Most of recent research on layered chalcogenides is understandably focused on single atomic layers. However, it is unclear if single-layer units are the most ideal structures for enhanced gas-solid interactions. To probe this issue further, we have prepared large-area MoS2 sheets ranging from single to multiple layers on 300 nm SiO2/Si substrates using the micromechanical exfoliation method. The thickness and layering of the sheets were identified by optical microscope, invoking recently reported specific optical color contrast, and further confirmed by AFM and Raman spectroscopy. The MoS2 transistors with different thicknesses were assessed for gas-sensing performances with exposure to NO2, NH3, and humidity in different conditions such as gate bias and light irradiation. The results show that, compared to the single-layer counterpart, transistors of few MoS2 layers exhibit excellent sensitivity, recovery, and ability to be manipulated by gate bias and green light. Further, our ab initio DFT calculations on single-layer and bilayer MoS2 show that the charge transfer is the reason for the decrease in resistance in the presence of applied field.

With a motivation to understand microscopic aspects of ScN, ZrN, and HfN relevant to the thermoelectric properties of nitride metal/semiconductor superlattices, we determine their electronic structure, vibrational spectra and thermal properties using first-principles calculations based on density functional theory with a generalized gradient approximation of the exchange correlation energy. We find a large energy gap in the phonon dispersions of metallic ZrN and HfN, but a gapless phonon spectrum for ScN spanning the same energy range, this suggests that a reduced thermal conductivity, suitable for thermoelectric applications, should arise in superlattices made with ScN and ZrN or ScN and HfN. To obtain an electronic energy band gap of ScN comparable to experiment, we use a Hubbard correction with a parameter U ͑=3.5 eV͒. Anomalies in the acoustic branches of the phonon dispersion of ZrN and HfN, manifested as dips in the bands, can be understood through the nesting of Fermi surface determined from our calculations. To connect with transport properties, we have determined effective masses of ScN and determined their dependence on the U parameter. Using the relaxation time approximation in the Boltzmann transport theory, we estimate the temperature dependence of the lattice thermal conductivity and discuss the chemical trends among these nitrides.

Dielectric properties of ultrathin AlO (1.1-4.4 nm) in metal-insulator-metal (M-I-M) Al/AlO/Al trilayers fabricated in situ using an integrated sputtering and atomic layer deposition (ALD) system were investigated. An M-I interfacial layer (IL) formed during the pre-ALD sample transfer even under high vacuum has a profound effect on the dielectric properties of the AlO with a significantly reduced dielectric constant (ε) of 0.5-3.3 as compared to the bulk ε ∼ 9.2. Moreover, the observed soft-type electric breakdown suggests defects in both the M-I interface and the AlO film. By controlling the pre-ALD exposure to reduce the IL to a negligible level, a high ε up to 8.9 was obtained on the ALD AlO films with thicknesses from 3.3 to 4.4 nm, corresponding to an effective oxide thickness (EOT) of ∼1.4-1.9 nm, respectively, which are comparable to the EOTs found in high-K dielectrics like HfO at 3-4 nm in thickness and further suggest that the ultrathin ALD AlO produced in optimal conditions may provide a low-cost alternative gate dielectric for CMOS. While ε decreases at a smaller AlO thickness, the hard-type dielectric breakdown at 32 MV/cm and in situ scanning tunneling spectroscopy revealed band gap ∼2.63 eV comparable to that of an epitaxial AlO film. This suggests that the IL is unlikely a dominant reason for the reduced ε at the AlO thickness of 1.1-2.2 nm but rather a consequence of the electron tunneling as confirmed in the transport measurement. This result demonstrates the critical importance in controlling the IL to achieving high-performance ultrathin dielectric in MIM structures.

The energy storage properties of Pb0.92La0.08Zr0.52Ti0.48O3 (PLZT) films grown via pulsed laser deposition were evaluated at variable film thickness of 125, 250, 500, and 1000 nm. These films show high dielectric permittivity up to ∼1200. Cyclic I-V measurements were used to evaluate the dielectric properties of these thin films, which not only provide the total electric displacement, but also separate contributions from each of the relevant components including electric conductivity (D1), dielectric capacitance (D2), and relaxor-ferroelectric domain switching polarization (P). The results show that, as the film thickness increases, the material transits from a linear dielectric to nonlinear relaxor-ferroelectric. While the energy storage per volume increases with the film thickness, the energy storage efficiency drops from ∼80% to ∼30%. The PLZT films can be optimized for different energy storage applications by tuning the film thickness to optimize between the linear and nonlinear dielectric properties and energy storage efficiency.