In synthetic diamond plate, the intrapulse correlated dynamics of self-phase modulation and spontaneous Raman scattering by optical phonons were for the first time directly investigated for tightly focused (focusing numerical aperture NA = 0.25) positively-chirped visible-range ultrashort laser pulses with variable durations (0.3-9.5 ps) and energies, transmitted through the sample. The observed modulation of the transmitted light spectra and Stokes Raman scattering spectra for the different pulse durations were related to nonthermal excitation of nonlinear phonon polarization and its eventual picosecond-scale suppression due to thermal decay of optical phonons on the timescale of electron-phonon thermalization in the material.