A new nucleation method to form diamond by chemically pretreating silicon (Ill)surfaces is reported. The nucleation consists of binding covalently 2,2-divinyladamantane molecules on the silicon substrate. Then low-pressure diamond growth was performed for 2 h via microwave plasma CVD in a tubular deposition system. The resulting diamond layers presented a good cristallinity and the Raman spectra showed a single very sharp peak at 1331 cm(-1), indicating high-quality diamonds.