Photonics / Fotonik
Permanent URI for this collectionhttps://hdl.handle.net/11147/2590
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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: 1Citation - Scopus: 1Calcium Indicators With Fluorescence Lifetime-Based Signal Readout: a Structure-Function Study(MDPI, 2024) Simonyan, Tatiana R.; Varfolomeeva, Larisa A.; Mamontova, Anastasia V.; Kotlobay, Alexey A.; Gorokhovatsky, Andrey Y.; Bogdanov, Alexey M.; Boyko, Konstantin M.The calcium cation is a crucial signaling molecule involved in numerous cellular pathways. Beyond its role as a messenger or modulator in intracellular cascades, calcium's function in excitable cells, including nerve impulse transmission, is remarkable. The central role of calcium in nervous activity has driven the rapid development of fluorescent techniques for monitoring this cation in living cells. Specifically, genetically encoded calcium indicators (GECIs) are the most in-demand molecular tools in their class. In this work, we address two issues of calcium imaging by designing indicators based on the successful GCaMP6 backbone and the fluorescent protein BrUSLEE. The first indicator variant (GCaMP6s-BrUS), with a reduced, calcium-insensitive fluorescence lifetime, has potential in monitoring calcium dynamics with a high temporal resolution in combination with advanced microscopy techniques, such as light beads microscopy, where the fluorescence lifetime limits acquisition speed. Conversely, the second variant (GCaMP6s-BrUS-145), with a flexible, calcium-sensitive fluorescence lifetime, is relevant for static measurements, particularly for determining absolute calcium concentration values using fluorescence lifetime imaging microscopy (FLIM). To identify the structural determinants of calcium sensitivity in these indicator variants, we determine their spatial structures. A comparative structural analysis allowed the optimization of the GCaMP6s-BrUS construct, resulting in an indicator variant combining calcium-sensitive behavior in the time domain and enhanced molecular brightness. Our data may serve as a starting point for further engineering efforts towards improved GECI variants with fine-tuned fluorescence lifetimes.Article Citation - WoS: 5Citation - Scopus: 4Polarity Induced Vapochromism and Vapoluminescence of Polythiophene Derivatives for Volatile Organic Compounds Classification(Elsevier, 2023) Karabacak, Soner; Qun, David Lee Chao; Ammanath, Gopal; Yeasmin, Sanjida; Yağmurcukardeş, Mehmet; Palaniappan, Alagappan; Liedberg, Bo; Yıldız, Ümit HakanPolarity induced vapochromic and vapoluminescent properties of cationic poly-3-alkoxythiophene derivatives (PT) casted on polyvinylidene fluoride (PVDF) membranes are reported. PT with six different pendant groups are designed to differentially interact with volatile organic compounds (VOC) of varying polarities, thereby enabling their classification. PT exhibit a rapid vapochromic response with a concurrent modulation of vapoluminescence due to the non-covalent cation-? interactions between the pendant groups and the PT backbone. Adsorption of VOC on pendant groups alters the conformation of PT backbone, thus resulting in an increase in intensity and blue shifting of fluorescence emission within the visible spectrum. The vapoluminescent responses are found to be more sensitive with a limit of detection (LOD) of ?7 ppm and a wider dynamic range as compared to the vapochromic responses with a LOD of ?60 ppm for the detection of a model VOC: chloroform. Notably, all the PT illustrate an instantaneous recovery of colour and luminescence upon desorption of VOC. PT interaction with VOC of varying polarities was ascertained using density functional theory (DFT) and principal component analysis (PCA) methodologies. In summary, the polarity induced vapochromic and vapoluminescent properties of PT could yield a selective and sensitive vapochromic and fluorometric dual-mode VOC detection platform. © 2023Article Citation - WoS: 1Citation - Scopus: 1A Multi-Layered Graphene Based Gas Sensor Platform for Discrimination of Volatile Organic Compounds Via Differential Intercalation(Royal Society of Chemistry, 2023) Özkendir İnanç, Dilce; Ng, Zhi Kai; Başkurt, Mehmet; Keleş, Berfin; Vardar, Gökay; Şahin, Hasan; Tsang, Siu Hon; Palaniappan, Alagappan; Yıldız, Ümit Hakan; Teo, EhtSelective and sensitive detection of volatile organic compounds (VOCs) is of critical importance for environmental monitoring, disease diagnosis and industrial applications. Among VOCs, assay development for primary alcohols has captured significant research attention since their toxicity causes adverse effects on gastrointestinal and central nerve systems, resulting in irreversible blindness, and coma, and can be even fatal at high exposure levels. However, selective detection of primary alcohols is extremely challenging owing to the similarity in their molecular structure and characteristic groups. Herein, we have attempted to investigate the differential methanol (MeOH)-ethanol (EtOH) discriminative properties of single-layer, bi-layer, and multi-layer graphene morphologies. Chemiresistors fabricated using the three morphologies of graphene illustrate discriminative MeOH-EtOH responses, which is attributed to the phenomenon of differential intercalation of MeOH within layered graphene morphologies as compared to that of EtOH. This hypothesis is verified by density functional theory calculations, which revealed that the adsorption of EtOH molecules on the graphene surface is more energetically favorable as compared to that of MeOH molecules, thereby inhibiting their intercalation within the layered graphene morphologies. It is further evaluated that the degree of MeOH intercalation increases with increasing layers of graphene for obtaining differential MeOH-EtOH responses. Experimental results suggest possibilities to develop selective and sensitive MeOH assays fabricated using various graphene morphologies in a combinatorial sensor array format.Article Citation - WoS: 6Citation - Scopus: 6Ion and Molecule Sieving Through Highly Stable Graphene-Based Laminar Membranes(Amer Chemical Soc, 2023) Yuan, Gang; Jiang, Yu; Wang, Xiao; Ma, Jiaojiao; Ma, Hao; Wang, Xiang; Hu, ShengBiological ion channels use both their sizes and residual groups to reject large ions and molecules and allow highly selective permeation of small species with similar sizes. To realize these properties in artificial membranes, the main challenge is the precise control of both the channel size and the interior at the nanoscale. Here we report the permeation of ions and molecules through interlayer channels in graphene-based laminar membranes. The amino groups decorated on channel walls are found to form hydrogen bond networks with intercalated water molecules, thus providing a highly stable laminate structure and a controlled channel size. Solutes with hydration diameters of >10 angstrom are precisely sieved out. Small species permeate through with selectivities of up to a few thousand, governed by their distinct electrical interactions with channels depending on the atomistic distance from the charged species to the channel walls. Our work offers important insights into manipulating channel structures for enhanced separation performance at the nanoscale.Article Citation - WoS: 6Citation - Scopus: 6Polar Solvent-Free Room Temperature Synthesis of Cspbx3 (x = Br, Cl) Perovskite Nanocubes(Royal Society of Chemistry, 2023) Güvenç, Çetin Meriç; Kocabaş, Aşkın; Balcı, SinanConventionally, colloidal lead halide perovskite nanocubes have been synthesized by the hot-injection or ligand-assisted reprecipitation (LARP) methods. We herein demonstrate a polar solvent-free room temperature method for the synthesis of CsPbX3 (X = Br, Cl) nanocubes. In addition to the commonly used ligand pair of oleylamine and oleic acid, guanidinium (GA) has been used to passivate the surface of the nanocrystals. Our study demonstrates that GA inhibits the formation of low dimensional structures such as nanowires and nanoplatelets and further supports the formation of perovskite nanocubes. In fact, GA diminishes the restricted monomer-addition effect of long-chain oleylammonium (OLAM) ions to the nanocrystal. We show that above a critical GA/OLAM molar ratio, the synthesis yields homogeneous CsPbX3 (X = Br, Cl) nanocubes. Importantly, we observe the nucleation and growth kinetics of the GA-assisted CsPbBr3 nanocube formation by using in situ absorption and photoluminescence (PL) measurements. Small nanocrystals with an excitonic absorption peak at around 435 nm and photoluminescence (PL) maxima at 447 nm were nucleated and continuously shifted to longer wavelengths during the growth period. Crucially, our method allows the synthesis of CsPbCl3 nanocubes at room temperature without using polar organic solvents. The synthesized CsPbBr3, CsPb(Cl0.5Br0.5)3, and CsPbCl3 nanocubes have PL peaks at 508 nm, 443 nm, and 405 nm, photoluminescence quantum yields (PLQY) of 85%, 58% and 5%, and lifetimes of 18.98 ns, 18.97 ns, and 14.74 ns, respectively.Article Citation - WoS: 8Citation - Scopus: 9Tuning the Colour of Solution Processed Perylene Tetraester Based Oleds From Yellowish-Green To Greenish-White: a Molecular Engineering Approach(Elsevier, 2023) Aksoy, Erkan; Bozkuş, Volkan; Varlıklı, CananThree regioisomericaly pure 1,7-di-ethynyl bridged perylene-3,4,9,10-tetracarboxy tetrabutylesters functionalized with triisopropylsilyl-ethynylen (PTE1), phenyl-ethynylen (PTE2) and tetraphenylsilyl-ethynylen (PTE3) groups were synthesized. Photophysical, thermal, electrochemical, and solution processed electroluminescence (EL) behaviours were investigated in comparison with a basic perylene-3,4,9,10-tetracarboxy tetrabutylester (PTEref) structure. Stepwise π conjugation, allowed tuning the absorption and photoluminescence wavelengths of the PTEs without disturbing the photo, thermal and electrochemical stabilities; ≫10h, >250 °C, and >50 cycles, respectively. Electron mobility of PTE2 is measured to be more than 10-fold of the other PTE derivatives. Individual utilization of PTE derivatives as solid-state emitters in poly(N-vinylcarbazole) (PVK): 2-(4-Biphenylyl)-5-phenyl-1,3,4-oxadiazole (PBD) host matrix produced yellowish-green EL. Benefiting from higher electron mobiliy, PTE2 emitter presented the best device efficiency values with an EL maximum of 535 nm. Whereas dual doping of the synthesized PTEs with PTEref resulted in greenish-white light with increased stability. Although the emitting layer contained no red emitting component, optimization of the dual doping ratio of PTEref:PTE3 produced a colour rendering index value of 76 with Commission Internationale d'Eclairage coordinates of (0.29, 0.37).Article Citation - WoS: 13Citation - Scopus: 14Synthesis of Albumin Nanoparticles in a Water-Miscible Ionic Liquid System, and Their Applications for Chlorambucil Delivery To Cancer Cells(Elsevier, 2022) Akdoğan, Yaşar; Sözer, Sümeyra Çiğdem; Akyol, Cansu; Başol, Merve; Karakoyun, Çiğdem; Çakan Akdoğan, GülçinSerum albumin has been a preferred protein to generate biodegradable and non-toxic nanoparticles (NPs) for drug delivery applications. Different methods applied for the preparation of serum albumin NPs mostly used organic solvents. Here, we prepared serum albumin NPs in an ionic liquid (IL) system. ILs are considered to be green and designer solvents with unique properties that can replace organic solvents in the synthesis of albumin NPs. Bovine serum albumin (BSA) proteins dissolved in water were transformed into BSA NPs in a water/ Triton™X (TX-100), 1-butanol/1-butyl-3-methylimidazolium trifluoromethanesulfonate (BmimCF3SO3) microemulsion-like system by using a high-speed homogenizer and crosslinker glutaraldehyde. The obtained BSA NPs have been used in drug loading and release studies with a hydrophobic anticancer drug chlorambucil (Chl). Drug loading increased as increasing the ratio of Chl incubated with BSA NPs. Monitoring the drug release by UV–Vis spectroscopy revealed a burst release at first 4 h, but two-thirds of drugs stayed with NPs upon diffusion method. On the other hand, cellular uptake of Chl loaded BSA NPs caused a significant MCF7 breast cancer cell death, whereas free Chl and unloaded BSA NPs did not have a significant effect on the cell viability. Furthermore, in vivo toxicity assessment of BSA NPs obtained in the IL system was conducted in the zebrafish animal model. It showed that zebrafish body is able to eliminate BSA NPs without any toxic side effects and encapsulation of Chl into NPs reduced the toxicity of free Chl. In summary, we showed that BSA NPs with size smaller than 200 nm could be prepared in BmimCF3SO3 mediated system. They can be used for Chl loading (up to 6.9 wt%) with a sustainable release and they induce significant cell death in Chl sensitive cancer cells up to 45% in 24 h. These results indicate that BSA NPs could be prepared alternatively in IL systems and used in drug delivery studies.Article Citation - WoS: 32Citation - Scopus: 31Wien Effect in Interfacial Water Dissociation Through Proton-Permeable Graphene Electrodes(Nature Research, 2022) Cai, Junhao; Griffin, Eoin; Guarochico-Moreira, Victor H.; Barry, D.; Xin, B.; Yağmurcukardeş, Mehmet; Zhang, Sheng; Geim, Andre K.; Peeters, François M.; Lozada-Hidalgo, MarceloStrong electric fields can accelerate molecular dissociation reactions. The phenomenon known as the Wien effect was previously observed using high-voltage electrolysis cells that produced fields of about 107 V m−1, sufficient to accelerate the dissociation of weakly bound molecules (e.g., organics and weak electrolytes). The observation of the Wien effect for the common case of water dissociation (H2O ⇆ H+ + OH−) has remained elusive. Here we study the dissociation of interfacial water adjacent to proton-permeable graphene electrodes and observe strong acceleration of the reaction in fields reaching above 108 V m−1. The use of graphene electrodes allows measuring the proton currents arising exclusively from the dissociation of interfacial water, while the electric field driving the reaction is monitored through the carrier density induced in graphene by the same field. The observed exponential increase in proton currents is in quantitative agreement with Onsager’s theory. Our results also demonstrate that graphene electrodes can be valuable for the investigation of various interfacial phenomena involving proton transport.Article Citation - WoS: 40Citation - Scopus: 38Anisotropic and Outstanding Mechanical, Thermal Conduction, Optical, and Piezoelectric Responses in a Novel Semiconducting Bcn Monolayer Confirmed by First-Principles and Machine Learning(Elsevier, 2022) Mortazavi, Bohayra; Fazel Shojaei; Yağmurcukardeş, Mehmet; Alexander Shapeev; Xiaoying ZhuangGraphene-like nanomembranes made of the neighboring elements of boron, carbon and nitrogen elements, are well-known of showing outstanding physical properties. Herein, with the aid of density functional theory (DFT) calculations, various atomic configurations of the graphene-like BCN nanosheets are investigated. DFT results reveal that depending on the atomic arrangement, the BCN monolayers may display semimetallic Dirac cone or semiconducting electronic nature. BCN nanosheets are also found to exhibit high piezoelectricity and carrier mobilities with considerable in-plane anisotropy, depending on the atomic arrangement. For the predicted most stable BCN monolayer, thermal and mechanical properties are explored using machine learning interatomic potentials. The room temperature tensile strength and lattice thermal conductivity of the most stable BCN monolayer are estimated to be orientation-dependent and remarkably high, over 78 GPa and 290 W/m.K, respectively. In addition, the thermal expansion coefficient of the monolayer BCN at room temperature is estimated to be −3.2 × 10−6 K−1, which is close to that of the graphene. The piezoelectric response of the herein proposed BCN lattice is also predicted to be close to that of the h-BN monolayer. Presented results highlight outstanding physics of the BCN nanosheets.