Laser pyrolysis synthesis and characterization of luminescent silicon nanocrystals

Quantum dots of silicon are very attractive materials due to their photoluminescence (PL) emission that can be very strong at room temperature in the visible range under UV illumination. Weighable batches are demanded for several applications in opto-electronic, photovoltaic, medicine, and so on. Laser pyrolysis of silane in a flow reactor is an efficient method to synthesize silicon nanocrystals, but up to now the production rate for the smallest particles was very low. We present here results of a work aimed to overcome this limitation. Optimization of the laser pyrolysis process has been performed through an elaborate study of the synthesis parameters. Weighable batches of very small silicon particles were obtained in a controlled and reproducible way, with production rate in the 0.1-1 g/h. High-resolution electron microscopy and specific surface measurements show that the particles were true silicon nanocrystals in the 4-9 nm range. We have then studied their PL properties. For this purpose, we have paid a particular attention to the surface passivation, an essential step to obtain efficient PL. Various ways were explored: natural oxidation under air and dispersion in liquids. We show that after natural oxidation, the PL properties are, as expected, in agreement with the quantum confinement model. Strong PL is also obtained by dispersion in solvents, but the interpretation is less straightforward in this case, and as discussed in the paper, needs further investigation.