The lack of a dipolar second order susceptibility (χ(2)) in silicon due to its centro-symmetric diamond lattice usually inhibits efficient second order nonlinear optical processes in the silicon bulk. Depositing stressed silicon nitride layers or growing a thermal oxide layer introduces an inhomogeneous strain into the silicon lattice and breaks the centro-symmetry of its crystal structure thereby creating a χ(2). This causes enhanced second harmonic generation and was observed in reflection and transmission measurements for wavelengths in the infrared. However strain is not the only means to break the structures symmetry. Fixed charges at the silicon nitride/silicon interface cause a high electric field close to the silicon interface which causes electric-field-induced-second-harmonic (EFISH) contributions too. The combination of both effects leads to χ(2) values which are estimated to be of the order as classic χ(2) materials like KDP or LiNiO3. This paves the way for the exploitation of other second order nonlinear processes in the area of silicon photonics and is an example how fundamental optical properties of materials can be altered by strain.
A study of the non-linear optical properties of Si-nc embedded in SiO2 has been performed by using the z-scan method in the nanosecond and femtosecond ranges. Substoichiometric SiOx films were grown by plasma-enhanced chemical-vapor deposition (PECVD) on silica substrates for Si excesses up to 24 at. %. An annealing at 1250 °C for 1 hour was performed in order to precipitate Si-nc, as shown by EFTEM images. Z-scan results have shown that, by using 5-ns pulses, the non-linear process is ruled by thermal effects and only a negative contribution can be observed in the non-linear refractive index, with typical values around -10-10 cm2/W. On the other hand, femtosecond excitation has revealed a pure electronic contribution to the nonlinear refractive index, obtaining values in the order of 10-12 cm2/W. Simulations of heat propagation have shown that the onset of the temperature rise is delayed more than half pulse-width respect to the starting edge of the excitation. A maximum temperature increase of ΔT = 123.1 °C has been found after 3.5 ns of the laser pulse maximum. In order to minimize the thermal contribution to the z-scan transmittance and extract the electronic part, the sample response has been analyzed during the first few nanoseconds. By this method we found a reduction of 20 % in the thermal effects. So that, shorter pulses have to be used to obtain just pure electronic non-linearities.
Optical gain has been recently observed in ion implanted Si nanocrystals (nc). Critical issues to the observation of optical gain are the formation of a waveguide structure to improve the mode confinement and a large nanocrystal area den-sity in the samples. Here we confirm these results by measuring optical gain by the variable stripe length (VSL) method on a set of silicon nanocrystals (nc) formed by plasma enhanced chemical vapor deposition (PECVD) and annealing treatments. Time resolved VSL measurements with ns pulses at high pumping fluencies have revealed fast component in the recombination dynamics under gain conditions. Lifetime shortening and superlinear emission have been unambi-guously observed. The spectral shape of the fast luminescence is consistent with the amplified spontaneous emission lineshape (ASE) observed under CW pumping conditions and overlaps the gain spectral band. The observation of light amplification is critically dependent on a very delicate balance among the nc gain cross sections, the optical mode losses of the waveguide structure, and the fast non radiative Auger processes. Within a four levels model we quantify the strong competition among all these processes and we obtain a satisfactory agreement with the experiments.
Silicon nanocrystals, formed by ion implantation and subsequent thermal annealing, show positive optical gain under intense laser excitation. Gain has been measured by the variable strip length method where the amplified spontaneous emission intensity, which is emitted from the sample edge, is measured as a function of the excitation volume. Exponential increase, line narrowing and directionality of stimulated emission have been measured. In addition, by growing silicon nanocrystals in a quartz substrate, single pass gain in pump and probe transmission experiments has been measured. Material gain values as high as those typically found in III-V semiconductors quantum dots have been measured. We claim that population inversion is realized between the fundamental and the recently identified Si equals O interface state. This model explains the gain observations and could account for the lack of auger saturation, free carrier absorption and size dispersion. Critical issues to obtain sizable gain are (1) high oxide quality, (2) high areal density of silicon nanocrystals, and (3) nanocrystals placed in the core region of a waveguide.
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