A bottom-up process from precursor
development for tin to plasma-enhanced
atomic layer deposition (PEALD) for tin(IV) oxide and its successful
implementation in a working thin-film transistor device is reported.
PEALD of tin(IV) oxide thin films at low temperatures down to 60 °C
employing tetrakis-(dimethylamino)propyl tin(IV) [Sn(DMP)4] and oxygen plasma
is demonstrated. The liquid precursor has been synthesized and thoroughly
characterized with thermogravimetric analyses, revealing sufficient
volatility and long-term thermal stability. [Sn(DMP)4]
demonstrates typical saturation behavior and constant growth rates
of 0.27 or 0.42 Å cycle–1 at 150 and 60 °C,
respectively, in PEALD experiments. Within the ALD regime, the films
are smooth, uniform, and of high purity. On the basis of these promising
features, the PEALD process was optimized wherein a 6 nm thick tin
oxide channel material layer deposited at 60 °C was applied in
bottom-contact bottom-gate thin-film transistors, showing a remarkable
on/off ratio of 107 and field-effect mobility of μFE ≈ 12 cm2 V–1 s–1 for the as-deposited thin films deposited at such low temperatures.
A study on the plasma-enhanced atomic layer deposition of amorphous inorganic oxides SiO and AlO on polypropylene (PP) was carried out with respect to growth taking place at the interface of the polymer substrate and the thin film employing in situ quartz-crystal microbalance (QCM) experiments. A model layer of spin-coated PP (scPP) was deposited on QCM crystals prior to depositions to allow a transfer of findings from QCM studies to industrially applied PP foil. The influence of precursor choice (trimethylaluminum (TMA) vs [3-(dimethylamino)propyl]-dimethyl aluminum (DMAD)) and of plasma pretreatment on the monitored QCM response was investigated. Furthermore, dyads of SiO/AlO, using different Al precursors for the AlO thin-film deposition, were investigated regarding their barrier performance. Although the growth of SiO and AlO from TMA on scPP is significantly hindered if no oxygen plasma pretreatment is applied to the scPP prior to depositions, the DMAD process was found to yield comparable AlO growth directly on scPP similar to that found on a bare QCM crystal. From this, the interface formed between the AlO and the PP substrate is suggested to be different for the two precursors TMA and DMAD due to different growth modes. Furthermore, the residual stress of the thin films influences the barrier properties of SiO/AlO dyads. Dyads composed of 5 nm AlO (DMAD) + 5 nm SiO exhibit an oxygen transmission rate (OTR) of 57.4 cm m day, which correlates with a barrier improvement factor of 24 against 5 when AlO from TMA is applied.
Vapor phase deposited iron oxide nanostructures are promising for fabrication of solid state chemical sensors, photoelectrodes for solar water splitting, batteries, and logic devices. The deposition of iron oxide via chemical vapor deposition (CVD) or atomic layer deposition (ALD) under mild conditions necessitates a precursor that comprises good volatility, stability, and reactivity. Here, a versatile iron precursor, namely [bis(N‐isopropylketoiminate) iron(II)], which possesses ideal characteristics both for low‐temperature CVD and water‐assisted ALD processes, is reported. The films are thoroughly investigated toward phase, composition, and morphology. As‐deposited ALD grown Fe2O3 layers are amorphous, while the CVD process in the presence of oxygen leads to polycrystalline hematite layers. The nanostructured iron oxide grown via CVD consists of nanoplatelets that are appealing for photoelectrochemical applications. Preliminary tests of the photoelectrocatalytic activity of CVD‐grown Fe2O3 layers show photocurrent densities up to 0.3 mA cm−2 at 1.2 V versus reversible hydrogen electrode (RHE) and 1.2 mA cm−2 at 1.6 V versus RHE under simulated sunlight (1 sun). Surface modification by cobalt oxyhydroxide (Co‐Pi) co‐catalyst is found to have a highly beneficial effect on photocurrent, leading to maximum monochromatic quantum efficiencies of 10% at 400 nm and 4% at 500 nm at 1.5 V versus RHE.
Identification and synthesis of intramolecularly donor-stabilized aluminium(III) complexes, which contain a 3-(dimethylamino)propyl (DMP) ligand, as novel atomic layer deposition (ALD) precursors has enabled the development of new and promising ALD processes for Al O thin films at low temperatures. Key for this promising outcome is the nature of the ligand combination that leads to heteroleptic Al complexes encompassing optimal volatility, thermal stability and reactivity. The first ever example of the application of this family of Al precursors for ALD is reported here. The process shows typical ALD like growth characteristics yielding homogeneous, smooth and high purity Al O thin films that are comparable to Al O layers grown by well-established, but highly pyrophoric, trimethylaluminium (TMA)-based ALD processes. This is a significant development based on the fact that these compounds are non-pyrophoric in nature and therefore should be considered as an alternative to the industrial TMA-based Al O ALD process used in many technological fields of application.
In article number 1907506, Anjana Devi and co‐workers introduce a new, nonpyrophoric zinc precursor for plasma enhanced atomic layer deposition (PEALD) of zinc oxide (ZnO). Here, oxygen plasma is used to react with adsorbed zinc precursor on chemiresistor structures to form highly pure ZnO which is used effectively as a selective gas sensing layer for NO2 in a functional gas sensor device.
Graphene
and other single-layer structures are pursued as high-flux
separation membranes, although imparting porosity endangers their
crystalline integrity. In contrast, bilayer silica composed of corner-sharing
(SiO4) units is foreseen to be permeable for small molecules
due to its intrinsic lattice openings. This study sheds light on the
mass transport properties of freestanding 2D SiO2 upon
using atomic layer deposition (ALD) to grow large-area films on Au/mica
substrates followed by transfer onto Si3N4 windows.
Permeation experiments with gaseous and vaporous substances reveal
the suspended material to be porous, but the membrane selectivity
appears to diverge from the size exclusion principle. Whereas the
passage of inert gas molecules is hindered with a permeance below
10–7 mol·s–1·m–2·Pa–1, condensable species like water are
found to cross vitreous bilayer silica a thousand times faster in
accordance with their superficial affinity. This work paves the way
for bilayer oxides to be addressed as inherent 2D membranes.
Owing to the limited availability of suitable precursors for vaporp hase deposition of rare-earth containing thin-filmm aterials, new or improved precursors are sought after.I nt his study,w ee xplored new precursors for atomic layer deposition(ALD)o fc erium (Ce) and ytterbium(Yb) containing thin films. As eries of homoleptic tris-guanidinate and tris-amidinatec omplexes of cerium (Ce) and ytterbium (Yb) were synthesized andt horoughlyc haracterized. The Csubstituents on the N-C-N backbone (Me, NMe 2 ,N Et 2 ,w here Me = methyl, Et = ethyl) and the N-substituents from symmetrical iso-propyl (iPr) to asymmetrical tertiary-butyl (tBu) and Et were systematically varied to study the influence of the substituents on the physicochemical properties of the resulting compounds. Single crystal structures of [Ce(dpdmg) 3 ] 1 and [Yb(dpdmg) 3 ] 6 (dpdmg = N,N'-diisopropyl-2-dimethylamido-guanidinate) highlightamonomeric nature in the solid-state with ad istorted trigonal prismatic geometry.T he thermogravimetric analysis shows that the complexes are volatile and emphasize that increasing asym-metryi nt he complexes lowers their meltingp oints while reducingt heir thermal stability.D ensityf unctionalt heory (DFT) was used to study the reactivity of amidinates and guanidinates of Ce and Yb complexes towards oxygen (O 2) and water (H 2 O). Signified by the DFT calculations, the guanidinates show an increased reactivity toward water compared to the amidinate complexes. Furthermore,t he Ce complexes are more reactive compared to the Yb complexes,i ndicating even ar eactivity towards oxygen potentiallye xploitable for ALD purposes. As arepresentative precursor,the highly reactive [Ce(dpdmg) 3 ] 1 wasu sed for proof-of-principleA LD depositions of CeO 2 thin films using watera sc o-reactant. The self-limited ALD growth process could be confirmed at 160 8Cw ithp olycrystalline cubic CeO 2 films formed on Si(100) substrates. This study confirmst hat moving towards nitrogen-coordinated rare-earth complexes bearing the guanidinate and amidinate ligands can indeed be very appealing in terms of new precursors for ALD of rare earth based materials.
In this paper, a direct chemical vapor deposition (CVD) approach is applied for the first time to synthesize high quality copper oxide (CuO), copper tungstate (CuWO4) and tungsten oxide (WO3) on F:SnO2 (FTO) substrates for photocatalytic water splitting.
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