WoS İndeksli Yayınlar Koleksiyonu
Permanent URI for this collectionhttps://hdl.handle.net/20.500.12573/394
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Article Citation - WoS: 8Citation - Scopus: 8Writing Chemical Patterns Using Electrospun Fibers as Nanoscale Inkpots for Directed Assembly of Colloidal Nanocrystals(Royal Soc Chemistry, 2020) Kiremitler, N. Burak; Torun, Ilker; Altintas, Yemliha; Patarroyo, Javier; Demir, Hilmi Volkan; Puntes, Victor F.; Onses, M. SerdarApplications that range from electronics to biotechnology will greatly benefit from low-cost, scalable and multiplex fabrication of spatially defined arrays of colloidal inorganic nanocrystals. In this work, we present a novel additive patterning approach based on the use of electrospun nanofibers (NFs) as inkpots for end-functional polymers. The localized grafting of end-functional polymers from spatially defined nanofibers results in covalently bound chemical patterns. The main factors that determine the width of the nanopatterns are the diameter of the NF and the extent of spreading during the thermal annealing process. Lowering the surface energy of the substrates via silanization and a proper choice of the grafting conditions enable the fabrication of nanoscale patterns over centimeter length scales. The fabricated patterns of end-grafted polymers serve as the templates for spatially defined assembly of colloidal metal and metal oxide nanocrystals of varying sizes (15 to 100 nm), shapes (spherical, cube, rod), and compositions (Au, Ag, Pt, TiO2), as well as semiconductor quantum dots, including the assembly of semiconductor nanoplatelets.Article Citation - WoS: 54Citation - Scopus: 57Ultralow Bandgap Molecular Semiconductors for Ambient-Stable and Solution-Processable Ambipolar Organic Field-Effect Transistors and Inverters(Royal Soc Chemistry, 2017) Ozdemir, Resul; Choi, Donghee; Ozdemir, Mehmet; Kwon, Guhyun; Kim, Hyekyoung; Sen, Unal; Usta, HakanThe design and development of novel ambipolar semiconductors is very crucial to advance various optoelectronic technologies including organic complementary (CMOS) integrated circuits. Although numerous high-performance ambipolar polymers have been realized to date, small molecules have been unable to provide high ambipolar performance in combination with ambient-stability and solution-processibility. In this study, by implementing highly p-electron deficient, ladder-type IFDK/IFDM acceptor cores with bithiophene donor units in D-A-D pi-architectures, two novel small molecules, 2OD-TTIFDK and 2OD-TTIFDM, were designed, synthesized and characterized in order to achieve ultralow band-gap (1.21-1.65 eV) semiconductors with sufficiently balanced molecular energetics for ambipolarity. The HOMO/LUMO energies of the new semiconductors are found to be -5.47/-3.61 and -5.49/-4.23 eV, respectively. Bottom-gate/top-contact OFETs fabricated via solution-shearing of 2OD-TTIFDM yield perfectly ambient stable ambipolar devices with reasonably balanced electron and hole mobilities of 0.13 cm(2) V-1 s(-1) and 0.01 cm(2) V-1 s(-1), respectively with I-on/I-off ratios of similar to 10(3)-10(4), and 2OD-TTIFDK-based OFETs exhibit ambipolarity under vacuum with highly balanced (mu(e)/mu(h) similar to 2) electron and hole mobilities of 0.02 cm(2) V-1 s(-1) and 0.01 cm(2) V-1 s(-1), respectively with I-on/I-off ratios of similar to 10(5)-10(6). Furthermore, complementary-like inverter circuits were demonstrated with the current ambipolar semiconductors resulting in high voltage gains of up to 80. Our findings clearly indicate that ambient-stability of ambipolar semiconductors is a function of molecular orbital energetics without being directly related to a bulk p-backbone structure. To the best of our knowledge, considering the processing, charge-transport and inverter characteristics, the current semiconductors stand out among the best performing ambipolar small molecules in the OFET and CMOS-like circuit literature. Our results provide an efficient approach in designing ultralow band-gap ambipolar small molecules with good solution-processibility and ambient-stability for various optoelectronic technologies, including CMOS-like integrated circuits.Article Citation - WoS: 25Citation - Scopus: 25Triisopropylsilylethynyl-Substituted Indenofluorenes: Carbonyl Versus Dicyanovinylene Functionalization in One-Dimensional Molecular Crystals and Solution-Processed N-Channel Ofets(Royal Soc Chemistry, 2018) Ozdemir, Resul; Park, Sangyun; Deneme, Ibrahim; Park, Yonghan; Zorlu, Yunus; Alidagi, Husniye Ardic; Usta, HakanThe design and synthesis of novel electron-deficient and solution-processable polycyclic aromatic hydrocarbons offers great opportunities for the development of low-cost and large-area (opto)electronics. Although (trialkylsilyl)ethynyl (R3Si-C?C-) has emerged as a very popular unit to solubilize organic semiconductors, it has been applied only to a limited class of materials that are mostly substituted on short molecular axes. Herein, two novel solution-processable indenofluorene-based semiconductors, TIPS-IFDK and TIPS-IFDM, bearing (triisopropylsilyl)ethynyl end units at 2,8-positions (long molecular axis substitution) were synthesized, and their single-crystal structures, optoelectronic properties, solution-sheared thin-film morphologies/microstructures, and n-channel field-effect responses were studied. In accordance with the DFT calculations, the HOMO/LUMO energies of the new compounds are found to be -5.77/-3.65 eV and -5.84/-4.18 eV for TIPS-IFDK and TIPS-IFDM, respectively, reflecting the high electron deficiency of the new -backbones. Both semiconductors exhibit slightly S-shaped molecular frameworks with highly coplanar IFDK/IFDM -cores, and they form slipped -stacked one-dimensional (1-D) columnar motifs in the solid state. However, substantial differences in the degree of - interactions and stacking distances (4.04 angstrom vs. 3.47 angstrom) were observed between TIPS-IFDK and TIPS-IFDM as a result of carbonyl vs. dicyanovinylene functionalization, which results in a three orders of magnitude variation in the charge carrier mobility of the corresponding thin films. Top-contact/bottom-gate OFETs fabricated via solution-shearing TIPS-IFDM yielded one of the best performances in the (trialkylsilyl)ethynyl literature ((e) = 0.02 cm(2) V-1 s(-1), I-on/I-off = 10(7)-10(8), and V-T approximate to 2 V under ambient atmosphere) for a 1-D polycrystalline semiconductor microstructure. To the best of our knowledge, the molecules presented here are the first examples of n-type semiconductors substituted with (trialkylsilyl)ethynyl groups on their long molecular axes.Article Citation - WoS: 16Citation - Scopus: 16The Hansen Solubility Approach Towards Green Solvent Processing: N-Channel Organic Field-Effect Transistors Under Ambient Conditions(Royal Soc Chemistry, 2024) Deneme, Ibrahim; Yildiz, Tevhide Ayca; Kayaci, Nilgun; Usta, HakanThe adoption of green solvents is of utmost importance for the solution-based fabrication of semiconductor thin films and for the commercialization of (opto)electronic devices, especially in response to evolving regulatory mandates for handling organic materials. Despite the increasing interest in this area, the scarcity of green solvent-processed n-channel OFETs, especially functioning under ambient conditions, highlights the need for further research. In this study, we demonstrated the Hansen solubility approach to study the solubility behavior of an ambient-stable n-type semiconductor, 2,2' -(2,8-bis(3-dodecylthiophen-2-yl)indeno[1,2-b]fluorene-6,12-diylidene)dimalononitrile (beta,beta'-C-12-TIFDMT), and to analyze potential green solvents for thin-film processing. The Hansen solubility parameters were determined to be delta(D) = 20.8 MPa1/2, delta(P) = 5.8 MPa1/2, and delta(H) = 5.5 MPa1/2 with a radius (R-0) of 8.3 MPa1/2. A green solvent screening analysis based on the minimal distance constraint and quantitative sustainability score identified ethoxybenzene, anisole, 2-methylanisole, and 2-methyltetrahydrofuran as suitable green solvents (R-a's = 5.17-7.93 MPa1/2 < R-0). A strong thermodynamic correlation was identified between the solubility and the semiconductor-solvent distance in the 3D Hansen solubility space, in which the maximum solubility limit could be estimated with the enthalpy of fusion (Delta H-fus) and melting temperature (T-mp) of the semiconductor. To the best of our knowledge, this relationship between the maximum solubility limit and thermal properties has been established for the first time for organic semiconductors. Bottom-gate/top-contact OFETs fabricated by spin-coating the semiconductor green solutions exhibited mu es reaching similar to 0.2 cm(2) V-1 s(-1) (I-on/I-off similar to 10(6)-10(7) and V-on similar to 0-5 V) under ambient conditions. This device performance, to our knowledge, is the highest reported for an ambient-stable green solvent-processed n-channel OFET. Our HSP-based rational approach and unique findings presented in this study can shed critical light on how green solvents can be efficiently incorporated in solution processing in organic (opto)electronics, and whether ambient-stable n-type semiconductors can continue to play an important role in green OFETs.Article Citation - WoS: 22Citation - Scopus: 24The Design and Fabrication of Supramolecular Semiconductor Nanowires Formed by Benzothienobenzothiophene (BTBT)-Conjugated Peptides(Royal Soc Chemistry, 2018) Khalily, Mohammad Aref; Usta, Hakan; Ozdemir, Mehmet; Bakan, Gokhan; Dikecoglu, F. Begum; Edwards-Gayle, Charlotte; Guler, Mustafa O.pi-Conjugated small molecules based on a [1]benzothieno[3,2-b]benzothiophene (BTBT) unit are of great research interest in the development of solution-processable semiconducting materials owing to their excellent charge-transport characteristics. However, the BTBT -core has yet to be demonstrated in the form of electro-active one-dimensional (1D) nanowires that are self-assembled in aqueous media for potential use in bioelectronics and tissue engineering. Here we report the design, synthesis, and self-assembly of benzothienobenzothiophene (BTBT)-peptide conjugates, the BTBT-peptide (BTBT-C-3-COHN-Ahx-VVAGKK-Am) and the C-8-BTBT-peptide (C-8-BTBT-C-3-COHN-Ahx-VVAGKK-Am), as -sheet forming amphiphilic molecules, which self-assemble into highly uniform nanofibers in water with diameters of 11-13(+/- 1) nm and micron-size lengths. Spectroscopic characterization studies demonstrate the J-type - interactions among the BTBT molecules within the hydrophobic core of the self-assembled nanofibers yielding an electrical conductivity as high as 6.0 x 10(-6) S cm(-1). The BTBT -core is demonstrated, for the first time, in the formation of self-assembled peptide 1D nanostructures in aqueous media for potential use in tissue engineering, bioelectronics and (opto)electronics. The conductivity achieved here is one of the highest reported to date in a non-doped state.Article Citation - WoS: 28Citation - Scopus: 29Symmetric Naphthalenediimidequaterthiophenes for Electropolymerized Electrochromic Thin Films(Royal Soc Chemistry, 2015) Figa, V.; Chiappara, C.; Ferrante, F.; Casaletto, M. P.; Principato, F.; Cataldo, S.; Pignataro, B.A new symmetric naphthalenediimidequaterthiophene (s-NDI2ODT4) was synthesized and exhibited the capability to electropolymerize alone or with EDOT affording polymers with controlled donor/acceptor monomer ratios. s-NDI2ODT4-EDOT-based copolymers showed low band gaps, wide optical absorption ranges extending to the near IR region, tuned electrical properties, thin-film surface morphology and hydrophilicity as well as high coloration efficiency in electrochromic devices.Article Citation - WoS: 16Citation - Scopus: 17Organic and Inorganic Semiconducting Materials-Based SERS: Recent Developments and Future Prospects(Royal Soc Chemistry, 2024) Ozdemir, Resul; Ozkan Hukum, Kubra; Usta, Hakan; Demirel, GokhanSurface-enhanced Raman spectroscopy (SERS) with high sensitivity/selectivity is a powerful analytical tool and has been widely used, particularly in the fields of chemistry, spectroscopy, molecular detection, food safety, anti-counterfeiting, and environmental monitoring. Conventional SERS detection relies on plasmonic materials (e.g., Au and Ag nanostructures) with exceedingly high enhancement factors up to 1012. However, these substrates encounter significant limitations, including poor reproducibility, high cost, lack of selectivity, limited SERS active area leading to inconsistent field enhancement and SERS signals, and the possibility of the photothermal decomposition of the analyte species. These drawbacks have the potential to impede detection accuracy and hinder large-scale practical applications. This review focuses on alternative approaches based on noble metal-free SERS substrates. Considering recent advancements in the field of SERS active platforms, we first introduce the implementation of inorganic compounds, including metal oxides, transition metal sulfides/-selenides/-tellurides, 2-D layered transition metal carbides and nitrides (Mxenes), metal-organic frameworks (MOFs), and single elemental inorganic materials for Raman signal enhancement applications. In the second part of the review, we highlight the fast-growing field of SERS-active organic platforms. Moreover, we discuss the promises and challenges for the future direction of organic and inorganic material-based SERS. Surface-enhanced Raman spectroscopy (SERS) is a powerful analytical tool and has been widely used, in different fields including molecular detection, food safety, anti-counterfeiting, and environmental monitoring.Article Citation - WoS: 16Citation - Scopus: 19On-Demand Weighing of Single Dry Biological Particles Over a 5-Order Dynamic Range(Royal Soc Chemistry, 2014) Chan, Bin-Da; Icoz, Kutay; Huang, Wanfeng; Chang, Chun-Li; Savran, Cagri A.We report a simple and highly versatile system to select and weigh individual dry biological particles. The system is composed of a microtweezer to pick and place individual particles and a cantilever-based resonator to weigh them. The system can weigh entities that vary from a red blood cell (similar to 10(-11) g) to the eye-brain complex of an insect (similar to 10(-6) g), covering a 5-order-of-magnitude mass range. Due to its versatility and ease of use, this weighing method is highly compatible with established laboratory practices. The system can provide complementary mass information for a wide variety of individual particles imaged using scanning electron microscopy and determine comparative weights of individual biological entities that are attached to microparticles as well as weigh fractions of individual biological entities that have been subjected to focused ion beam milling.Article Citation - WoS: 7Citation - Scopus: 8Microstructural Modulation of Organic Passivation Layers for Metal Oxide Semiconductors to Achieve High Bias Stability(Royal Soc Chemistry, 2020) Ho, Dongil; Jeong, Ha-Yun; Minh Nhut Le; Usta, Hakan; Kwon, Hyuck-In; Kim, Myung-Gil; Kim, Choongik; Le, Minh NhutElectrical properties of metal oxide thin-film transistors (TFTs) are tunedviathe microstructural control of organic back-channel passivation layers. In this study, organic semiconductor (OSC) passivation layers with various molecular and physicochemical properties are employed to identify the back-channel passivation mechanism in solution-processed amorphous indium gallium zinc oxide (a-IGZO) TFTs. The OSC microstructure influences the passivation of electrical defects ina-IGZO TFTs by compensating for acceptor-like trap states and dangling bonds in the back-channel. First, the distance between an n-type OSC (C-60) and thea-IGZO back-channel is controlled by employing phosphonic acid molecules with different carbon chain lengths. Positive bias stress stability is tuned by applying both the OSC and carbon chain effect, leading to stable, high-performance TFTs with the determination of subgap density of states to confirm the compensation effects on the total acceptor-like defect states. The n-doping of identical passivation layers is further investigated by using perylenedicarboximide derivatives to confirm the proposed n-doping mechanism. Finally, the semiconductor 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene is selected on the basis of our proposed passivation model and exhibited good passivation characteristics. This study demonstrates an ideal molecular design for organic passivation layers, which shows significant potential for the realization of stable, high-performance TFTs.Article Citation - WoS: 25Citation - Scopus: 25Indenofluorenes for Organic Optoelectronics: the Dance of Fused Five- and Six-Membered Rings Enabling Structural Versatility(Royal Soc Chemistry, 2022) Can, Ayse; Facchetti, Antonio; Usta, HakanPolycyclic pi-conjugated hydrocarbons (PCHs), either unfunctionalized or structurally modified derivatives, have attracted tremendous interest in the past few decades as high-performance semiconductors for use in new generations of organic (opto)electronic devices. Among several PCHs realized to date, the 6-5-6-5-6 pi-fused-ring backbone of indenofluorene (IF) stands out as a unique semiconducting architecture with great structural and property versatility affording six different regioisomers, diverse functionalization/substitution positions, pi-conjugation/delocalization patterns, aromatic behaviors, and electronic structures. In this review, we summarize and analyze the historical and recent advances in the design and implementation of IF-based semiconductors in organic transistor and solar cell devices, as well as in understanding the chemical structure-molecular property-semiconductivity relationships. Following an introduction to the fascinating properties of an IF pi-framework that distinguishes this core among PCHs, we present IF-based semiconductors and discuss their properties by classifying them into four main families (IF-diones, IF-DCVs/IF-TTFs, pi-IFs, and (un)substituted DH-IFs) considering whether methylene or methine C-bridges are present and how these positions are functionalized or substituted. For each family, design and synthetic approaches, molecular properties, and transistor/solar cell device applicability and/or performance are reviewed and discussed. At the end, we conclude with a section discussing the challenges and opportunities for future progress of IF-based semiconductor materials and related (opto)electronic technologies.