We report the synthesis and characterization of a two-dimensional (2D) MX2Y2-type (M = metal, X, Y = N, S, O, and X ≠ Y) copper 1,3,5-triamino-2,4,6-benzenetriol metal–organic framework (Cu3(TABTO)2-MOF). The role of oxygen in the synthesis of this MOF was investigated. Copper metal is formed along with the MOF when the synthesis is done in argon as suggested by XRD. When the reaction was exposed to air with vigorous stirring, copper metal was not observed by XRD. However, if there is no stirring, then copper metal is formed, and we learned that this is because oxygen was not allowed to enter the solvent due to the formation of a MOF film at the air/water interface. For the sample synthesized in argon (Cu3(TABTO)2-Ar), an insulating Cu3(TABTO)2-Ar pellet (σ < 10–10 S cm–1) became a metallic conductor with an electrical conductivity of 0.78 S cm–1 at 300 K after exposure to iodine vapor. This work provides further insights into the role of oxygen in the synthesis of redox-active ligand-based MOFs, expands the family of 2D redox-active ligand-based electrically conductive MOFs, and offers more opportunities in sensing, photocatalytic, electronic, and energy-related applications.
Molybdenum oxides have various crystal structures and physical properties due to the multiple valence states of the 4d molybdenum. Among them, MoO2 has a distorted rutile structure with chemical stability and metallic behavior. In this study we grew epitaxial (100) MoO2 thin films on (0001) Al2O3 substrates. Through careful control of the Ar-partial pressure and growth temperature, we determined the optimal growth condition. From our structural assessments, MoO2 epitaxial thin films with high crystallinity can only be achieved in very narrow growth conditions such as 500˚C and 7 mTorr. The thin film prepared under optimal condition showed good metallic behavior, which was confirmed by electronic transport and optical reflectance measurements. A detailed electronic structure was also investigated by spectroscopic ellipsometry.
Stochastic inhomogeneous oxidation is an inherent characteristic of copper (Cu), often hindering color tuning and bandgap engineering of oxides. Coherent control of the interface between metal and metal oxide remains unresolved. Coherent propagation of an oxidation front in single‐crystal Cu thin film is demonstrated to achieve a full‐color spectrum for Cu by precisely controlling its oxide‐layer thickness. Grain‐boundary‐free and atomically flat films prepared by atomic‐sputtering epitaxy allow tailoring of the oxide layer with an abrupt interface via heat treatment with a suppressed temperature gradient. Color tuning of nearly full‐color red/green/blue indices is realized by precise control of the oxide‐layer thickness; the samples cover ≈50.4% of the standard red/green/blue color space. The color of copper/copper oxide is realized by the reconstruction of the quantitative yield color from the oxide “pigment” (complex dielectric functions of Cu2O) and light‐layer interference (reflectance spectra obtained from the Fresnel equations) to produce structural color. Furthermore, laser‐oxide lithography is demonstrated with micrometer‐scale linewidth and depth through local phase transformation to oxides embedded in the metal, providing spacing necessary for semiconducting transport and optoelectronics functionality.
An interesting van der Waals material, Ta2NiSe5 has been known one of strong excitonic insulator candidates since it has very small or zero bandgap and can have a strong exciton binding energy because of its quasi-one-dimensional crystal structure. Here we investigate a single crystal Ta2NiSe5 using optical spectroscopy. Ta2NiSe5 has quasi-one-dimensional chains along the a-axis. We have obtained anisotropic optical properties of a single crystal Ta2NiSe5 along the a- and c-axes. The measured a- and c-axis optical conductivities exhibit large anisotropic electronic and phononic properties. With regard to the a-axis optical conductivity, a sharp peak near 3050 cm−1 at 9 K, with a well-defined optical gap ( 1800 cm−1) and a strong temperature-dependence, is observed. With an increase in temperature, this peak broadens and the optical energy gap closes around ∼325 K (). The spectral weight redistribution with respect to the frequency and temperature indicates that the normalized optical energy gap () is . The temperature-dependent superfluid plasma frequency of the excitonic condensation in Ta2NiSe5 has been determined from measured optical data. Our study may pave new avenues in the future research on excitonic insulators.
We investigated the superconducting transition temperature (Tc), critical current density (Jc) and optical properties of optimally doped Ba(Fe0.95Ni0.05)2As2 (Ni-Ba122) single-crystalline epitaxial thin films grown by pulsed laser deposition for the first time. The Tc at zero resistivity was about 20.5 K and the Jc at self-field and 4.2 K was 2.8 MA cm−2 calculated by the Bean model. The superconducting properties such as Tc and Jc of thin films are comparable to those of bulk single-crystal samples. The superfluid plasma frequency (λp,S) of Ni-Ba122 thin film is ∼7033 cm−1 obtained by optical spectroscopic technique. Based on this plasma frequency, we obtained the London penetration depth (λL), ∼226 nm at 8 K, which is comparable to those of optimally Co- and K-doped BaFe2As2 single crystals.
Although large exciton binding energies of typically 0.6–1.0 eV are observed for monolayer transition metal dichalcogenides (TMDs) owing to strong Coulomb interaction, multilayered TMDs yield relatively low exciton binding energies owing to increased dielectric screening. Recently, the ideal carrier-multiplication threshold energy of twice the bandgap has been realized in multilayered semiconducting 2H-MoTe2 with a conversion efficiency of 99%, which suggests strong Coulomb interaction. However, the origin of strong Coulomb interaction in multilayered 2H-MoTe2, including the exciton binding energy, has not been elucidated to date. In this study, unusually large exciton binding energy is observed through optical spectroscopy conducted on CVD-grown 2H-MoTe2. To extract exciton binding energy, the optical conductivity is fitted using the Lorentz model to describe the exciton peaks and the Tauc–Lorentz model to describe the indirect and direct bandgaps. The exciton binding energy of 4 nm thick multilayered 2H-MoTe2 is approximately 300 meV, which is unusually large by one order of magnitude when compared with other multilayered TMD semiconductors such as 2H-MoS2 or 2H-MoSe2. This finding is interpreted in terms of small exciton radius based on the 2D Rydberg model. The exciton radius of multilayered 2H-MoTe2 resembles that of monolayer 2H-MoTe2, whereas those of multilayered 2H-MoS2 and 2H-MoSe2 are large when compared with monolayer 2H-MoS2 and 2H-MoSe2. From the large exciton binding energy in multilayered 2H-MoTe2, it is expected to realize the future applications such as room-temperature and high-temperature polariton lasing.
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