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: 13Citation - Scopus: 13Tuning the Shades of Red Emission in InP/ZnSe Nanocrystals With Narrow Full Width for Fabrication of Light-Emitting Diodes(Amer Chemical Soc, 2023-10-13) Soheyli, Ehsan; Bicer, Aysenur; Ozel, Sultan Suleyman; Tiras, Kevser Sahin; Mutlugun, Evren; Sahin Tiras, KevserWhile Cd-based luminescent nanocrystals (NCs) are the most mature NCs for fabricating efficient red light-emitting diodes (LEDs), their toxicity related limitation is inevitable, making it necessary to find a promising alternative. From this point of view, multishell-coated, red-emissive InP-based NCs are excellent luminescent nanomaterials for use as an emissive layer in electroluminescent (EL) devices. However, due to the presence of oxidation states, they suffer from a wide emission spectrum, which limits their performance. This study uses tris-(dimethyl-amino)-phosphine (3DMA-P) as a low-cost aminophosphine precursor and a double HF treatment to suggest an upscaled, cost-effective, and one-pot hot-injection synthesis of purely red-emissive InP-based NCs. The InP core structures were coated with thick layers of ZnSe and ZnS shells to prevent charge delocalization and to create a narrow size distribution. The purified NCs showed an intense emission signal as narrow as 43 nm across the entire red wavelength range (626-670 nm) with an emission quantum efficiency of 74% at 632 nm. The purified samples also showed an emission quantum efficiency of 60% for far-red wavelengths of 670 nm with a narrow full width of 50 nm. The samples showed a relatively long average emission lifetime of 50-70 ns with a biexponential decay profile. To demonstrate the practical ability of the prepared NCs in optoelectronics, we fabricated a red-emissive InP-based LEDs. The best-performing device showed an external quantum efficiency (EQE) of 1.16%, a luminance of 1039 cd m(-2), and a current efficiency of 0.88 cd A(-1).Article Citation - WoS: 6Citation - Scopus: 7Tailored Synthesis of Iron Oxide Nanocrystals for Formation of Cuboid Mesocrystals(Amer Chemical Soc, 2021-08-02) Soran-Erdem, Zeliha; Sharma, Vijay Kumar; Hernandez-Martinez, Pedro Ludwig; Demir, Hilmi VolkanIn this work, we systematically studied the shape- and size-controlled monodisperse synthesis of iron oxide nanocrystals (IONCs) for their use as building blocks in the formation of mesocrystals. For this aim, on understanding the influence of the oleic acid concentration, iron-oleate concentration, and heating rate on the synthesis of robust and reproducible IONCs with desired sizes and shapes, we synthesized highly monodisperse similar to 11 nm sized nanocubes and nanospheres. Magnetic measurements of both cubic and spherical IONCs revealed the presence of mixed paramagnetic and superparamagnetic phases in these nanocrystals. Moreover, we observed that the magnetic moments of the nanocubes are more substantial compared to their spherical counterparts. We then demonstrated a simple magnetic-field-assisted assembly of nanocubes into three-dimensional (3D) cuboid mesocrystals while nanospheres did not form any mesocrystals. These findings indicate that small cubic nanocrystals hold great promise as potential building blocks of 3D magnetic hierarchical structures with their superior magnetic properties and mesocrystal assembly capability, which may have high relevance in various fields ranging from high-density data storage to biomedical applications.Article Citation - WoS: 13Citation - Scopus: 13Sulfobetaine-Based Homo- and Copolymers by Raft: Cross-Linked Micelles and Aqueous Solution Properties(Amer Chemical Soc, 2022-08-04) Gurdap, Seda; Bayram, Nazende Nur; Isoglu, Ismail Alper; Isoglu, Sevil Dincer; Dinçer İşoǧlu, SevilIn this study, we describe the synthesis and aqueous solution behavior of temperature-sensitive N-(3-sulfopropyl)-N-methacroyloxyethyl-N,N-dimethylammonium betaine (SBMA) homopolymers and core cross-linked micelles (CCMs) with an SBMA shell. Reversible addition- fragmentation chain transfer polymerization has been utilized to synthesize sulfobetaine homopolymers, followed by CCM formation during copoly-merization in the presence of an acid-degradable cross-linker. First, SBMA homopolymers of varying chain lengths were synthesized, and it has been demonstrated that an increase in the chain length and concentration of the homopolymer resulted in an increase in the upper critical solution temperature (UCST). Besides, micelles showed concentration-dependent dual temperature-sensitive behavior with UCST and LCST transitions. Also, homopolymers and CCMs were characterized by FTIR, H-1-NMR, GPC, and TEM. Micelle formation and temperature sensitivity were also investigated by DLS. As a result, stabilized micelles were successfully prepared with the motivation of preventing premature drug release and achieving a pH-and temperature-controlled system. Due to their dual-responsive characteristics, the CCMs show promising potential to be used as smart drug carriers for controlled delivery.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: 11Citation - Scopus: 13Solution-Processable Indenofluorenes on Polymer Brush Interlayer: Remarkable N-Channel Field-Effect Transistor Characteristics Under Ambient Conditions(Amer Chemical Soc, 2023-08-15) Can, Ayse; Deneme, Ibrahim; Demirel, Gokhan; Usta, HakanThe development of solution-processable n-type molecularsemiconductorsthat exhibit high electron mobility (& mu;(e) & GE;0.5 cm(2)/(V & BULL;s)) under ambient conditions, along withhigh current modulation (I (on)/I (off) & GE; 10(6)-10(7)) andnear-zero turn on voltage (V (on)) characteristics,has lagged behind that of other semiconductors in organic field-effecttransistors (OFETs). Here, we report the design, synthesis, physicochemicaland optoelectronic characterizations, and OFET performances of a libraryof solution-processable, low-LUMO (-4.20 eV) 2,2 & PRIME;-(2,8-bis(3-alkylthiophen-2-yl)indeno[1,2-b]fluorene-6,12-diylidene)dimalononitrile small molecules, & beta;,& beta;& PRIME;-C (n) -TIFDMTs, having varied alkyl chain lengths (n = 8, 12, 16). An intriguing correlation is identifiedbetween the solid-isotropic liquid transition enthalpies andthe solubilities, indicating that cohesive energetics, which are tunedby alkyl chains, play a pivotal role in determining solubility. Thesemiconductors were spin-coated under ambient conditions on denselypacked (grafting densities of 0.19-0.45 chains/nm(2)) ultrathin (& SIM;3.6-6.6 nm) polystyrene-brush surfaces.It is demonstrated that, on this polymer interlayer, thermally induceddispersive interactions occurring over a large number of methyleneunits between flexible alkyl chains (i.e., zipper effect) are criticalto achieve a favorable thin-film crystallization with a proper microstructureand morphology for efficient charge transport. While C-8 and C-16 chains show a minimal zipper effect upon thermalannealing, C-12 chains undergo an extended interdigitationinvolving & SIM;6 methylene units. This results in the formationof large crystallites having lamellar stacking ((100) coherence length & SIM;30 nm) in the out-of-plane direction and highly favorablein-plane & pi;-interactions in a slipped-stacked arrangement. Uninterruptedmicrostructural integrity (i.e., no face-on (010)-oriented crystallites)was found to be critical to achieving high mobilities. The excellentcrystallinity of the C-12-substituted semiconductor thinfilm was also evident in the observed crystal lattice vibrations (phonons)at 58 cm(-1) in low-frequency Raman scattering. Two-dimensionalmicrometer-sized (& SIM;1-3 & mu;m), sharp-edged plate-likegrains lying parallel with the substrate plane were observed. OFETsfabricated by the current small molecules showed excellent n-channelbehavior in ambient with & mu;(e) values reaching & SIM;0.9cm(2)/(V & BULL;s), I (on)/I (off) & SIM; 10(7)-10(8), and V (on) & AP; 0 V. Our study notonly demonstrates one of the highest performing n-channel OFET devicesreported under ambient conditions via solution processing but alsoelucidates significant relationships among chemical structures, molecularproperties, self-assembly from solution into a thin film, and semiconductingthin-film properties. The design rationales presented herein may openup new avenues for the development of high-electron-mobility novelelectron-deficient indenofluorene and short-axis substituted donor-acceptor & pi;-architectures via alkyl chain engineering and interface engineering.Article Citation - WoS: 25Citation - Scopus: 25Self-Resonant Microlasers of Colloidal Quantum Wells Constructed by Direct Deep Patterning(Amer Chemical Soc, 2021-05-24) Gheshlaghi, Negar; Foroutan-Barenji, Sina; Erdem, Onur; Altintas, Yemliha; Shabani, Farzan; Humayun, Muhammad Hamza; Demir, Hilmi VolkanHere, the first account of self-resonant fully colloidal mu-lasers made from colloidal quantum well (CQW) solution is reported. A deep patterning technique is developed to fabricate well-defined high aspect-ratio on-chip CQW resonators made of grating waveguides and in-plane reflectors. The fabricated waveguide-coupled laser, enabling tight optical confinement, assures in-plane lasing. CQWs of the patterned layers are closed-packed with sharp edges and residual-free lifted-off surfaces. Additionally, the method is successfully applied to various nanoparticles including colloidal quantum dots and metal nanoparticles. It is observed that the patterning process does not affect the nanocrystals (NCs) immobilized in the attained patterns and the different physical and chemical properties of the NCs remain pristine. Thanks to the deep patterning capability of the proposed method, patterns of NCs with subwavelength lateral feature sizes and micron-scale heights can possibly be fabricated in high aspect ratios.Article Citation - WoS: 27Citation - Scopus: 29Revisiting the Role of Charge Transfer in the Emission Properties of Carborane-Fluorophore Systems: A TDDFT Investigation(Amer Chemical Soc, 2022-06-05) Tahaoglu, Duygu; Usta, Hakan; Alkan, FahriIn this study, we performed a detailed investigation of the S-1 potential energy surface (PES) of o-carborane-anthracene (o-CB-Ant) with respect to the C-C bond length on o-CB and the dihedral angle between o-CB and Ant moieties. The effects of different substituents (F, Cl, CN, and OH) on carbon- or boron-substituted o-CB, along with a pi-extended acene-based fluorophore, pentacene, on the nature and energetics of S-1 -> S-0 transitions are evaluated. Our results show the presence of a non-emissive S-1 state with an almost pure charge transfer (CT) character for all systems as a result of significant C-C bond elongation (C-C = 2.50-2.56 angstrom) on o-CB. In the case of unsubstituted o-CB-Ant, the adiabatic energy of this CT state corresponds to the global minimum on the S-1 PES, which suggests that the CT state could be involved in emission quenching. Despite large deformations on the o-CB geometry, predicted energy barriers are quite reasonable (0.3-0.4 eV), and the C-C bond elongation can even occur without a noticeable energy penalty for certain conformations. With substitution, it is shown that the dark CT state becomes even more energetically favorable when the substituent shows -M effects (e.g., -CN), whereas substituents showing +M effects (e.g., -OH) can result in an energy increase for the CT state, especially for partially stretched C-C bond lengths. It is also shown that the relative energy of the CT state on the PES depends strongly on the LUMO level of the fluorophore as this state is found to be energetically less favorable compared to other conformations when anthracene is replaced with pi-extended pentacene. To our knowledge, this study shows a unique example of a detailed theoretical analysis on the PES of the S-1 state in o-CB-fluorophore systems with respect to substituents or fluorophore energy levels. Our findings could guide future experimental work in emissive o-CB-fluorophore systems and their sensing/optoelectronic applications.
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