Synthesis of nitrogen-doped diamond films using vibrational excitation of ammonia molecules in laser-assisted combustion flames

摘要

Nitrogen-doped diamond was synthesized in open air using laser-assisted combustion flame method. A wavelength-tunable CO2 laser was used to resonantly excite the vibration modes of ammonia molecules, which were added into the diamond forming combustion flame. The wavelength of the CO2 laser was tuned to match frequencies of the NH wagging mode of the ammonia molecules. High efficiency energy coupling was achieved at laser wavelengths of 9.219, 10.35, and 10.719 μm, which are related to a rotational–vibrational transition (1084.63 cm−1), and splitting of the NH wagging mode (υ2+, 932.51 cm−1 and υ2−, 968.32 cm−1). Vibrational excitations of the ammonia molecules under these wavelengths actively intervenes the reaction courses, which steers the chemical reaction in the combustion flame and eventually promotes nitrogen concentration in the deposited diamond films. Concentration of the doped nitrogen atoms reaches up to 1.5 × 1020 atoms/cm3 in the diamond films deposited with a laser wavelength of 9.219 μm. Optical emission spectroscopy and mass spectrometry were used to study the evolution of chemical reactions with and without laser excitations.