The syntheses of copper and silver delafossite-type oxides from their constituent binary metal oxides, oxide hydroxides and hydroxides, by low temperature (<210°C) and low pressure (<20 atm) hydrothermal reactions are described. Particular emphasis is placed on how the acid-base character of a constituent oxide determines its solubility and therefore whether a particular delafossite-type oxide can be synthesized, a strategy utilized by geologists and mineralogists to understand the conditions necessary for the synthesis of various minerals. Thus, the geochemical and corrosion science literature are shown to be useful in understanding the reaction conditions required for the syntheses of delafossite-type oxides and the relationship between reactant metal oxide acid-base character, solubility, aqueous speciation, and product formation. Manipulation of the key parameters, temperature, pressure, pH, and reactant solubility, results in broad families of phase-pure delafossite-type oxides in moderate to high yields for copper, CuBO 2 (B
Epitaxial La 2 NiMnO 6 thin films have been grown on (001)-orientated SrTiO 3 using the pulsed laser deposition technique. The thin films samples are semiconducting and ferromagnetic with a Curie temperature close to 270 K, a coercive field of 920 Oe, and a saturation magnetization of 5 µ B per formula unit. Transmission electron microscopy, conducted at room temperature, reveals a majority phase having "I-centered" structure with a ≈ c ≈ a sub 2 and b ≈ 2a sub along with minority phase domains having a "P-type" structure (a sub being the lattice parameter of the cubic perovskite structure). A discussion on the absence of Ni/Mn long-range ordering, in light of recent literature on the ordered double-perovskite La 2 NiMnO 6 is presented.
Owing to high carrier mobilities, good environmental/thermal stability, excellent optical transparency, and compatibility with solution processing, thin-film transistors (TFTs) based on amorphous metal oxide semiconductors (AOSs) are promising alternatives to those based on amorphous silicon (a-Si:H) and low-temperature (<600 °C) poly-silicon (LTPS). However, solution-processed display-relevant indium-gallium-tin-oxide (IGZO) TFTs suffer from low carrier mobilities and/or inferior bias-stress stability versus their sputtered counterparts. Here we report that three types of environmentally benign carbohydrates (sorbitol, sucrose, and glucose) serve as especially efficient fuels for IGZO film combustion synthesis to yield high-performance TFTs. The results indicate that these carbohydrates assist the combustion process by lowering the ignition threshold temperature and, for optimal stoichiometries, enhancing the reaction enthalpy. IGZO TFT mobilities are increased to >8 cm(2) V(-1) s(-1) on SiO2/Si gate dielectrics with significantly improved bias-stress stability. The first correlations between precursor combustion enthalpy and a-MO densification/charge transport are established.
Despite 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 π-deficient building blocks. Since thiazole insertion into π-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 thiazole–thiophene 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 (μ e ) as high as 1.30 cm2/(V·s) (I on/I off > 106) 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 0.001–0.021 cm2/(V·s) to 0.20–0.70 cm2/(V·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 π-conjugated semiconductor thin-films, and it should be studied more in future optoelectronic applications.
BiCuOS, which is isostructural to the layered rare-earth oxysulfides LnCuOS (Ln = La-Eu), was synthesized by a single-step hydrothermal reaction at low temperature (250 degrees C) and pressure (<20 atm). Particular emphasis is placed on how the selection of the proper reaction conditions, such as temperature and pH, achieves a mutual high solubility of the metal-oxide reactants, Bi2O3 and Cu2O, and thus generates BiCuOS in a good yield. The optical and electrical properties of BiCuOS were measured to determine the influence of replacing a rare-earth cation with bismuth. The electrical conductivity of BiCuOS is increased over that of certain layered rare-earth oxysulfides, LnCuOS (Ln = La, Pr, and Nd), and is similar to that of the cerium members, CeCuOS and CeAgOS. Band structure calculations reveal that, similar to other potential transparent conductors containing sixth-row elements, relativistic effects significantly lower the energy of the conduction band, and thus narrow the optical band gap. These low-energy conduction bands are responsible for the electrical and optical properties of BiCuOS.
A single-step, low-temperature (<210 degrees C) and -pressure (<20 atm) hydrothermal method has been developed to synthesize a series of silver delafossites, AgBO2 (B = Al, Ga, Sc, and In). Experimental and computational studies were performed to understand the optical and electric properties of these silver delafossites, including the first in-depth study of AgAlO2 and AgScO2. Their properties were examined as a function of the trivalent cation radius and compared to those of copper delafossites to elucidate the role of both the A- and B-site cations. While optical band gaps for silver delafossites were larger and visible light absorption was lower than values previously reported for polycrystalline powder samples of copper delafossites, the conductivities of silver delafossites are similar or lower. Electronic structure calculations indicate that these properties are due to the scarcity of silver 4d states just below the valence band maximum.
Phase-pure BiCuOSe, which is isostructural to the layered p-type transparent conductor LaCuOS, has been synthesized in high yield by a single-step hydrothermal reaction at low temperature (250 °C) and pressure (<20 atm). A moderate reaction temperature of 250 °C was sufficiently high to solubilize both Bi2O3 and Cu2O and stabilize monovalent copper and low enough to impede the oxidation of dianionic selenium. BiCuOSe exhibits a relatively high electrical conductivity (σ ≈ 3.3 S cm−1) and a reduced band gap (E g = 0.75 eV), which compare favorably with the optoelectronic properties of BiCuOS and the cerium-based oxysulfides, CeAgOS and CeCuOS.
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