We have implemented linear and nonlinear optical spectroscopies to monitor and control the growth of SixGe1-x films. Using spectroscopic ellipsometry and the virtual substrate approximation (VSA), controlled growth of compositionally graded SiGe films deposited by chemical vapor deposition (CVD) is achieved by adjustment of disilane now based on feedback from ellipsometric inputs, Stepped and linear growth profiles are investigated. Using spectroscopic, surface second harmonic generation (SHG) by a tunable, unamplified Ti:sapphire 100 femtosecond (fs) laser, shifts of the SH spectral feature near the Si E-1 critical point with varying Ge composition are observed. A comparison is made to linear spectroscopy and related qualitatively to surface composition. Data acquisition time is then reduced to a few seconds by substituting a 10 fs laser and spectrally dispersing generated SH radiation onto an array detector, thus enabling real-time spectroscopic SHG. The reflected SH spectrum near the E-1 region is also highly sensitive to bull; boron doping of SiGe. Definite trends in the peak positions and amplitudes as a function of boron incorporation are observed and interpreted qualitatively in terms of dc-electric-field-induced SHG in the depletion region. The results demonstrate the feasibility of SE and spectroscopic SHG operating as complementary, in situ sensors of Sice CVD.