Si clusters are produced in a gas aggregation source and fly through ultrahigh vacuum onto a cold target where they are codeposited with water vapor. Melting of the ice yields immediately a suspension of nanoparticles that emits intense, nondegrading luminescence in the blue wavelength range. Spectroscopic analysis reveals a Si/SiO core-shell structure where the luminescence stems from oxygen deficient defects. The main advantage of our production method is that it yields the luminescent Si nanoparticles in one step. © 2009 American Institute of Physics. ͓DOI: 10.1063/1.3167355͔The process of light emission from materials with an indirect band gap in the bulk has attracted much interest both from a fundamental point of view and from the prospect of applications.1,2 Since the discovery of luminescence from porous silicon at room temperature 3,4 twenty years ago, fabrication of devices such as silicon-based light emitting diodes ͑Ref. 5͒ and lasers 6 has been achieved, and a large variety of types of photoluminescent silicon have been reported in the literature. These include nanowires and nanorods, 7-13 Si/SiO, Si/SiOH sandwich, and core-shell systems, [14][15][16] as well as Si clusters produced by laser photolysis 17,18 or by Si ion implantation in silica glass. 19,20 Furthermore, luminescent Si quantum dots in solutions have been investigated. [21][22][23] Nanoparticles in solution receive great attention because of applications in biological imaging and diagnostic labeling.
24In all the above-mentioned examples the production method plays a crucial role in the way the luminescence wavelength and luminescence efficiency is controlled. Some industrial production methods require specific conditions. For instance, in complementary metal-oxide-semiconductor ͑CMOS͒ processing, a maximum process temperature of only 450°C is allowed. The compatibility with the CMOS production process will become important because integration of light emitters is one of the major goals on the road map in semiconductor industries. This is because the performance of electronic integrated circuits is expected to be greatly increased by using optical signal transmission. 25 While the origins of the luminescence of porous silicon are still debated, the imperative of quantum confinement is generally accepted.26 Free Si clusters down to the size of a few atoms can be produced in molecular beam machines.17,27-31 A further and major requirement to achieve luminescence from Si is a suitable passivation of the surface.32 Pure free Si clusters exhibit dangling bonds that efficiently quench luminescence. 33 In this paper we report on a combination of the cluster beam approach and a passivation technique that overcomes this limitation. Central to this method is the in situ chemical interaction between the surface of pure silicon clusters and a passivation agent. The method yields luminescent clusters in aqueous suspensions immediately and the luminescence intensity remains stable over a period of more than three months. High temperature treatments ...