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Our study shows that metastable quintet state of spin crossover complex [Fe(dpp)2(NCS)2] · py (dpp=dipyrido[3,2-a:2′,3′-c] phenazine, py=pyridine) at low temperatures may be realized by a rapid cooling. The relaxation from quintet state to singlet spin at low temperatures depends on the both of time and previous history of the sample. The U-shaped dents of the magnetic effective moment depending on the temperature after initial rapid zero-field cooling indicate an obvious affection of magnetic field to the realization of singlet state in the transition range. The observations for this sample are indeed consistent with the fact that cooperative effects play a very important role in the spin transition. © 1999 American Institute of Physics.

Amorphous twisted SiO(2) nanobelts have been synthesized on Si wafers using facile thermal evaporation. These nanobelts are produced together with SiO(2) nanowires and a small quantity of SiO(2) nanosprings. Spectral and microstructural analyses suggest that the twisted SiO(2) nanobelts and nanosprings form via a polar surface driven process. Spontaneous polarization on the very thin polar crystalline SiO(2) layers on the amorphous SiO(2) nanobelt and nanospring surfaces makes the nuclei rearrange orderly and causes the nanobelt and nanowire to roll up at a certain twisty angle. The cathodoluminescence spectrum acquired from these SiO(2) nanostructures reveals three emission bands at 4.4, 3.7, and 2.7 eV originating from oxygen-related defect centers. The polar surface driven mechanism can adequately explain the growth of these novel twisty nanobelts and nanosprings which have potential applications in sensors, transducers, resonators, and photonics.

Efficient resonant electron transfer from the surface bonding structure to the conduction band of quantum confined Si nanocrystals is observed by Si nanocrystals in a toluene suspension. Based on the electron transfer mechanism, the enhancement of photoluminescence originates from the band-to-band recombination in the p-type Si nanocrystals suspended in a toluene solution. The energy levels of the electrons in the Si nanocrystals chemisorbed with toluene molecules are calculated using the method of linear combination of atomic orbitals, and the characteristics of the obtained density of states is in good agreement with the observed photoluminescence properties.

111-oriented p-type Si wafer with a resistivity of 1-5 Omega cm was implanted with Fe+ and then annealed at 1100 degrees C in N2 for 60 min, followed by anodization in a solution of HF to form porous structure with beta-FeSi2 nanocrystallites. Photoluminescence (PL) spectral measurements show that a strong PL peak appears in the range of 610-670 nm. The position of the PL peak remains unchanged, but its intensity increases with the storage time in air until about three months and then saturates. C60 molecules were chemically coupled on the porous structure through a kind of silane coupling agent to form a nanocomposite. It is revealed that the stable PL peak monotonically shifts to a pinning wavelength at 570 nm. Experimental results from PL, PL excitation, Raman scattering, and x-ray diffraction measurements clearly show that the pinned PL originates from optical transition in C60-related defect states, whereas the photoexcited carriers occur in the beta-FeSi2 nanocrystallites formed during anodization. This work opens a new way to tailor nanometer environment for seeking optimal luminescent properties.

Photoluminescence (PL) measurements have been performed on the nanocomposites of higher fullerene-coupled porous silicon (PS) nanocrystals. For the C70PS and C76(78)PS nanocomposites, the PL spectra show a pinning wavelength at approximately 565 nm and for the C84PS and C94PS nanosystems the pinning wavelength is at approximately 590 nm. The PL pinning property is closely related to the sorts of the coupled fullerenes. A band mixing model of direct and indirect gaps in a nanometer environment consisting of nc-Si core, SiO2 surface layer, and coupled fullerene has been proposed for calculation of electronic states. Good agreement is achieved between the experiments and theory.

A uniquely structured SiO(x)-capped (x = 0.5-0.8) Si nanowire array with strong blue emission, like a nanobeacon array, was fabricated using electroless metal (silver) deposition on a water plasma-treated Si wafer. Formation of the nanoscale light source array can be understood on the basis of a self-assembled localized microscopic electrochemical cell model and a diffusion-limited aggregation process. Photoluminescence spectral analysis reveals that the intensity of the broad blue-emitting luminescent band centred at around 435 nm strongly depends upon the irradiation of H(2)O(+), HO(+), and O(+) ions, which are present in the water plasma. We attribute the blue PL band to the optical transition of the self-trapped excitons at the surfaces of SiO(x) nanocaps.

Using electrochemical etching of a polycrystalline 3C-SiC target and subsequent ultrasonic treatment in water solution, we have fabricated suspensions of 3C-SiC nanocrystallites that luminesce. Transmission electron microscope observations show that the 3C-SiC nanocrystallites, which uniformly disperse in water, have sizes in the range of 1-6 nm. Photoluminescence and photoluminescence excitation spectral examinations show clear evidence for the quantum confinement of 3C-SiC nanocrystallites with the emission band maximum ranging from 440 to 560 nm. Tunable, composite polystyrene/SiC film can be made by adding polystyrene to a toluene suspension of the 3C-SiC nanocrystallites and then coating the resulting solution onto a Si wafer.

Using C60 molecule as a kind of surface-passivated agent to modify the electronic structure of Si nanocrystallites in porous silicon, we disclose that this kind of C60/nanocrystalline Si coupling system can show a strong blue emission at approximately 460 nm when stored in air for more than one year. After a full characterization of the photoluminescence properties, we propose a luminescent center in the SiOx layer at the surface of a Si nanocrystallite. It is a pair consisting of an oxygen vacancy and an interstitial oxygen. The interstitial oxygen also forms a peroxy linkage with a neighboring lattice oxygen. Radiative recombination of carriers photogenerated from Si nanocrystallite cores in the luminescent centers results in the observed blue photoluminescence. Neutron irradiation experiments support our assignment of the blue emission mechanism. This work improves the understanding of the origin of blue emission from silicon/oxygen-related nanostructured materials.

Four groups of Si nanostructures with and without beta-SiC nanocrystals were fabricated for clarifying the origin of a blue emission with a double-peak structure at 417 and 436 nm. Spectral analyses and microstructural observations show that the blue emission is related to the existence of excess Si atoms in these Si nanostructures. The energy levels of electrons in Si nanocrystals with vacancy defects formed from the excess Si atoms are calculated and the characteristics of the obtained density of states coincide with the observed double-peak emission. The present work provides a possible mechanism of the blue emission in various Si nanostructures.

Si-based Er-doped Si nanostructures were fabricated for exploring efficient light emission from Er ions and Si nanocrystallites. High-resolution transmission electron microscopy observations reveal that Si nanocrystallites are spherically embedded in the SiO2 matrix. Energy-dispersive x-ray analysis indicates that the Er centers are distributed at the surfaces of nanocrystallites surrounded by the SiO2 matrix. Low-frequency Raman scattering investigation shows that Lamb's theory can be adopted to exactly calculate the surface vibration frequencies from acoustic phonons confined in spherical Si nanocrystallites and the matrix effects are negligible.

We propose two designs with which one can obtain a circular light disk with both uniform irradiance and phase, namely, a homodisk on a plane target from a TEM(0, 0) Gaussian beam. The first design is pure-phase filtering masks based on wave theory and computer simulation. The second design, an aspherical lens, satisfies the two requirements successively. We used geometrical optics to obtain uniform irradiance with the aspherical lens. The theoretical results of both designs are reasonably good.