Al-doped ZnO (AZO) films were deposited by atomic layer deposition (ALD) on borosilicate glass and sapphire(0001) substrates. The Al composition of the films was varied from 1% to 4% by controlling the ratio of Zn:Al pulses. Film resistivity was measured as a function of Al content and the substrate temperature used for ALD deposition. X-ray diffraction (XRD) was performed on the films, showing a reduction in lattice parameter, as a function of Al concentration, indicating that Al 3þ ions occupy substitutional sites in the ZnO lattice. The resistivity of films deposited on sapphire substrates (7.7 Â 10 -4 Ω cm) was lower than that on glass (3.0 Â 10 -3 Ω cm), because of the formation of textured grains with the c-axis aligned with respect to the sapphire surface, as confirmed by XRD. The surface morphology of the films on glass and sapphire was compared using scanning tunneling microscopy (STM) and scanning electron microscopy (SEM), which showed similar grain sizes on each substrate, suggesting that the difference in conductivity was due to grain orientation rather than microstructural differences. Optical transparency was measured to be >80% for wavelengths of 370-1600 nm.

Quantum dots provide unique advantages in the design of novel optoelectronic devices owing to the ability to tune their properties as a function of size. Here we demonstrate a new technique for fabrication of quantum dots during the nucleation stage of atomic layer deposition (ALD) of PbS. Islands with sub-10 nm diameters were observed during the initial ALD cycles by transmission electron microscopy, and in situ observations of the coalescence and sublimation behavior of these islands show the possibility of further modifying the size and density of dots by annealing. The ALD process can be used to cover high-aspect-ratio nanostructures, as demonstrated by the uniform coating of a Si nanowire array with a single layer of PbS quantum dots. Photoluminescence measurements on the quantum dot/nanowire composites show a blue shift when the number of ALD cycles is decreased, suggesting a route to fabricate unique three-dimensional nanostructured devices such as solar cells.

Atomic layer deposition (ALD) was used to grow both PbS quantum dots and Al 2 O 3 barrier layers in a solid-state quantum dot-sensitized solar cell (QDSSC). Barrier layers grown prior to quantum dots resulted in a near-doubling of device efficiency (0.30% to 0.57%) whereas barrier layers grown after quantum dots did not improve efficiency, indicating the importance of quantum dots in recombination processes.

Area-selective atomic layer deposition (ALD) of lead sulfide (PbS) was achieved on octadecyltrichlorosilane (ODTS)-patterned silicon substrates. We investigated the capability of ODTS self-assembled monolayers (SAMs) to deactivate the ALD PbS surface reactions as a function of dipping time in ODTS solution. The reaction mechanism was investigated using density functional theory (DFT), which showed that the initial ALD half-reaction is energetically unfavorable on a methyl-terminated SAM surface. Conventional photolithography was used to create oxide patterns on which ODTS SAMs were selectively grown. Consequently, PbS thin films were grown selectively only where ODTS was not present, whereas deposition was blocked in regions where ODTS was grown. The resulting fabricated patterns were characterized by scanning electron microscopy and Auger electron spectroscopy, which demonstrated that ALD PbS was well confined to defined patterns with high selectivity by ODTS SAMs. In addition, AFM lithography was employed to create nanoscale PbS patterns. Our results show that this method can be applied to various device-fabrication processes, presenting new opportunities for various nanofabrication schemes and manifesting the benefits of self-assembly.

New deposition techniques for amorphous oxide semiconductors compatible with silicon back end of line manufacturing are needed for 3D monolithic integration of thin‐film electronics. Here, three atomic layer deposition (ALD) processes are compared for the fabrication of amorphous zinc tin oxide (ZTO) channels in bottom‐gate, top‐contact n‐channel transistors. As‐deposited ZTO films, made by ALD at 150–200 °C, exhibit semiconducting, enhancement‐mode behavior with electron mobility as high as 13 cm2 V−1 s−1, due to a low density of oxygen‐related defects. ZTO deposited at 200 °C using a hybrid thermal‐plasma ALD process with an optimal tin composition of 21%, post‐annealed at 400 °C, shows excellent performance with a record high mobility of 22.1 cm2 V–1 s–1 and a subthreshold slope of 0.29 V dec–1. Increasing the deposition temperature and performing post‐deposition anneals at 300–500 °C lead to an increased density of the X‐ray amorphous ZTO film, improving its electrical properties. By optimizing the ZTO active layer thickness and using a high‐k gate insulator (ALD Al2O3), the transistor switching voltage is lowered, enabling electrical compatibility with silicon integrated circuits. This work opens the possibility of monolithic integration of ALD ZTO‐based thin‐film electronics with silicon integrated circuits or onto large‐area flexible substrates.

This work explains the bowing effect of the band gap as a result of the changing S concentration in Zn(O,S).

There is an increasing interest in additive nanomanufacturing processes, which enable customizable patterning of functional materials and devices on a wide range of substrates. However, there are relatively few techniques with the ability to directly 3D print patterns of functional materials with sub-micron resolution. In this study, we demonstrate the use of additive electrohydrodynamic jet (ejet) printing with an average line width of 312 nm, which acts as an inhibitor for area-selective atomic layer deposition (AS-ALD) of a range of metal oxides. We also demonstrate subtractive e-jet printing with solvent inks that dissolve polymer inhibitor layers in specific regions, which enables localized AS-ALD within those regions. The chemical selectivity and morphology of e-jet patterned polymers towards binary and ternary oxides of ZnO, Al 2 O 3 , and SnO 2 were quantified using X-ray photoelectron spectroscopy, atomic force microscopy, and Auger electron spectroscopy. This approach enables patterning of functional oxide semiconductors, insulators, and transparent conducting oxides with tunable composition, Åscale control of thickness, and sub-μm resolution in the x−y plane. Using a combination of additive and subtractive e-jet printing with AS-ALD, a thin-film transistor was fabricated using zinc−tin-oxide for the semiconductor channel and aluminum-doped zinc oxide as the source and drain electrical contacts. In the future, this technique can be used to print integrated electronics with sub-micron resolution on a variety of substrates.

Atomic layer deposition allows the fabrication of BaTiO3 (BTO) ultrathin films with tunable dielectric properties, which is a promising material for electronic and optical technology. Industrial applicability necessitates a better understanding of their atomic structure and corresponding properties. Through the use of element-specific X-ray absorption near edge structure (XANES) analysis, O K-edge of BTO as a function of cation composition and underlying substrate (RuO2 and SiO2) is revealed. By employing density functional theory and multiple scattering simulations, we analyze the distortions in BTO’s bonding environment captured by the XANES spectra. The spectral weight shifts to lower energy with increasing Ti content and provides an atomic scale (microscopic) explanation for the increase in leakage current density. Differences in film morphologies in the first few layers near substrate–film interfaces reveal BTO’s homogeneous growth on RuO2 and its distorted growth on SiO2. This work links structural changes to BTO thin-film properties and provides insight necessary for optimizing future BTO and other ternary metal oxide-based thin-film devices.