No abstract

High-energy metallic ions were implanted in silica matrices, obtaining spherical-like metallic nanoparticles (NPs) after a proper thermal treatment. These NPs were then deformed by irradiation with Si ions, obtaining an anisotropic metallic nanocomposite. An average large birefringence of 0.06 was measured for these materials in the 300-800 nm region. Besides, their third order nonlinear optical response was measured using self-diffraction and P-scan techniques at 532 nm with 26 ps pulses. By adjusting the incident light's polarization and the angular position of the nanocomposite, the measurements could be directly related to, at least, two of the three linear independent components of its third order susceptibility tensor, finding a large, but anisotropic, response of around 10(-7) esu with respect to other isotropic metallic systems. For the nonlinear optical absorption, we were able to shift from saturable to reverse saturable absorption depending on probing the Au NP's major or minor axes, respectively. This fact could be related to local field calculations and NP's electronic properties. For the nonlinear optical refraction, we passed from self-focusing to self-defocusing, when changing from Ag to Au.

We studied the absorptive and refractive nonlinearities at 532 nm and 26 ps pulses for silicon-nitride films containing silicon nanoclusters (nc-Si) prepared by remote plasma-enhanced chemical vapor deposition (RPECVD). Using a self-diffraction technique, we measured for the as-grown sample beta=7.7x10(-9)m/W, n(2)=1.8x10(-16)m(2)/W, and /chi(3)1111/ = 4.6x10(-10)esu; meanwhile, when the sample was exposed to an annealing process at 1000 degrees C during one hour in a nitrogen atmosphere, we obtained beta=-5x10(-10)m/W, n2=9x10(-17)m(2)/W, and /chi(3)1111/=1.1x10(-10)esu. A pure electronic nonlinear refraction was identified and a large threshold ablation of 41 J/cm(-2) was found for our films. By fitting nonlinear optical transmittance measurements, we were able to estimate that the annealed sample exhibits a response time close to 1 fs. We report an enhancement in the photoluminescence (PL) signal after the annealing process, as well as a red-shift due to an increment in size of the nc-Si during the thermal process.

The study of the third-order optical nonlinear response exhibited by a composite containing gold nanoparticles and silicon quantum dots nucleated by ion implantation in a high-purity silica matrix is presented. The nanocomposites were explored as an integrated configuration containing two different ion-implanted distributions. The time-resolved optical Kerr gate and z-scan techniques were conducted using 80 fs pulses at a 825 nm wavelength; while the nanosecond response was investigated by a vectorial two-wave mixing method at 532 nm with 1 ns pulses. An ultrafast purely electronic nonlinearity was associated to the optical Kerr effect for the femtosecond experiments, while a thermal effect was identified as the main mechanism responsible for the nonlinear optical refraction induced by nanosecond pulses. Comparative experimental tests for examining the contribution of the Au and Si distributions to the total third-order optical response were carried out. We consider that the additional defects generated by consecutive ion irradiations in the preparation of ion-implanted samples do not notably modify the off-resonance electronic optical nonlinearities; but they do result in an important change for near-resonant nanosecond third-order optical phenomena exhibited by the closely spaced nanoparticle distributions.

Silicon nanocrystals embedded in silicon nitride films were grown by direct plasma enhanced chemical vapor deposition at 300 degrees C, using mixtures of SiH2Cl2/NH3/H2/Ar. The films composition and chemical stability was tested by Fourier Transform Infrared Spectroscopy and Rutherford Backscattering Spectroscopy. The influence of hydrogen abundance during the deposition process on the photoluminescence of as-grown samples was studied as a function of the radiofrequency power and hydrogen dilution flow rate. In situ Optical Emission Spectroscopy allowed the diagnostic of the species in the plasma region and their general trends as a function of the radiofrequency power. The changes in the hydrogen content and silicon incorporation to the film as a function of the radiofrequency power were discussed in terms of silicon nanocrystals formation and growth in the silicon nitride matrix. The photoluminescence emission from the as-grown samples was found to red-shift with increasing hydrogen abundance. This observation is consistent with the increase in silicon content associated to nc-Si of larger size. On the other hand, the photoluminescence intensity was observed to decrease for very high radiofrequency powers and hydrogen dilutions. High Resolution Transmission Electron Microscopy confirmed the presence of silicon nanocrystals embedded in the amorphous silicon nitride matrix and allowed the correlation between the nanocrystals size and the photoluminescence emission energy using the quantum confinement model.