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  1. Ana Sayfa
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Yazar "Demir, Hilmi Volkan" seçeneğine göre listele

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    Amplified spontaneous emission and lasing in colloidal nanoplatelets
    (American Chemical Society, 2014) Güzeltürk, Burak; Kelestemur, Yusuf; Olutaş, Murat; Delikanli, Savaş; Demir, Hilmi Volkan
    Colloidal 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 (de core. One- and two-photon absorption pumped amplified spontaneous emission thresholds are found as low as 41 mu J/cm(2) and 4.48 mJ/cm(2), 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/cm(2). These excellent results are attributed to the superior properties of the NPLs as optical gain media.
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    Giant modal gain coefficients in colloidal II-VI nanoplatelets
    (Amer Chemical Soc, 2019) Güzeltürk, Burak; Pelton, Matthew; Olutaş, Murat; Demir, Hilmi Volkan
    Modal gain coefficient is a key figure of merit for a laser material. Previously, net modal gain coefficients larger than a few thousand cm(-1) were achieved in II-VI and III-V semiconductor gain media, but this required operation at cryogenic temperatures. In this work, using pump-fluence-dependent variable-stripe-length measurements, we show that colloidal CdSe nanoplatelets enable giant modal gain coefficients at room temperature up to 6600 cm(-1) under pulsed optical excitation. Furthermore, we show that exceptional gain performance is common to the family of CdSe nanoplatelets, as shown by examining samples having different vertical thicknesses and lateral areas. Overall, colloidal II-VI nanoplatelets with superior optical gain properties are promising for a broad range of applications, including high-speed light amplification and loss compensation in plasmonic photonic circuits.
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    Highly efficient nonradiative energy transfer from colloidal semiconductor quantum dots to wells for sensitive noncontact temperature probing
    (Wiley-V C H Verlag Gmbh, 2016) Olutaş, Murat; Güzeltürk, Burak; Keleştemur, Yusuf; Güngör, Kıvanç; Demir, Hilmi Volkan
    This study develops and shows highly efficient exciton-transferring hybrid semiconductor nanocrystal films of mixed dimensionality comprising quasi 0D and 2D colloids. Through a systematic study of time-resolved and steady-state photoluminescence spectroscopy as a function of the donor-to-acceptor molar concentration ratio and temperature, a high-efficiency nonradiative energy transfer (NRET) process from CdZnS/ZnS core/shell quantum dots (QDs) directed to atomically flat CdSe nanoplatelets (NPLs) in their solid-state thin films is uncovered. The exciton funneling in this system reaches transfer efficiency levels as high as 90% at room temperature. In addition, this study finds that with decreasing temperature exciton transfer efficiency is increased to a remarkable maximum level of approximate to 94%. The enhancement in the dipole-dipole coupling strength with decreasing temperature is well accounted by increasing photoluminescence quantum yield of the donor and growing spectral overlap between the donor and the acceptor. Furthermore, NRET efficiency exhibits a highly linear monotonic response with changing temperature. This makes the proposed QD-NPL composites appealing for noncontact sensitive temperature probing based on NRET efficiencies as a new metric. These findings indicate that combining colloidal nanocrystals of different dimensionality enables efficient means of temperature probing at an unprecedented sensitivity level at nanoscale through almost complete exciton transfer.
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    Low-threshold optical gain and lasing of colloidal nanoplatelets
    (IEEE, 2014) Keleştemur, Yusuf; Güzeltürk, Burak; Olutaş, Murat; Delikanlı, Savaş; Demir, Hilmi Volkan
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    Near-infrared-emitting five-monolayer thick copper-doped CdSe nanoplatelets
    (Wiley-V C H Verlag Gmbh, 2019) Sharma, Ashma; Sharma, Manoj; Güngör, Kıvanç; Olutaş, Murat; Dede, Didem; Demir, Hilmi Volkan
    Doped nanocrystals are instrumental to the high-performance luminescent solar concentrators (LSCs) and the color conversion devices. Recently, copper (Cu)-doped three and four monolayer (ML) thick CdSe nanoplatelets (NPLs) have been shown superior to the existing Cu-doped quantum dots (QDs) for their use in LSCs. However, additional improvement in the LSC performance can be achieved by further redshifting the emission into the near-infrared (NIR) region of electromagnetic spectrum and increasing the absorbed portion of the solar irradiation. Cu-doping into higher thicknesses of these atomically flat NPLs (e.g., >= 5 ML) can achieve these overarching goals. However, addition of the dopant ions during the nucleation stage disturbs this high-temperature growth process and leads to multiple populations of NPLs and QDs. Here, by carefully controlling the precursor chemistry the successful doping of Cu in five ML thick NPLs by high-temperature nucleation doping method is demonstrated. The optimized synthesis method shows nearly pure population of doped five ML thick NPLs, which possess approximate to 150 nm Stokes-shifted NIR emission with high quantum yield of 65 +/- 2%. Structural, elemental, and optical studies are conducted to confirm the successful doping and understand the detailed photophysics. Finally, these materials are tested experimentally and theoretically for their performance as promising LSC materials.
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    Nonradiative energy transfer between doped and undoped flat semiconductor nanocrystals of colloidal quasi-2D nanoplatelets
    (Amer Chemical Soc, 2019) Yeltik, Aydan; Olutaş, Murat; Sharma, Manoj; Güngör, Kıvanç; Demir, Hilmi Volkan
    Atomically flat colloidal semiconductors such as nanoplatelets (NPLs) promise great potential for different optoelectronic applications. Here, we systematically investigate the excitonic energy transfer from colloidal Cu-doped CdSe to undoped core/shell CdSe/CdS nanoplatelets via steady-state and time-resolved photoluminescence spectros-copy techniques. We show the strong quenching in photoluminescence emission of the doped NPL donors together with significant modifications in the time-resolved kinetics by changing the concentration of the undoped NPL acceptors in close proximity. This newly presented all-colloidal and all-quasi-2D doped-undoped NPL-NPL hybrid system shows near-unity room-temperature energy transfer efficiency (99%) in solid films. We strongly believe that such highly efficient energy transfer in doped-undoped hybrid films will create more interest in the scientific community to further explore different donor/acceptor combinations with these newly reported doped NPLs for next-generation energy harvesting applications.
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    Stacking in colloidal nanoplatelets : tuning excitonic properties
    (Amer Chemical Soc, 2014) Güzeltürk, Burak; Erdem, Onur; Olutaş, Murat; Kelestemur, Yusuf; Demir, Hilmi Volkan
    Colloidal semiconductor quantum wells, also commonly known as nanoplatelets (NPLs), have arisen among the most promising materials for light generation and harvesting applications. Recently, NPLs have been found to assemble in stacks. However, their emerging characteristics essential to these applications have not been previously controlled or understood. In this report, we systematically investigate and present excitonic properties of controlled column-like NPL assemblies. Here, by a controlled gradual process, we show that stacking in colloidal quantum wells substantially increases exciton transfer and trapping. As NPLs form into stacks, surprisingly we find an order of magnitude decrease in their photoluminescence quantum yield, while the transient fluorescence decay is considerably accelerated. These observations are corroborated by ultraefficient Forster resonance energy transfer (FRET) in the stacked NPLs, in which exciton migration is estimated to be in the ultralong range (>100 nm). Homo-FRET (i.e., FRET among the same emitters) is found to be ultraefficient, reaching levels as high as 99.9% at room temperature owing to the close-packed collinear orientation of the NPLs along with their large extinction coefficient and small Stokes shift, resulting in a large Forster radius of similar to 13.5 nm. Consequently, the strong and long-range homo-FRET boosts exciton trapping in nonemissive NPLs, acting as exciton sink centers, quenching photoluminescence from the stacked NPLs due to rapid nonradiative recombination of the trapped excitons. The rate-equation-based model, which considers the exciton transfer and the radiative and nonradiative recombination within the stacks, shows an excellent match with the experimental data. These results show the critical significance of stacking control in NPL solids, which exhibit completely different signatures of homo-FRET as compared to that in colloidal nanocrystals due to the absence of inhomogeneous broadening.
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    Temperature-dependent emission kinetics of colloidal semiconductor nanoplatelets strongly modified by stacking
    (Amer Chemical Soc, 2016) Erdem, Onur; Olutaş, Murat; Güzeltürk, Burak; Keleştemur, Yusuf; Demir, Hilmi Volkan
    We systematically studied temperature-dependent emission kinetics in solid films of solution-processed CdSe nanoplatelets (NPLs) that are either intentionally stacked or nonstacked. We observed that the steady-state photoluminescence (PL) intensity of nonstacked NPLs considerably increases with decreasing temperature, whereas there is only a slight increase in stacked NPLs. Furthermore, PL decay time of the stacked NPL ensemble is comparatively much shorter than that of the nonstacked NPLs, and this result is consistent at all temperatures. To account for these observations, we developed a probabilistic model that describes excitonic processes in a stack using Markov chains, and we found excellent agreement between the model and experimental results. These findings develop the insight that the competition between the radiative channels and energy transfer assisted hole trapping leads to weakly temperature-dependent PL intensity in the case of the stacked NPL ensembles as compared to the nonstacked NPLs lacking strong energy transfer. This study shows that it is essential to account for the effect of NPL stacking to understand their resulting PL emission properties.
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    Type-II Colloidal Quantum Wells: CdSe/CdTe Core/Crown Heteronanoplatelets
    (American Chemical Society, 2015) Kelestemur, Yusuf; Olutaş, Murat; Delikanlı, Savaş; Güzeltürk, Burak; Akgül, Mehmet Zafer; Demir, Hilmi Volkan
    Solution-processed quantum wells, also known as colloidal nanoplatelets (NPLs), are emerging as promising materials for colloidal optoelectronics. In this work, we report the synthesis and characterization of CdSe/CdTe core/crown NPLs exhibiting a Type-II electronic structure and Type-II specific optical properties. Here, based on a core-seeded approach, the CdSe/CdTe core/crown NPLs were synthesized with well-controlled CdTe crown coatings. Uniform and epitaxial growth of CdTe crown region was verified by using structural characterization techniques including transmission electron microscopy (TEM) with quantitative EDX analysis and X-ray diffraction (XRD). Also the optical properties were systematically studied in these Type-II NPLs that reveal strongly red-shifted photoluminescence (up to similar to 150 nm) along with 2 orders of magnitude longer fluorescence lifetimes (up to 190 ns) compared to the Type-I NPLs owing to spatially indirect excitons at the Type-II interface between the CdSe core and the CdTe crown regions. Photoluminescence excitation spectroscopy confirms that this strongly red-shifted emission actually arises from the CdSe/CdTe NPLs. In addition, temperature-dependent time-resolved fluorescence spectroscopy was performed to reveal the temperature-dependent fluorescence decay kinetics of the Type-II NPLs exhibiting interesting behavior. Also, water-soluble Type-II NPLs were achieved via ligand exchange of the CdSe/CdTe core/crown NPLs by using 3-mercaptopropionic acid (MPA), which allows for enhanced charge extraction efficiency owing to their shorter chain length and enables high quality film formation by layer-by-layer (LBL) assembly. With all of these appealing properties, the CdSe/CdTe core/crown heterostructures having Type-II electronic structure presented here are highly promising for light-harvesting applications.

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