Impact on the Gas Barrier Property of Silicon Oxide Films Prepared by Tetramethylsilane-Based PECVD Incorporating with Ammonia

Abstract

Abstract:The gas barrier property of a silicon oxide (SiO x ) film synthesized from plasma-enhanced chemical vapor deposition using the tetramethysilane (TMS)-oxygen gas mixture was modified by introducing ammonia gas in the glow discharge. The change in the glow discharge with the ammonia gas incorporation was monitored by an optical emission spectrometer (OES). Structures, chemical bond configurations, and material properties of the resulting films were investigated. The introduced ammonia gas in the TMS-oxygen plasma resulted in emission lines dominated by the N 2 and CN species with the suppression of the OH and oxygen-related radicals, thereby introducing nitrogen and carbon atoms in the deposited film. A silicon oxynitride (SiO x N y ) film had the best surface morphology and the lowest residual internal stress was achievable by controlling the reactant gas flow ratio of the ammonia and oxygen. The barrier property to the water vapor permeation of the silicon oxide film (~1.65 g/m 2 /day) deposited onto the polyethylene terephthalate (PET) substrate was thus greatly improved to 0.06 g/m 2 /day for the film synthesized from an adequate TMS-oxygen-ammonia gas mixture.

High Performance Multilayered Organosilicon/Silicon Oxynitride Water Barrier Structure Consecutively Deposited by Plasma-Enhanced Chemical Vapor Deposition at a Low-Temperature

“…The spectra were composed of a significant Si-O-Si stretching mode (denoted as TO 3 in Figure 2b) and a shoulder that could be deconvolved into three peaks at about 1101, 1143, and 1194 cm −1 , respectively. As referred to in the reports [15,17,[19][20][21], these peaks could be identified as the C- reduction in the deposition rate with the deposition temperature increasing was ascribed to the enhancement in the lateral diffusion of the products on the coating surface at an elevated temperature. Meanwhile, the evolutions of the physic-to chemi-adsorptions on the surface that were activated by the substrate temperature were likely to be the main reason for the sharp decrease in the deposition rate as the temperature increased from 30 to 60 °C , which may have resulted in the film densification and a better adhesion to the substrate.…”

“…The surface morphologies of the 300 nm-thick SiOxNy film, the one-paired, and the three-paired organosilicon/SiOxNy multilayered structures are shown in Figure 8a-c, respectively (the corresponding cross-sectional morphologies are given in Figure 8(a1-c1)). In Figure 8a, significant white protrusions in circular shapes (as indicated by arrows) associated with the coverage of the voids were distributed over the surface of the SiOxNy film [17,40,41]. Cracks from the substrate to the film surface could be seen in Figure 8(a1).…”

“…The spectra were composed of a significant Si-O-Si stretching mode (denoted as TO3 in Figure 2b) and a shoulder that could be deconvolved into three peaks at about 1101, 1143, and 1194 cm −1 , respectively. As referred to in the reports [15,17,[19][20][21], these peaks could be identified as the C-H/C-C bonds and the second asymmetric modes of the longitudinal-optic (LO4) and the transverse-optic (TO4) vibration pairs in the Si-O-Si networks. The formation of the C-H/C-C bond was ascribed to the plasma polymerization of only the TMS monomer, whereas the intensity of the TO4 mode corresponded to the degree of the structural disorder in the Si-O-Si networks.…”

“…By optimizing the stress residing in the multilayered structure, a WVTR lower than 10 −4 g/m 2 /day was obtained from the three-paired organosilicon/SiO x multilayered structure [16]. Moreover, the impact of the nitrogen atoms introduced into the SiO x barrier film employed a PECVD system using the reactant gases of tetramethylsilane [TMS; Si(CH 3 ) 4 , TMS], and oxygen with ammonia (NH 3 ) gas incorporation was also demonstrated [17]. The voids that appeared in the SiO x film originating from the terminated bounds in the Si-O-Si networks were filled with the limited incorporation of nitrogen atoms as evidence of their surface morphologies, thus leading to improvement on the barrier performance.…”

Pre-grafted Group on PE Surface by DBD Plasma and Its Influence on the Oxygen Permeation with Coated SiOx

“…In Figure 6 a, the weak peak at 910 cm −1 assigned to the Si–N [ 52 ] in allylamine-modified PE was considered from the incorporated nitrogen, which can release the inner residual stress in the as-deposited SiOx [ 53 ] and be beneficial to a small OTR as shown in Figure 1 .…”