The diamond films were deposited on a Si substrate with chemical vapor deposition MCVD using methanehydrogen gas. Raman active phonon and sp2/sp3 ratio in diamond/Si(100) films were investigated by Raman spectra in the difference scattering configurations. Furthermore, the Raman scattering spectrum of diamond/Si (100) hetero-junction was measured with different thickness to investigate the spin dynamics of nitrogen vacancy spins. The Fluorescence scanning microscopy indicated that nitrogen vacancy center electron spin was coupled to the host nitrogen nuclear spin by the electron spin resonance. The strong peak of 1332 cm?1 displayed the F2g symmetry of diamond, while the broad E2g mode peak of 1550 cm?1 was a broad band G mode, and 1150 cm?1 peak corresponded to the nano-diamond and disordered graphitic carbon form with disordered SP2 hybridization. The Raman spectra of the diamond films were observed as a function of the residual stress, crystal size and their orientation. The peaks of 1132 cm?1 and 1480 cm?1 were associated with hydrogen bonding. The transport of diamond exhibited sp3 spin related effect. The diamond/Si(100) PDOS is the results of spin-related couple of sp3, p and d orbital hybridization. The spin dynamics was achieved by the orbital competition, strong crystal field and charge order.