저널

The orientational cross-over phenomena in an RF sputtering growth of TiN films were studied in an in-situ, real-time synchrotron x-ray scattering experiment. For the films grown with pure Ar sputtering gas, the cross-over from the more strained (002)-oriented grains to the less strained (111)-oriented grains occurred as the film thickness was increased. As the sputtering power was increased, the cross-over thickness, at which the growth orientation changes from the <002> to the <111> direction, was decreased. The addition of $N_2$ besides Ar as sputtering gas suppressed the cross-over, and consequently resulted in the (002) preferred orientation without exhibiting the cross-over. We attribute the observed cross-over phenomena to the competition between the surface and the strain energy. The x-ray powder diffraction, the x-ray reflectivity, and the ex-situ AFM surface topology study consistently suggest that the microscopic growth front was in fact always the (002) planes. In the initial stage of growth, the (002) planes were aligned to the substrate surface to minimize the surface energy. At later stages, however, the (002) growth front tilted away from the surface by about $60^{circ}$ to relax the strain, which caused the cross-over of the preferred growth direction to the <111> direction.