The hysteresis and kinetics of capillary condensation of N2 and Ar in linear mesopores, produced by etching of Si wafers, have been studied for different pore shapes, including the ink bottle geometry. Pore blocking has been observed in the solid state of the pore fillings, but not in the liquid state. We conclude that individual local geometries such as the pore mouth, a blind end, or a single constriction have no effect on the shape of sorption isotherms, that the pore space should be regarded as a statistical ensemble of pore segments with a lot of quenched disorder.

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We show that light emission from different systems of silicon nanocrystals does behave as expected for indirect-band-gap quantum dots. Photoluminescence excited on the low energy part of the distribution of Si nanocrystals exhibits a set of narrow peaks associated with Si TA and TO momentumconserving phonon-assisted optical transitions. These spectra allow us to determine the ratio of nophonon transitions to TA and TO phonon-assisted processes over a wide range of confinement energies. The ratio between these recombination channels changes by 2 orders of magnitude with increasing confinement energy. For confinement energies above 0.7 eV the radiative transitions are governed by no-phonon quasidirect processes. [S0031-9007 (98)07199-3] PACS numbers: 78.55.Ap, 78.66.Li

Molecular oxygen plays an important role in many of the chemical reactions involved in the synthesis of biological life. In this review, we explore the interaction between O2 and silicon nanocrystals, which can be employed in the photosynthesis of singlet oxygen. We demonstrate that nanoscale Si has entirely new properties owing to morphological and quantum size effects, i.e., large accessible surface areas and excitons of variable energies and with well‐defined spin structures. These features result in new emerging functionality for nanoscale silicon: it is a very efficient spin‐flip activator of O2, and therefore, a chemically and biologically active material. This whole effect is based on energy transfer from long‐lived electronic excitations confined in Si nanocrystals to surrounding O2 via the exchange of single electrons of opposite spin, thus enabling the spin‐flip activation of O2. Further, we discuss the implications of these findings for physics, chemistry, biology, and medicine.

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The spontaneous formation of organized nanocrystals in semiconductors has been observed during heteroepitaxial growth and chemical synthesis. The ability to fabricate size-controlled silicon nanocrystals encapsulated by insulating SiO2 would be of significant interest to the microelectronics industry. But reproducible manufacture of such crystals is hampered by the amorphous nature of SiO2 and the differing thermal expansion coefficients of the two materials. Previous attempts to fabricate Si nanocrystals failed to achieve control over their shape and crystallographic orientation, the latter property being important in systems such as Si quantum dots. Here we report the self-organization of Si nanocrystals larger than 80 A into brick-shaped crystallites oriented along the (111) crystallographic direction. The nanocrystals are formed by the solid-phase crystallization of nanometre-thick layers of amorphous Si confined between SiO2 layers. The shape and orientation of the crystallites results in relatively narrow photoluminescence, whereas isotropic particles produce qualitatively different, broad light emission. Our results should aid the development of maskless, reproducible Si nanofabrication techniques.