WoS İndeksli Yayınlar Koleksiyonu
Permanent URI for this collectionhttps://hdl.handle.net/20.500.12573/394
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Article Citation - WoS: 2Citation - Scopus: 1Fully Inorganic Colloidal CsPbBr3 Perovskite Nanocrystals with Zn-Doping and Metal Oxide Encapsulation for Luminescent Display Panels(Amer Chemical Soc, 2025-11-07) Khorasani, Azam; Soheyli, Ehsan; Mutlugun, EvrenPerovskite nanocrystals (PeNCs) are emerging as exceptional materials due to their high photoluminescence quantum yield, tunable bandgap, and excellent charge carrier mobility, enabling a wide range of colors and promising applications in optoelectronics and photovoltaics. Despite their advantages, PeNCs face stability challenges caused by environmental factors. In the presented study, a facile and versatile colloidal hot-injection method was used to apply the beneficial aspects of Zn-doping in cesium lead bromide (CsPbBr3) PeNCs. The uniform platelet-shaped Zn-doped CsPbBr3 PeNCs were prepared by doping with a 0.1 molar ratio of zinc-oleate solution in the perovskite precursors during synthesis. Then, zinc-oxide (ZnO) and nickel-oxide (NiO) coating layers were utilized separately to effectively reduce surface defects, encapsulate PeNCs, and improve their stability issues. To fabricate the coated PeNCs with metal oxides, zinc acetate and nickel(II) acetate tetrahydrate solutions were prepared individually and added to the crude perovskite solutions. The quantum yield of Zn-doped CsPbBr3 (CsPb1-xZnxBr3) PeNCs coated with ZnO increased from 50% for bare CsPbBr3 to over 84%, while NiO-coated PeNCs exhibited a higher yield of 90% both of which remarkably enhanced the emission stability. Moreover, NiO coatings represented a proper protection against surface imperfections and improved resistance to external stimuli. The combination of facile/effective preparation method, excellent emission efficiency, and reliable emission stability nominates the prepared colloidal composite for display pixels, detectors, and lasers.Article Citation - WoS: 13Citation - Scopus: 11Understanding the Effect of Symmetry Breaking on Plasmon Coupling From TDDFT(Amer Chemical Soc, 2021-05-26) Alkan, Fahri; Aikens, Christine M.We perform a time-dependent density functional theory (TDDFT) investigation for the optical properties of nanorod assemblies for different sizes (Ag-10, Ag-59, and Ag-139), interparticle distances, and orientations with a focus on the effect of symmetry breaking via an angle on plasmon coupling. For the model systems, the angle (theta) between the particles is varied between 0 and 180 degrees, where theta = 0 degrees and theta = 180 degrees correspond to symmetric side-by-side and end-to-end orientations of the nanorods, respectively. Our analysis reveals that for a sufficiently large interparticle distance (r > 0.7 nm), where the wave-function overlap between monomers is negligible, TDDFT results agree quite well with the predictions of the dipole-dipole interaction model for the intensity of the different modes of coupled plasmons. For smaller gap distances (0.4-0.5 nm), a charge-transfer plasmon (CTP) mode occurs for the symmetry broken case of the Ag-10 dimer. For the assemblies of larger nanorods, however, the CTP mode is predicted to be less pronounced, especially for the cases where the deviation from the end-to-end geometry is larger than 30 degrees. The orbital overlap and configuration-interaction analyses show that these results are related to the fact that the relative overlap strength between monomeric energy levels is significantly reduced for symmetry-broken orientations of larger nanorods.Article Citation - WoS: 19Citation - Scopus: 19Understanding and Tailoring Excited State Properties in Solution-Processable Oligo(p-Phenyleneethynylene)s: Highly Fluorescent Hybridized Local and Charge Transfer Character via Experiment and Theory(Amer Chemical Soc, 2021-10-13) Usta, Hakan; Cosut, Bunyemin; Alkan, FahriRod-shaped oligo(p-phenyleneethynylene) (OPE) offers an attractive p-framework for the development of solution-processable highly fluorescent molecules having tunable hybridized local and charge transfer (HLCT) excited states and (reverse) intersystem crossing ((R)ISC) channels. Herein, an HLCT oligo(p-phenyleneethynylene) library was studied for the first time in the literature in detail systematically via experiment and theory. The design, synthesis, and full characterization of a new highly fluorescent (Phi(PL-solution) similar to 1) sky blue emissive 4',4 ''-((2,5-bis((2-ethylhexyl)oxy)-1,4-phenylene)bis(ethyne-2,1-diyl))bis(N,N-diphenyl-[1,1'-bi-phenyl]-4-amine) (2EHO-TPA-PE) was also reported. The new molecule consists of a D'-Ar-pi-D-pi-Ar-D' molecular architecture with an extended pi-spacer and no acceptor unit, and detailed structural, physicochemical, single-crystal, and optoelectronic characterizations were performed. A high solid-state quantum efficiency (Phi(PL-solution) similar to 0.8) was achieved as a result of suppressed exciton-phonon/vibronic couplings (no pi-pi interactions and multiple (14 per dimeric form) strong C-H center dot center dot center dot pi interactions). Strong solution-phase/solid-state dipole-dependent tunable excited state behavior (local excited (LE) -> HLCT -> charge transfer (CT)) and decay dynamics covering a wide spectral region were demonstrated, and the CT state was observed to be highly fluorescent despite extremely large Stokes shift (similar to 130 nm)/fwhm (similar to 125 nm) and significant charge separation (0.75 charge.nm). Employing the Lippert-Mataga model, along with detailed photophysical studies and TDDFT calculations, key relationships between molecular design-electronic structure-exciton characteristics were elucidated with regards to HLCT and hot exciton channel formations. The interstate coupling between CT and LE states and the interplay of this coupling with respect to medium polarity were explored. A key relationship between excited-state symmetry breaking process and the formation of HLCT state was discussed for TPA-ended rod-shaped OPE p-systems. (R)ISC-related delayed fluorescence (tau similar to 2-6 ns) processes were evident following the prompt decays (similar to 0.4-0.9 ns) both in the solution and in the solid-state. As a unique observation, the delayed fluorescence could be tuned and facilitated via small dielectric changes in the medium. Our results and the molecular engineering perspectives presented in this study may provide unique insights into the structural and electronic factors governing tunable excited state and hot-exciton channel formations in OPEs for (un)conventional solution-processed luminescence applications.Article Citation - WoS: 18Citation - Scopus: 18Ultrahigh Vacuum Self-Assembly of Rotationally Commensurate C8-BTBT/MoS2 Mixed-Dimensional Heterostructures(Amer Chemical Soc, 2019-02-12) Liu, Xiaolong; Balla, Itamar; Sangwan, Vinod K.; Usta, Hakan; Facchetti, Antonio; Marks, Tobin J.; Hersam, Mark C.Mixed-dimensional van der Waals heterostructures combine the advantages of nanomaterials with qualitatively distinct properties such as the extended bandstructures and high charge carrier mobilities of inorganic two-dimensional materials and the discrete orbital energy levels and strong optical absorption of zero-dimensional organic molecules. The synergistic interplay between nanomaterials of distinct dimensionality has enabled a variety of unique applications such as antiambipolar transistors, sensitized photodetectors, and gate-tunable photovoltaics. Because the performance of mixed-dimensional heterostructure devices depends sensitively on the buried interfacial structure, it is of great interest to identify materials and chemistries that naturally form highly ordered heterointerfaces. Toward this end, here we demonstrate ultrahigh vacuum self-assembly of 2,7-dioctyl[1]benzothieno [3,2-b][1]benzothiophene (C8-BTBT) monolayers onto epitaxial MoS2/graphene heterostructures. With molecular-resolution scanning tunneling microscopy and spectroscopy, the resulting C8-BTBT/MoS2/graphene mixed-dimensional heterostructures are found to be rotationally commensurate with well-defined physical and electronic structures. It is further shown that the self-assembled C8-BTBT monolayers are insensitive to the structural defects and electronic perturbations of the underlying MoS2 substrate, which provides significant processing latitude. For these reasons, this work will facilitate ongoing efforts to utilize organic/MoS2/graphene mixed-dimensional heterostructures for electronic, optoelectronic, and photovoltaic applications.Article Citation - WoS: 4Citation - Scopus: 4Transparent Films Made of Highly Scattering Particles(Amer Chemical Soc, 2020-01-13) Erdem, Talha; Yang, Lan; Xu, Peicheng; Altintas, Yemliha; O'Neil, Thomas; Caciagli, Alessio; Eiser, ErikaToday, colloids are widely employed in various products from creams and coatings to electronics. The ability to control their chemical, optical, or electronic features by controlling their size and shape explains why these materials are so widely preferred. Nevertheless, altering some of these properties may also lead to some undesired side effects, one of which is an increase in optical scattering upon concentration. Here, we address this strong scattering issue in films made of binary colloidal suspensions. In particular, we focus on raspberry-type polymeric particles made of a spherical polystyrene core decorated by small hemispherical domains of acrylate with an overall positive charge, which display an unusual stability against aggregation in aqueous solutions. Their solid films display a brilliant red color due to Bragg scattering but appear completely white on account of strong scattering otherwise. To suppress the scattering and induce transparency, we prepared films by hybridizing them with oppositely charged PS particles with a size similar to that of the bumps on the raspberries. We report that the smaller PS particles prevent raspberry particle aggregation in solid films and suppress scattering by decreasing the spatial variation of the refractive index inside the film. We believe that the results presented here provide a simple strategy to suppress strong scattering of larger particles to be used in optical coatings.Article Citation - WoS: 28Citation - Scopus: 29Three-Dimensional Au-Coated Electrosprayed Nanostructured BODIPY Films on Aluminum Foil as Surface-Enhanced Raman Scattering Platforms and Their Catalytic Applications(Amer Chemical Soc, 2017-05-16) Yilmaz, Mehmet; Erkartal, Mustafa; Ozdemir, Mehmet; Sen, Unal; Usta, Hakan; Demirel, GokhanThe design and development of three-dimensional (3D) nanostructures with high surface-enhanced Raman scattering (SERS) performances have attracted considerable attention in the fields of chemistry, biology, and materials science. Nevertheless, electrospraying of organic smalt molecules on low-cost flexible substrates has never been studied to realize large-scale SERS-active platforms. Here, we report the facile, efficient, and low-cost fabrication of-Stable and reproducible Au-coated electrosprayed organic semiconductor films (Au@BDY-4TEBDY) on flexible regular aluminum foil at a large scale (5 cm X 5 cm) for practical SERS and catalytic applications. To this end, a well-designed-acceptor-donor-atceptor-type solution-processable molecular semiconductor, BDY-4T-BDY, developed by our group, is used because of its advantageous structural and electrical properties. The morphology of the electrosprayed organic film changes by solution concentration, and two different 3D morphologies with out-of-plane features are obtained. Highly uniform dendritic nanoribbons with sharp needle-like tips and vertically oriented nanoplates (similar to 50 nm thickness) are achieved when electrospraying solution concentrations of 240 and 253% w/v.(mgimL) are, respectively, used. When these electrosprayed organic films are coated with a nanoscopic thin (30 nm) Au layer, the resulting Au@BDY-4T-BDY platforms demonstrate remarkable SERS enhancement factors up to 1.7 X 10(6) with excellent Raman signal reproducibility (relative standard deviation <= 0.13) for methylene blue over the entire film. Finally, Au@BDY-4T-BDY films showed good catalytic activity for the reduction of 4-nitrophenol to 4-aminophenol with rate constants of 1.3 X 10(-2) and 9.2 X 10(-3) min(-1). Our results suggest that electrospraying of rationally designed organic semiconductor molecules on flexible substrates holds great promise to enable low-cost, solution-processed, SERS-active platforms.Article Citation - WoS: 14Citation - Scopus: 13Spectrally Tunable White Light-Emitting Diodes Based on Carbon Quantum Dot-Doped Poly(N-Vinylcarbazole) Composites(Amer Chemical Soc, 2024-01-26) Sahin Tiras, Kevser; Bicer, Aysenur; Soheyli, Ehsan; Mutlugun, EvrenElectroluminescent white light-emitting diodes (WLEDs) are always of great interest for emerging display applications. Carbon-based quantum dots (CQDs) are the newest emerging nanoscale materials that can be employed for this purpose, owing to their broad and bright light emission properties. In the present work, highly luminescent CQDs with an emission quantum yield of 60% were prepared via a colloidal solvothermal method and subsequent silica gel column chromatography. The photoluminescence (PL) peak was located at 550 nm possessing yellow emission, with a full width at half-maximum of 98 nm and a relatively long lifetime of 10.23 ns through a single-exponential recombination pathway. CQDs were employed in an electroluminescent device architecture of an ITO/PEDOT:PSS/TFB/CQD:PVK/TPBi/LiF/Al structure and blended with poly(N-vinylcarbazole) (PVK) to evaluate their ability to reach white electroluminescent emission. Results confirmed a high external quantum efficiency (EQE) of 0.76% and a maximum luminescence of 774.3 cd<middle dot>m(-2). Tuning the ratio between CQDs and PVK from 1:10.25 to 1:5.75 resulted in a systematic shift in CIE x-y coordinates from 0.23-0.26 to 0.21-0.24, located close to the cool white region. The results of the present study can be considered a step forward in fabricating efficient WLEDs based on low-cost CQDs.Article Citation - WoS: 61Citation - Scopus: 74Solution-Processable Bodipy-Based Small Molecules for Semiconducting Microfibers in Organic Thin-Film Transistors(Amer Chemical Soc, 2016-05-23) Ozdemir, Mehmet; Choi, Donghee; Kwon, Guhyun; Zorlu, Yunus; Cosut, Bunyemin; Kim, Hyekyoung; Usta, HakanElectron-deficient pi-conjugated small molecules can function as electron-transporting semiconductors in various optoelectronic applications. Despite their unique structural, optical, and electronic properties, the development of BODIPY-based organic semiconductors has lagged behind that of other pi-deficient units. Here, we report the design and synthesis of two novel solution-proccessable BODIPY-based small molecules (BDY-3T-BDY and BDY-4T-BDY) for organic thin-film transistors (OTFTs). The new semiconductors were fully characterized by H-1/C-13 NMR, mass spectrometry, cyclic voltammetry, UV-vis spectroscopy, photoluminescence, differential scanning calorimetry, and thermogravimetric analysis. The single-crystal X-ray diffraction (XRD) characterization of a key intermediate reveals crucial structural properties. Solution-sheared top-contact/bottom-gate OTFTs exhibited electron mobilities up to 0.01 cm(2)/V center dot s and current on/off ratios of >10(8). Film microstructural and morphological characterizations indicate the formation of relatively long (similar to 0.1 mm) and micrometer-sized (1-2 mu m) crystalline fibers for BDY-4T-BDY-based films along the shearing direction. Fiber-alignment-induced charge-transport anisotropy (mu?/mu approximate to 10) was observed, and higher mobilities were achieved when the microfibers were aligned along the conduction channel, which allows for efficient long-range charge-transport between source and drain electrodes. These OTFT performances are the highest reported to date for a BODIPY-based molecular semiconductor, and demonstrate that BODIPY is a promising building block for enabling solution-processed, electron-transporting semiconductor films.Article Citation - WoS: 16Citation - Scopus: 17Solid-State Encapsulation and Color Tuning in Films of Cesium Lead Halide Perovskite Nanocrystals for White Light Generation(Amer Chemical Soc, 2019-01-30) Torun, Ilker; Altintas, Yemliha; Yazici, Ahmet Faruk; Mutlugun, Evren; Onses, M. SerdarPerovskite nanocrystals (PNCs) are highly demanding nanomaterials for solid-state lighting applications. A challenge for their exploitation in practical applications is the insufficient ambient and water stability associated with their ionic nature. Here we report a novel route for solid-state encapsulation of films of perovskite nanocrystals (PNCs) through vapor-phase deposition of a thin and hydrophobic layer of fluoroalkyltrichlorosilanes (FAS). High quality nanoscale crystals of CsPbBr3 were synthesized with well established colloidal methods and coated on solid substrates. The films of PNCs were then subjected to vapor of FAS for short durations of time (<60 s) in ambient atmosphere, resulting in deposition of a thin (<20 nm) hydrophobic layer. Besides providing a barrier for water and humidity, the vapor-phase deposition of FAS was accompanied by the blue shift of the emission wavelength of the PNCs. The color shift results from the partial exchange of Br with Cl anions, which emerge during the self-hydrolysis of the silane molecules. Throughout this process, we demonstrate the enhanced water stability of the films of PNCs and fine tunability of the wavelength in films from 516 nm to 488 nm. The fabrication of a white-light-emitting diode and tunability of the color coordinates with the duration of the FAS deposition were demonstrated. The rapid, scalable, and inexpensive solid-state encapsulation approach shows great promise for films of halide perovskites.Conference Object Selective Dye Uptake From Aqueous Industrial Waste Mixtures by Novel Covalent Organic Frameworks(Amer Chemical Soc, 2015) Filikci, Semra; Ulasan, Mehmet; Citir, Murat; Yavuz, Mustafa