Uniform broad-area deposition and patterning of SiO2 nanofilms by 172 nm photochemical conversion of liquid tetraethoxysilane layers at 300 K

Oxide films of the quality required for the fabrication of electronic and photonic devices are typically deposited at elevated temperatures and thermal equilibrium, thereby adversely impacting thermal budgets. We report the deposition and patterning of silicon dioxide (SiO2) films of high electrical and optical quality on Si(100) or polymer substrates in a N2 atmosphere and at 300 K by the photochemical conversion of thin liquid tetraethoxysilane (TEOS) layers with narrowband vacuum ultraviolet radiation [vacuum ultraviolet (VUV), 172 nm] provided by efficient microplasma lamps. Irradiating liquid TEOS layers, produced by spin-coating the precursor onto a substrate, with a VUV intensity of 13 mW cm−2, yields 40 nm-thick SiO2 films having a dielectric breakdown strength (Eb) of 5 MV cm−1, for which no precedent exists in the deposition of oxide films at 300 K. If room temperature-deposited films are post-annealed at 200 °C, Eb rises to 7.5 MV cm−1, which is <12% below the measured value (8.5 MV cm−1) for 40 nm SiO2 films grown by thermal oxidation. The deposition of 1 µm thick, stoichiometric SiO2 films requires only 20 min of VUV illumination at low optical fluences, and films with thicknesses of ∼35–60 nm exhibit a refractive index of 1.45 (633 nm). X-ray photoelectron spectrometry and Rutherford backscattering analysis indicate that, despite the deposition temperature, hydrocarbon impurity levels are near or below the detection limit. The capability for depositing 960 nm-thick SiO2 films uniformly (to within 0.6%) by liquid → solid photochemical conversion over a 5 cm diameter Si substrate and patterning films onto flexible polymer substrates has also been demonstrated.