Silicon nitride films fabricated by a plasma-enhanced chemical vapor deposition method for coatings of the laser interferometer gravitational wave detector

Silicon is a potential substrate material for the large-areal-size mirrors of the next-generation laser interferometer gravitational wave detector operated in cryogenics. Silicon nitride thin films uniformly deposited by a chemical vapor deposition method on large-size silicon wafers is a common practice in the silicon integrated circuit industry. We used plasma-enhanced chemical vapor deposition to deposit silicon nitride films on silicon and studied the physical properties of the films that are pertinent to application of mirror coatings for laser interferometer gravitational wave detectors. We measured and analyzed the structure, optical properties, stress, Young's modulus, and mechanical loss of the films, at both room and cryogenic temperatures. Optical extinction coefficients of the films were in the ${10}^{\ensuremath{-}5}$ range at 1550-nm wavelength. Room-temperature mechanical loss of the films varied in the range from low ${10}^{\ensuremath{-}4}$ to low ${10}^{\ensuremath{-}5}$ within the frequency range of interest. The existence of a cryogenic mechanical loss peak depended on the composition of the films. We measured the bond concentrations of $\mathrm{N}─\mathrm{H}$, $\mathrm{Si}─\mathrm{H}$, $\mathrm{Si}─\mathrm{N}$, and $\mathrm{Si}─\mathrm{Si}$ bonds in the films and analyzed the correlations between bond concentrations and cryogenic mechanical losses. We proposed three possible two-level systems associated with the $\mathrm{N}─\mathrm{H}$, $\mathrm{Si}─\mathrm{H}$, and $\mathrm{Si}─\mathrm{N}$ bonds in the film. We inferred that the dominant source of the cryogenic mechanical loss for the silicon nitride films is the two-level system of exchanging position between a ${\mathrm{H}}^{+}$ and electron lone pair associated with the $\mathrm{N}─\mathrm{H}$ bond. Under our deposition conditions, superior properties in terms of high refractive index with a large adjustable range, low optical absorption, and low mechanical loss were achieved for films with lower nitrogen content and lower $\mathrm{N}─\mathrm{H}$ bond concentration. Possible pairing of the silicon nitride films with other materials in the quarter-wave stack is discussed.