The influence of the composition within multilayered heterostructure oxide semiconductors has a critical impact on the performance of thin-film transistor (TFT) devices. The heterostructures, comprising alternating polycrystalline indium oxide and zinc oxide layers, are fabricated by a facile atomic layer deposition (ALD) process, enabling the tuning of its electrical properties by precisely controlling the thickness of the individual layers. This subsequently results in enhanced TFT performance for the optimized stacked architecture after mild thermal annealing at temperatures as low as 200 °C. Superior transistor characteristics, resulting in an average field-effect mobility (μ) of 9.3 cm V s ( W/ L = 500), an on/off ratio ( I/ I) of 5.3 × 10, and a subthreshold swing of 162 mV dec, combined with excellent long-term and bias stress stability are thus demonstrated. Moreover, the inherent semiconducting mechanism in such multilayered heterostructures can be conveniently tuned by controlling the thickness of the individual layers. Herein, devices comprising a higher InO/ZnO ratio, based on individual layer thicknesses, are predominantly governed by percolation conduction with temperature-independent charge carrier mobility. Careful adjustment of the individual oxide layer thicknesses in devices composed of stacked layers plays a vital role in the reduction of trap states, both interfacial and bulk, which consequently deteriorates the overall device performance. The findings enable an improved understanding of the correlation between TFT performance and the respective thin-film composition in ALD-based heterostructure oxides.

Multilayer indium/zinc oxide thin films show high performance in transistor device performance depending on their layer sequence and thickness.

Here, we show that the synergistic interplay between two binding equilibria, acting at different sites of a (Zn)phthalocyanine-amidine molecule (Pc1), enables the dissociation of the photoinactive phthalocyanine dimer (Pc1)2 into a three-component system, in which a sequence of light harvesting, charge separation, and charge shift is successfully proven. The aforementioned dimer is assembled by dual amidine-Zn(II) coordination between neighboring Pc1 molecules and gives rise to high association constants (KD ≈ 10(11) M(-1)). Such extraordinary stability hampers the individual binding of either carboxylic acid ligands through the amidine group or pyridine-type ligands through the Zn(II) metal atom to (Pc1)2. However, the combined addition of both ligands, which cooperatively bind to different sites of Pc1 through distinct noncovalent interactions, efficiently shifts the overall equilibrium toward a photoactive tricomponent species. In particular, when a fullerene-carboxylic acid (C60A) and either a dimethylamino-pyridine (DMAP) or a phenothiazine-pyridine ligand (PTZP) are simultaneously present, the photoactivity is turned on and evidence is given for an electron transfer from photoexcited Pc1 to the electron-accepting C60A that affords the DMAP-Pc1(•+)-C60A(•-) or PTZP-Pc1(•+)-C60A(•-) radical ion pair states. Only in the latter case does a cascade of photoinduced electron transfer processes afford the PTZP(•+)-Pc1-C60A(•-) radical ion pair state. The latter is formed via a thermodynamically driven charge shift evolving from PTZP-Pc1(•+)-C60A(•-) and exhibits lifetimes that are notably longer than those of DMAP-Pc1(•+)-C60A(•-).

ZnS nanoparticles have been synthesized on vertically aligned carbon nanotubes by gas-phase conversion of ZnO nanoparticles which have been tethered on vertically aligned carbon nanotubes using atomic layer deposition (ALD). The resulting ZnO@CNT nanocomposite has been converted to ZnS@CNT by reacting it with hydrogen sulfide using thioacetamide as a precursor. The composition of the resulting nanocomposite could be tuned from a mixed ternary ZnS/ZnO@CNT nanocomposite to a pure ZnS@CNT nanocomposite. At the same time, the amount of wurtzite and sphalerite phases varies in the ZnS@CNT nanocomposite. The resulting nanocomposites were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), selected area electron diffraction (SAED), ultraviolet-visible diffuse reflectance spectroscopy (UV-VIS DRS) and photoluminescence spectroscopy (PL). Finally, the different nanocomposites were tested for their photocatalytic activity by the photocatalytic decomposition under visible light using methyl orange (MO). Herein a systematic study of the photocatalytic activity of different compositions of ZnS in the ZnS@CNT nanocomposite was performed for the first time.