WoS İndeksli Yayınlar Koleksiyonu / WoS Indexed Publications Collection
Permanent URI for this collectionhttps://hdl.handle.net/11147/7150
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Article Citation - WoS: 7Citation - Scopus: 7Breaking the Boundaries of the Goldschmidt Tolerance Factor With Ethylammonium Lead Iodide Perovskite Nanocrystals(American Chemical Society, 2024) Güvenç, Çetin Meriç; Toso, Stefano; Ivanov, Yurii P.; Saleh, Gabriele; Balcı, Sinan; Divitini, Giorgio; Manna, LiberatoWe report the synthesis of ethylammonium lead iodide (EAPbI3) colloidal nanocrystals as another member of the lead halide perovskites family. The insertion of an unusually large A-cation (274 pm in diameter) in the perovskite structure, hitherto considered unlikely due to the unfavorable Goldschmidt tolerance factor, results in a significantly larger lattice parameter compared to the Cs-, methylammonium- and formamidinium-based lead halide perovskite homologues. As a consequence, EAPbI3 nanocrystals are highly unstable, evolving to a nonperovskite delta-EAPbI3 polymorph within 1 day. Also, EAPbI3 nanocrystals are very sensitive to electron irradiation and quickly degrade to PbI2 upon exposure to the electron beam, following a mechanism similar to that of other hybrid lead iodide perovskites (although degradation can be reduced by partially replacing the EA+ ions with Cs+ ions). Interestingly, in some cases during this degradation the formation of an epitaxial interface between (EA x Cs1-x )PbI3 and PbI2 is observed. The photoluminescence emission of the EAPbI3 perovskite nanocrystals, albeit being characterized by a low quantum yield (similar to 1%), can be tuned in the 664-690 nm range by regulating their size during the synthesis. The emission efficiency can be improved upon partial alloying at the A site with Cs+ or formamidinium cations. Furthermore, the morphology of the EAPbI3 nanocrystals can be chosen to be either nanocube or nanoplatelet, depending on the synthesis conditions.Article Citation - WoS: 17Citation - Scopus: 19Strong Coupling of Carbon Quantum Dots in Liquid Crystals(American Chemical Society, 2022) Sarısözen, Sema; Polat, Nahit; Mert Balcı, Fadime; Güvenç, Çetin Meriç; Kocabaş, Çoşkun; Yağlıoğlu, Halime Gül; Balcı, SinanCarbon quantum dots (CDs) have recently received a tremendous amount of interest owing to their attractive optical properties. However, CDs have broad absorption and emission spectra limiting their application ranges. We herein, for the first time, show synthesis of water-soluble red emissive CDs with a very narrow line width (∼75 meV) spectral absorbance and hence demonstrate strong coupling of CDs and plasmon polaritons in liquid crystalline mesophases. The excited state dynamics of CDs has been studied by ultrafast transient absorption spectroscopy, and CDs display very stable and strong photoluminescence emission with a quantum yield of 35.4% and a lifetime of ∼2 ns. More importantly, we compare J-aggregate dyes with CDs in terms of their absorption line width, photostability, and ability to do strong coupling, and we conclude that highly fluorescent CDs have a bright future in the mixed light-matter states for emerging applications in future quantum technologies.Article Citation - WoS: 7Citation - Scopus: 6L2[gaxfa1–xpbi3]pbi4 (0 ≤ X ≤ 1) Ruddlesden–popper Perovskite Nanocrystals for Solar Cells and Light-Emitting Diodes(American Chemical Society, 2022) Güvenç, Çetin Meriç; Tunç, İlknur; Balcı, SinanThe main challenges to overcome for colloidal 2D Ruddlesden–Popper (RP) organo-lead iodide perovskite nanocrystals (NCs) are phase instability and low photoluminescence quantum yield (PLQY). Herein, we demonstrate colloidal synthesis of guanidinium (GA)-L2[GAPbI3]PbI4, formamidinium (FA)-L2[FAPbI3]PbI4, and GA and FA alloyed L2[GA0.5FA0.5PbI3]PbI4 NCs without using polar or high boiling point nonpolar solvents. Importantly, we show that optical properties and phase stability of L2[APbI3]PbI4 NCs can be affectively tuned by alloying with guanidinium and formamidinium cations. Additionally, the band gap of NCs can be rapidly engineered by bromide ion exchange in L2[GAxFA1–xPbI3]PbI4 (0 ≤ x ≤ 1) NCs. Our approach produces a stable dispersion of L2[FAPbI3]PbI4 NCs with 12.6% PLQY that is at least three times higher than the previously reported PLQY in the nanocrystals. Furthermore, L2[GAPbI3]PbI4 and L2[GA0.5FA0.5PbI3]PbI4 NC films exhibit improved ambient stability over 10 days, which is significantly higher than L2[FAPbI3]PbI4 NC films, which transform to an undesired 1D phase within 6 days. The colloidally synthesized guanidinium- and formamidinium-based 2D RP organo-lead iodide perovskite NCs with improved stability and high PLQY demonstrated in this study may find applications in solar cells and light-emitting diodes. Therefore, large A-site cation-alloyed 2D RP perovskite NCs may provide a new way to rationalize high-performance and stable perovskite solar cells and light-emitting diodes.Article Citation - WoS: 16Citation - Scopus: 16Silylethynyl substitution for preventing aggregate formation in perylene diimides(American Chemical Society, 2021) Aksoy, Erkan; Danos, Andrew; Li, Chunyong; Monkman, Andrew P.; Varlıklı, CananEthynylene-bridged perylene diimides (PDIs) with different sized silane groups have been synthesized as a steric blocking group to prevent the formation of non-radiative trap sites, for example, strong H-aggregates and other dimers or excimers. Excited singlet-state exciton dynamics were investigated by time-resolved photoluminescence and ultrafast pump-probe transient absorption spectroscopy. The spectra of the excimer or dimer aggregates formed by the PDIs at high concentrations were also determined. Although the photophysical properties of the bare and shielded PDIs are identical at micromolar concentrations, more shielded PDI2 and PDI3 exhibited resistance to aggregation, retaining higher photoluminescence quantum yield even at 10 mM concentration and in neat films. The PDIs also exhibited high photostability (1 h of continuous excitation), as well as electrochemical stability (multiple cycles with cyclic voltammetry). Prevention of dimer/aggregate formation in this manner will extend the uses of PDIs to a variety of high concentration photonics and optoelectronic applications, such as organic light-emitting diodes, organic photovoltaics, and luminescent solar concentrators.Article Citation - WoS: 2Citation - Scopus: 31-Octanol Is a Functional Impurity Modifying Particle Size and Photophysical Properties of Colloidal Zncdsse/Zns Nanocrystals(American Chemical Society, 2021) Sevim Ünlütürk, Seçil; Çağır, Ali; Varlıklı, Canan; Özçelik, SerdarImpurities in trioctylphophine (TOP) strongly affect nanocrystal synthesis. 1-Octanol among other contaminants in TOP is identified for the first time as a functional impurity by H-1 NMR. The deliberate addition of 1-octanol into trioctylphosphine reduced particle size and modified photophysical properties of ZnCdSSe/ZnS colloidal nanocrystals. NMR analysis furthermore revealed that 1-octanol is bonded to the nanocrystal surfaces. The ratio of integrals for the O-CH2 protons of 1-octanol, which is the lowest compared to the other ligands, suggests that 1-octanol plays a critical role to tune the particle size of nanocrystals. The increased amount of 1-octanol added into TOP reduces the particle size from 9.8 to 7.2 nm, causing a progressive blue shift in the UV-vis and PL spectra but leaving the alloy composition unaffected. The rate of nonradiative processes is enhanced with the amount of 1-octanol added into TOP, correlating with higher dislocation density observed in the nanocrystals. As a conclusion, 1-octanol is proposed as a functional impurity that varies particle size and nonradiative photophysical processes in the ZnCdSSe/ZnS colloidal nanocrystals.Article Citation - WoS: 13Citation - Scopus: 15Hybrid J-aggregate-graphene phototransistor(American Chemical Society, 2020) Yakar, Ozan; Balcı, Osman; Uzlu, Burkay; Polat, Nahit; Arı, Ozan; Tunç, İlknur; Balcı, SinanJ-aggregates are fantastic self-assembled chromophores with a very narrow and extremely sharp absorbance band in the visible and near-infrared spectrum, and hence they have found many exciting applications in nonlinear optics, sensing, optical devices, photography, and lasing. In silver halide photography, for example, they have enormously improved the spectral sensitivity of photographic process due to their fast and coherent energy migration ability. On the other hand, graphene, consisting of single layer of carbon atoms forming a hexagonal lattice, has a very low absorption coefficient. Inspired by the fact that J-aggregates have carried the role to sense the incident light in silver halide photography, we would like to use Jaggregates to increase spectral sensitivity of graphene in the visible spectrum. Nevertheless, it has been an outstanding challenge to place isolated J-aggregate films on graphene to extensively study interaction between them. We herein noncovalently fabricate isolated J-aggregate thin films on graphene by using a thin film fabrication technique we termed here membrane casting (MC). MC significantly simplifies thin film formation of water-soluble substances on any surface via porous polymer membrane. Therefore, we reversibly modulate the Dirac point of graphene in the J-aggregate/graphene van der Waals (vdW) heterostructure and demonstrate an all-carbon phototransistor gated by visible light. Owing to the hole transfer from excited excitonic thin film to graphene layer, graphene is hole-doped. In addition, spectral and power responses of the all-carbon phototransistor have been measured by using a tunable laser in the visible spectrum. The first integration of J-aggregates with graphene in a transistor structure enables one to reversibly write and erase charge doping in graphene with visible light that paves the way for using J-aggregate/graphene vdW heterostructures in optoelectronic applications.Article Citation - WoS: 8Citation - Scopus: 8Reducing the Efficiency Roll Off and Applied Potential-Induced Color Shifts in Cdse@zns/Zns-based Light-Emitting Diodes(American Chemical Society, 2020) Özgüler, Şahika; Diker, Halide; Ünlütürk, Seçil Sevim; Özçelik, Serdar; Varlıklı, CananGreen light-emitting CdSe@ZnS/ZnS (QD) nano-particles were synthesized; the photophysical and morphological properties of their films, which were prepared by spin coating from six different concentrations, corresponding to absorbance values of 0.6, 1.1, 1.6, 2.1, 2.8, and 4.0, were determined. Increasing the absorbance value from 0.6 to 4.0 did not change the photophysical properties of QD films to a large extent, whereas it resulted in an increment in QD film thickness from 20 to 110 nm. The films were utilized as an emissive layer in QD light-emitting diodes with poly(9-vinylcarbazole) (PVK), PVK:2-(4-biphenyllyl)-5-(4-tert-butylphenyl)-1,3,4-oxadiazole (PBD), and PVK:1,3-bis[(4-tert-butylphenyl)-1,3,4-oxadiazolyl]-phenylene (OXD-7) hole-transport layers (HTLs). The presence of PBD or OXD-7 in PVK reduced the efficiency values but played a positive role in the color purity and efficiency roll off. The maximum color temperature and electroluminescence wavelength shifts obtained with applied potential were 109, 50, and 50 K and 11, 5, and 5 nm for pure-PVK, PVK:PBD, and PVK:OXD-7-based devices, respectively. Hole mobility, capacitance (at 10(3) Hz), and charge-transfer efficiency values were 9.0 x 10(-7), 6.8 x 10(-7), and 4.2 x 10(-7) cm(2) V s(-1), 1.7, 1, and 1 nF, and 6.90%, 15.50%, and 16.10% for pure-PVK, PVK:PBD, and PVK:OXD-7-based devices, respectively. Enhanced color purity and lowered efficiency roll off obtained with PVK:PBD and PVK:OXD-7 HTLs were attributed to decreased capacitance, increased charge-transfer efficiency, and reduced Joule heating.Article Citation - WoS: 4Citation - Scopus: 4Color-Tunable All-Inorganic Cspbbr3 Perovskites Nanoplatelet Films for Photovoltaic Devices(American Chemical Society, 2019) Özcan, Mehmet; Özen, Sercan; Topçu, Gökhan; Demir, Mustafa Muammer; Şahin, HasanHerein, we demonstrate a novel coating approach to fabricate CsPbBr3 perovskite nanoplatelet film with heat-free process via electrospraying from precursor solution. A detailed study is carried out to determine the effect of various parameters such as ligand concentration, electric field, flow rate, etc. on the optical properties. By controlling the volume ratios of the oleylamine (OAm) and oleic acid (OA), the coalescing and thickness of the resulting nanoplatelets can be readily tuned that results in control over emission in the range of 100 nm without any antisolvent crystallization or heating processes. The varying electrical field and flow rate was found as inefficient on the emission characteristics of the films. In addition, the crystal films were obtained under ambient conditions on the ITO coated glass surfaces as in the desired pattern. As a result, we demonstrated a facile and reproducible way of synthesizing and coating of CsPbBr3 perovskite nanoplatelets which is suitable for large-scale production. In this method, the ability of tuning the degree of quantum confinement for perovskite nanoplatelets is promising approach for the one-step fabrication of crystal films that may enable the use in optoelectronics.Article Citation - WoS: 35Citation - Scopus: 40Two-Dimensional Covalent Crystals by Chemical Conversion of Thin Van Der Waals Materials(American Chemical Society, 2019) Sreepal, Vishnu; Yağmurcukardeş, Mehmet; Vasu, Kalangi S.; Kelly, Daniel J.; Taylor, Sarah F. R.; Şahin, Hasan; Kravets, Vasyl G.; Nair, Rahul R.Most of the studied two-dimensional (2D) materials have been obtained by exfoliation of van der Waals crystals. Recently, there has been growing interest in fabricating synthetic 2D crystals which have no layered bulk analogues. These efforts have been focused mainly on the surface growth of molecules in high vacuum. Here, we report an approach to making 2D crystals of covalent solids by chemical conversion of van der Waals layers. As an example, we used 2D indium selenide (InSe) obtained by exfoliation and converted it by direct fluorination into indium fluoride (InF3), which has a nonlayered, rhombohedral structure and therefore cannot possibly be obtained by exfoliation. The conversion of InSe into InF3 is found to be feasible for thicknesses down to three layers of InSe, and the obtained stable InF3 layers are doped with selenium. We study this new 2D material by optical, electron transport, and Raman measurements and show that it is a semiconductor with a direct bandgap of 2.2 eV, exhibiting high optical transparency across the visible and infrared spectral ranges. We also demonstrate the scalability of our approach by chemical conversion of large-area, thin InSe laminates obtained by liquid exfoliation, into InF3 films. The concept of chemical conversion of cleavable thin van der Waals crystals into covalently bonded noncleavable ones opens exciting prospects for synthesizing a wide variety of novel atomically thin covalent crystals.Article Citation - WoS: 28Citation - Scopus: 28Enhanced Stability of Single-Layer W-Gallenene Through Hydrogenation(American Chemical Society, 2018) Badalov, S. V.; Yağmurcukardeş, Mehmet; Peeters, François M.; Şahin, HasanUsing density functional theory based first-principles calculations, the effect of surface hydrogenation on the structural, dynamical, electronic, and mechanical properties of monolayer washboard-gallenene (w-gallenene) is investigated. It is found that the dynamically stabilized strained monolayer of w-gallenene has a metallic nonmagnetic ground state. Both one-sided and two-sided hydrogenations of w-gallenene suppress its dynamical instability even when unstrained. Unlike one-sided hydrogenated monolayer w-gallenene (os-w-gallenene), two-sided hydrogenated monolayer w-gallenene (ts-w-gallenene) possesses the same crystal structure as w-gallenene. Electronic band structure calculations reveal that monolayers of hydrogenated derivatives of w-gallenene exhibit also metallic nonmagnetic ground state. Moreover, the linear-elastic constants, in-plane stiffness and Poisson ratio, are enhanced by hydrogenation, which is opposite to the behavior of other hydrogenated monolayer crystals. Furthermore, monolayer w-gallenene and ts-w-gallenene remain dynamically stable up to relatively higher biaxial strains as compared to borophene. With its enhanced dynamical stability, robust metallic character, and enhanced linear-elastic properties, hydrogenated monolayer w-gallenene is a potential candidate for nanodevice applications as a two-dimensional flexible metal.
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