Comparison of the Atomic Layer Deposition of Tantalum Oxide Thin Films Using Ta(NtBu)(NEt2)3, Ta(NtBu)(NEt2)2Cp, and H2O.

The growth characteristics of Ta2O5 thin films by atomic layer deposition (ALD) were examined using Ta(NtBu)(NEt2)3 (TBTDET) and Ta(NtBu)(NEt2)2Cp (TBDETCp) as Ta-precursors, where tBu, Et, and Cp represent tert-butyl, ethyl, and cyclopentadienyl groups, respectively, along with water vapor as oxygen source. The grown Ta2O5 films were amorphous with very smooth surface morphology for both the Ta-precursors. The saturated ALD growth rates of Ta2O5 films were 0.77 Å cycle-1 at 250 °C and 0.67 Å cycle-1 at 300 °C using TBTDET and TBDETCp precursors, respectively. The thermal decomposition of the amido ligand (NEt2) limited the ALD process temperature below 275 °C for TBTDET precursor. However, the ALD temperature window could be extended up to 325 °C due to a strong Ta-Cp bond for the TBDETCp precursor. Because of the improved thermal stability of TBDETCp precursor, excellent nonuniformity of ∼2% in 200 mm wafer could be achieved with a step coverage of ∼90% in a deep hole structure (aspect ratio 5:1) which is promising for 3-dimensional architecture to form high density memories. Nonetheless, a rather high concentration (∼7 at. %) of carbon impurities was incorporated into the Ta2O5 film using TBDETCp, which was possibly due to readsorption of dissociated ligands as small organic molecules in the growth of Ta2O5 film by ALD. Despite the presence of high carbon concentration which might be an origin of large leakage current under electric fields, the Ta2O5 film using TBDETCp showed a promising resistive switching performance with an endurance cycle as high as ∼17 500 for resistance switching random access memory application. The optical refractive index of the deposited Ta2O5 films was 2.1-2.2 at 632.8 nm using both the Ta-precursors, and indirect optical band gap was estimated to be ∼4.1 eV for both the cases.

Reaction Mechanism Underlying Atomic Layer Deposition of Antimony Telluride Thin Films.

The mechanism underlying the deposition of SbTe films by alternating exposures to Sb(NMe2)3 and Te(GeMe3)2 was investigated. Sb(NMe2)3 and Te(GeMe3)2 were selected because they have very high vapor pressure and are free of Si, Cl, and O atoms in the molecules. The mechanism of deposition was proposed by density functional theory (DFT) calculation and was verified by in-situ quartz crystal microbalance (QCM) analysis. DFT calculation expected the ligand-exchange reactions between the Sb and Te precursors to form Me2NGeMe3 as the byproduct. QCM analysis indicated that a single -NMe2 group in Sb(NMe2)3 reacts with -TeGeMe3 on the surface to form an Sb2Te3 film, and that a small fraction of Sb is incorporated into the film by the thermal decomposition of Sb(NMe2)3. The Te(GeMe3)2 molecules were thermally stable up to 120 degrees C, while the Sb(NMe2)3 molecules decomposed at temperatures of 60 degrees C and higher. Sb-rich SbTe films with different Sb contents were prepared by controlling the partial decomposition of Sb(NMe2)3 molecules, which was enhanced by increasing the pulse time of the precursor.

Controllable synthesis of molybdenum tungsten disulfide alloy for vertically composition-controlled multilayer.

The effective synthesis of two-dimensional transition metal dichalcogenides alloy is essential for successful application in electronic and optical devices based on a tunable band gap. Here we show a synthesis process for Mo1-xWxS2 alloy using sulfurization of super-cycle atomic layer deposition Mo1-xWxOy. Various spectroscopic and microscopic results indicate that the synthesized Mo1-xWxS2 alloys have complete mixing of Mo and W atoms and tunable band gap by systematically controlled composition and layer number. Based on this, we synthesize a vertically composition-controlled (VCC) Mo1-xWxS2 multilayer using five continuous super-cycles with different cycle ratios for each super-cycle. Angle-resolved X-ray photoemission spectroscopy, Raman and ultraviolet-visible spectrophotometer results reveal that a VCC Mo1-xWxS2 multilayer has different vertical composition and broadband light absorption with strong interlayer coupling within a VCC Mo1-xWxS2 multilayer. Further, we demonstrate that a VCC Mo1-xWxS2 multilayer photodetector generates three to four times greater photocurrent than MoS2- and WS2-based devices, owing to the broadband light absorption.

Layer-controlled, wafer-scale, and conformal synthesis of tungsten disulfide nanosheets using atomic layer deposition.

The synthesis of atomically thin transition-metal disulfides (MS2) with layer controllability and large-area uniformity is an essential requirement for their application in electronic and optical devices. In this work, we describe a process for the synthesis of WS2 nanosheets through the sulfurization of an atomic layer deposition (ALD) WO3 film with systematic layer controllability and wafer-level uniformity. The X-ray photoemission spectroscopy, Raman, and photoluminescence measurements exhibit that the ALD-based WS2 nanosheets have good stoichiometry, clear Raman shift, and bandgap dependence as a function of the number of layers. The electron mobility of the monolayer WS2 measured using a field-effect transistor (FET) with a high-k dielectric gate insulator is shown to be better than that of CVD-grown WS2, and the subthreshold swing is comparable to that of an exfoliated MoS2 FET device. Moreover, by utilizing the high conformality of the ALD process, we have developed a process for the fabrication of WS2 nanotubes.