WoS İndeksli Yayınlar Koleksiyonu
Permanent URI for this collectionhttps://hdl.handle.net/20.500.12573/394
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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: 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: 53Citation - Scopus: 59Thickness-Tunable Self-Assembled Colloidal Nanoplatelet Films Enable Ultrathin Optical Gain Media(Amer Chemical Soc, 2020-07-31) Erdem, Onur; Foroutan, Sina; Gheshlaghi, Negar; Guzelturk, Burak; Altintas, Yemliha; Demir, Hilmi VolkanWe propose and demonstrate construction of highly uniform, multilayered superstructures of CdSe/CdZnS core/shell colloidal nanoplatelets (NPLs) using liquid interface self-assembly. These NPLs are sequentially deposited onto a solid substrate into slabs having monolayer-precise thickness across tens of cm(2) areas. Because of near-unity surface coverage and excellent uniformity, amplified spontaneous emission (ASE) is observed from an uncharacteristically thin film having 6 NPL layers, corresponding to a mere 42 nm thickness. Furthermore, systematic studies on optical gain of these NPL superstructures having thicknesses ranging from 6 to 15 layers revealed the gradual reduction in gain threshold with increasing number of layers, along with a continuous spectral shift of the ASE peak (similar to 18 nm). These observations can be explained by the change in the optical mode confinement factor with the NPL waveguide thickness and propagation wavelength. This bottom-up construction technique for thickness-tunable, three-dimensional NPL superstructures can be used for large-area device fabrication.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: 37Citation - Scopus: 39Spectrally Wide-Range Efficient, and Bright Colloidal Light-Emitting Diodes of Quasi-2D Nanoplatelets Enabled by Engineered Alloyed Heterostructures(Amer Chemical Soc, 2020-08-25) Altintas, Yemliha; Liu, Baiquan; Hernandez-Martinez, Pedro Ludwig; Gheshlaghi, Negar; Shabani, Farzan; Sharma, Manoj; Demir, Hilmi VolkanRecently, there has been tremendous interest in the synthesis and optoelectronic applications of quasi-two-dimensional colloidal nanoplatelets (NPLs). Thanks to the ultranarrow emission linewidth, high-extinction coefficient, and high photostability, NPLs offer an exciting opportunity for high-performance optoelectronics. However, until now, the applications of these NPLs are limited to available discrete emission ranges, limiting the full potential of these exotic materials as efficient light emitters. Here, we introduce a detailed systematic study on the synthesis of NPLs based on the alloying mechanisms in core/shell, core/alloyed shell, alloyed core/shell, and alloyed core/alloyed shell heterostructures. Through the engineering of the band gap supported by the theoretical calculations, we carefully designed and successfully synthesized the NPL emitters with continuously tunable emission. Unlike conventional NPLs showing discrete emission, here, we present highly efficient core/shell NPLs with fine spectral tunability from green to deep-red spectra. As an important demonstration of these efficient emitters, the first-time implementation of yellow NPL light-emitting diodes (LEDs) has been reported with record device performance, including the current efficiency surpassing 18.2 cd A(-1), power efficiency reaching 14.8 lm W-1, and record luminance exceeding 46 900 cd m(-2). This fine and wide-range color tunability in the visible range from stable and efficient core/shell NPLs is expected to be extremely important for the optoelectronic applications of the family of colloidal NPL emitters.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: 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: 54Citation - Scopus: 58Proton Conducting Self-Assembled Metal-Organic Framework/Polyelectrolyte Hollow Hybrid Nanostructures(Amer Chemical Soc, 2016-08-29) Sen, Unal; Erkartal, Mustafa; Kung, Chung-Wei; Ramani, Vijay; Hupp, Joseph T.; Farha, Omar K.Herein, a room temperature chemical process to synthesize functional, hollow nanostructures from zeolitic imidazolate framework-8 (ZIF-8) and poly(vinylphosphonic acid) (PVPA) is reported. Syntheses are initiated by physically blending the components a process that is accompanied first by encapsulation of ZIF-8 crystallites by PVPA and then by fragmentation of the crystallites. The fragmentation process is driven by partial displacement of the methyl-imidazolate ligands of Zn(II) in ZIF-8 by phosphonate groups on PVPA. Differences in rates of diffusion for the components of the reactive mixture yield a Kirkendall-like effect that is expressed as a hollow-particle morphology. The obtained hollow nanostructures feature hybrid shells containing PVPA, ZIF-8, and their cross-reacted products. The hybrid structures display substantial proton conductivities that increase with increasing temperature, even under the anhydrous conditions prevailing at temperatures above the boiling point of water. For example, at T = 413 K the proton conductivity of ZIF-8@PVPA reaches 3.2 (+/- 0.12) x 10(-3) S cm(-1), a value comparatively higher than that for PVPA (or ZIF-8) in isolation. The high value may reflect the availability in the hybrid structures of free (and partially free), amphoteric imidazole species, and their hydrogen-bonding interactions with phosphonate and/or phosphonic acid units. The persistence of ample conductivity at high temperature reflects the elimination of phosphonic acid group dehydration and dimerization-an effect that strikingly degrades the conductivity of pure PVPA under anhydrous conditions.Article Citation - WoS: 75Citation - Scopus: 74Perfluoroalkyl-Functionalized Thiazole Thiophene Oligomers as N-Channel Semiconductors in Organic Field-Effect and Light-Emitting Transistors(Amer Chemical Soc, 2014-11-04) Usta, Hakan; Sheets, William Christopher; Denti, Mitchell; Generali, Gianluca; Capelli, Raffaella; Lu, Shaofeng; Facchetti, AntonioDespite their favorable electronic and structural properties, the synthetic development and incorporation of thiazole-based building blocks into n-type semiconductors has lagged behind that of other pi-deficient building blocks. Since thiazole insertion into pi-conjugated systems is synthetically more demanding, continuous research efforts are essential to underscore their properties in electron-transporting devices. Here, we report the design, synthesis, and characterization of a new series of thiazolethiophene tetra- (1 and 2) and hexa-heteroaryl (3 and 4) co-oligomers, varied by core extension and regiochemistry, which are end-functionalized with electron-withdrawing perfluorohexyl substituents. These new semiconductors are found to exhibit excellent n-channel OFET transport with electron mobilities (mu(e)) as high as 1.30 cm(2)/(V center dot s) (I-on/I-off > 10(6)) for films of 2 deposited at room temperature. In contrary to previous studies, we show here that 2,2'-bithiazole can be a very practical building block for high-performance n-channel semiconductors. Additionally, upon 2,2'- and 5,5'-bithiazole insertion into a sexithiophene backbone of well-known DFH-6T, significant charge transport improvements (from 0.0010.021 cm(2)/(V center dot s) to 0.200.70 cm(2)/(V center dot s)) were observed for 3 and 4. Analysis of the thin-film morphological and microstructural characteristics, in combination with the physicochemical properties, explains the observed high mobilities for the present semiconductors. Finally, we demonstrate for the first time implementation of a thiazole semiconductor (2) into a trilayer light-emitting transistor (OLET) enabling green light emission. Our results show that thiazole is a promising building block for efficient electron transport in ?-conjugated semiconductor thin-films, and it should be studied more in future optoelectronic applications.
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