Weblike aggregates of coalesced Si nanocrystals are produced by a laser vaporization-controlled condensation technique. SEM micrographs show particles with ∼10 nm diameter but the Raman shift suggests the presence of particles as small as ∼4 nm. FTIR of the freshly prepared particles shows weak peaks due to the stretching, bending, and rocking vibrations of the Si-O-Si bonds, indicating the presence of a surface oxidized layer, SiO x (x < 2). Further oxidation of the Si core appears to be very slow and inefficient under ambient temperature, but annealing at higher temperatures facilitates the oxidation. The particles show luminescence properties that are similar to those of porous Si and Si nanoparticles produced by other techniques. The nanoparticles do not luminesce unless, by exposure to air, they acquire the SiO x passivated coating. They show a short-lived blue emission characteristic of the SiO 2 coating and a biexponential longer-lived red emission. The short lifetime component of the red emission, about 12 µs, does not depend on emission wavelength. The longer-lived component has a lifetime that ranges from 80 to over 130 µs (at 300 K), increasing with emission wavelength. The results are consistent with the quantum confinement mechanism as the source of the red photoluminescence.
IntroductionIn recent years, there has been an intense interest in the synthesis and characterization of nanoparticles. 1-8 Due to their finite small size, the nanoparticles often exhibit novel properties which are different from the bulk materials' properties. [1][2][3][4][5][6][7][8] Research in this area is motivated by the possibility of designing nanostructured materials that possess novel electronic, optical, magnetic, photochemical, and catalytic properties. Such materials are essential for technological advances in photonics, quantum electronics, nonlinear optics, and information storage and processing.Among the many interesting nanoparticles, silicon nanocrystals show important promise for use in Si-based devices for optical communication. This exciting possibility has been hampered by the indirect band gap of bulk Si which prevents efficient electron-photon energy conversion. However, the discovery that porous and nanocrystalline Si emit visible light with a high quantum yield has raised hopes for new photonic Si-based devices. 9-16 This discovery has also stimulated interest in the synthesis of Si nanocrystals which are believed to be the luminescent centers in porous silicon. 9,[17][18][19][20][21][22][23][24][25] Various methods have been used to make Si nanocrystals. They have been generated by the slow combustion of silane, 26 reduction of SiCl 4 by Na, 27 separation from porous Si, 28 UV or IR laser photolysis of silane-type precursors, 29 thermal evaporation, 30 microwave discharge, 31 RF sputtering, 32 and hightemperature aerosol techniques. 18 In most cases, some control over particle size can be achieved by lowering the concentration of the nucleating particles. Laser vaporization of metals has the advantage ...