.6 to 1.8 V, a third graphene layer was observed to increase the turn-on voltage again, which is attributed to an increased roughness of the graphene layer stack. © 2015, Springer-Verlag Berlin Heidelberg.Item Open Access Light-induced paramagnetism in colloidal Ag+-doped CdSe nanoplatelets(American Chemical Society, 2021-03-25) Najafi, A.; Sharma, Manoj; Delikanlı, Savaş; Bhattacharya, A.; Murphy, J. R.; Pientka, J.; Sharma, A.; Quinn, A. P.; Erdem, Onur; Kattel, S.; Kelestemur, Y.; Kovalenko, M. V.; Rice, W. D.; Demir, Hilmi Volkan; Petrou, A.We describe a study of the magneto-optical properties of Ag+-doped CdSe colloidal nanoplatelets (NPLs) that were grown using a novel doping technique. In this work, we used magnetic circularly polarized luminescence and magnetic circular dichroism spectroscopy to study light-induced magnetism for the first time in 2D solution-processed structures doped with nominally nonmagnetic Ag+ impurities. The excitonic circular polarization (PX) and the exciton Zeeman splitting (ΔEZ) were recorded as a function of the magnetic field (B) and temperature (T). Both ΔEZ and PX have a Brillouin-function-like dependence on B and T, verifying the presence of paramagnetism in Ag+-doped CdSe NPLs. The observed light-induced magnetism is attributed to the transformation of nonmagnetic Ag+ ions into Ag2+, which have a nonzero magnetic moment. This work points to the possibility of incorporating these nanoplatelets into spintronic devices, in which light can be used to control the spin injection.Item Open Access Manganese doped fluorescent paramagnetic nanocrystals for dual-modal imaging(Wiley-VCH Verlag, 2014) Sharma, V. K.; Gokyar, S.; Kelestemur, Y.; Erdem, T.; Unal, E.; Demir, Hilmi VolkanIn this work, dual-modal (fluorescence and magnetic resonance) imaging capabilities of water-soluble, low-toxicity, monodisperse Mn-doped ZnSe nanocrystals (NCs) with a size (6.5 nm) below the optimum kidney cutoff limit (10 nm) are reported. Synthesizing Mn-doped ZnSe NCs with varying Mn2+ concentrations, a systematic investigation of the optical properties of these NCs by using photoluminescence (PL) and time resolved fluorescence are demonstrated. The elemental properties of these NCs using X-ray photoelectron spectroscopy and inductive coupled plasma-mass spectroscopy confirming Mn2+ doping is confined to the core of these NCs are also presented. It is observed that with increasing Mn2+ concentration the PL intensity first increases, reaching a maximum at Mn2+ concentration of 3.2 at% (achieving a PL quantum yield (QY) of 37%), after which it starts to decrease. Here, this high-efficiency sample is demonstrated for applications in dual-modal imaging. These NCs are further made water-soluble by ligand exchange using 3-mercaptopropionic acid, preserving their PL QY as high as 18%. At the same time, these NCs exhibit high relaxivity (≈2.95 mM-1 s-1) to obtain MR contrast at 25°C, 3 T. Therefore, the Mn2+ doping in these water-soluble Cd-free NCs are sufficient to produce contrast for both fluorescence and magnetic resonance imaging techniques.Item Open Access Tattoo-like multi-color physically unclonable functions(John Wiley and Sons Inc, 2023-12-07) Kiremitler, N. B.; Esidir, A.; Drake, G. A.; Yazıcı, A. F.; Şahin, F.; Torun, I.; Kalay, M.; Kelestemur, Y.; Demir, Hilmi Volkan; Shim, M.; Mutlugün, Evren; Önses, Mustafa SerdarAdvanced anti-counterfeiting and authentication approaches are in urgent need of the rapidly digitizing society. Physically unclonable functions (PUFs) attract significant attention as a new-generation security primitive. The challenge is design and generation of multi-color PUFs that can be universally applicable to objects of varied composition, geometry, and rigidity. Herein, tattoo-like multi-color fluorescent PUFs are proposed and demonstrated. Multi-channel optical responses are created by electrospraying of polymers that contain semiconductor nanocrystals with precisely defined photoluminescence. The universality of this approach enables the use of dot and dot-in-rod geometries with unique optical characteristics. The fabricated multi-color PUFs are then transferred to a target object by using a temporary tattoo approach. Digitized keys generated from the red, green and blue fluorescence channels facilitate large encoding capacity and rapid authentication. Feature matching algorithms complement the authentication by direct image comparison, effectively alleviating constraints associated with imaging conditions. The strategy that paves the way for the development of practical, cost-effective, and secure anticounterfeiting systems is presented.Item Open Access Tunable White-Light-Emitting Mn-Doped ZnSe Nanocrystals(American Chemical Society, 2014-02-06) Sharma, V. K.; Guzelturk, B.; Erdem, T.; Kelestemur, Y.; Demir, Hilmi VolkanWe report white-light-emitting Mn-doped ZnSe nanocrystals (NCs) that are synthesized using modified nucleation doping strategy. Tailoring three distinct emission mechanisms in these NCs, which are MnSe-related blue emission (410 and 435 nm), Zn-related defect state green emission (520 nm), and Mn-dopant related orange emission (580 nm), allowed us to achieve excitation wavelength tailorable white-light generation as studied by steady state and time-resolved fluorescence spectroscopy. These NCs will be promising as single component white-light engines for solid-state lighting.Item Open Access Ultralow threshold one-photon-and two-photon-pumped optical gain media of blue-emitting colloidal quantum dot films(American Chemical Society, 2014) Guzelturk, B.; Kelestemur, Y.; Akgul, M. Z.; Sharma, V. K.; Demir, Hilmi VolkanColloidal quantum dots (QDs) offer advantageous properties as an optical gain media for lasers. Optical gain in the QDs has been shown in the whole visible spectrum, yet it has been intrinsically challenging to realize efficient amplified spontaneous emission (ASE) and lasing in the blue region of the visible spectrum. Here, we synthesize large-sized core/gradient shell CdZnS/ZnS QDs as an efficient optical gain media in the blue spectral range. In this Letter, we demonstrate for the first time that two-photon-absorption-pumped ASE from the blue-emitting QD is achievable with a threshold as low as 6 mJ/cm(2). Utilizing these QDs, we also report one-photon-absorption-pumped ASE at an ultralow threshold of similar to 60 mu J/cm(2), which is comparable to the state-of-the-art red-emitting QD-based gain media. This one-photon-pumped ASE threshold is an order of magnitude better than that of the previously reported best blue-emitting QD-based gain media.