Plasmon-enhanced multi-photon excited photoluminescence of Au, Ag, and Pt nanoclusters.

In this work, we have studied the multi-photon excited photoluminescence from metal nanoclusters (NCs) of Au, Ag and Pt embedded in Al2O3matrix by ion implantation. The thermal annealing process allows to obtain a system composed of larger plasmonic metal nanoparticles (NPs) surrounded by photoluminescent ultra-small metal NCs. By exciting at 1064 nm, visible emission, ranging from 450 to 800 nm, was detected. The second and fourth-order nature of the multiphoton process was verified in a power-dependent study measured for each sample below the damage threshold. Experiments show that Au and Ag NCs exhibit a four-fold enhanced multiphoton excited photoluminescence with respect to that observed for Pt NCs, which can be explained as a result of a plasmon-mediated near-field process that is of less intensity for Pt NPs. These findings provide new opportunities to combine plasmonic nanoparticles and photoluminescent nanoclusters inside a robust inorganic matrix to improve their optical properties. Plasmon-enhanced multiphoton excited photoluminescence from metal nanoclusters may find potential application as ultrasmall fluorophores in multiphoton sensing, and in the development of solar cells with highly efficient energy conversion modules.

Tuning the aspect ratio of silver nanospheroids embedded in silica: erratum.

We present a corrigendum to our Letter [Opt. Lett.35, 703 (2010)10.1364/OL.35.000703]. In the original Letter we inadvertently included in Fig. 2(a) a TEM micrograph corresponding to a different, but very similar, sample. This corrigendum replaces Fig. 2(a) with a correct version. Since the main results are rather based in optical absorption measurements, and their modeling by using the T-matrix method, this correction does not affect the results and conclusions of the original Letter.

Third order nonlinear optics in Ag nanocubes: local and nonlocal optical responses as a function of excitation wavelength and particle size.

Colloidal silver nanocubes in solution were analyzed by the Z-scan technique in the resonant and non-resonant regimes. Three different systems with particle sizes of 56, 99 and 215 nm, and concentrations of 0.378, 0.831 and 0.715 mg/mL, respectively, were obtained by the polyol method. Nonlinear excitation of the samples was performed with laser pulses of 26 ps, at a repetition rate of 10 Hz, and using three different wavelenghts (355, 532 and 1064 nm), exciting only the electronic part of the optical nonlinearity, and avoiding induced thermal loading of the samples. Whenever observable, samples showed saturable absorption for all wavelengths, which was dependent, in general, on concentration and incident intensity. For samples featuring sizes of 55 and 99 nm, saturable absorption could be observed for wavelengths close to their dipolar surface plasmon resonances; while, for samples with sizes of 99 and 215 nm, saturable absorption and positive nonlinear optical refraction (only for size of 215 nm) could be observed at 1064 nm. Besides, for some samples, nonlinear optical response followed the incident intensity profile at wavelengths close to resonance. On the contrary, for wavelengths out of resonance, the nonlinear optical behavior showed to be nonlocal, ie, its profile was narrower than the incident one.

Third-order nonlinear optical properties of colloidal Au nanorods systems: saturable and reverse-saturable absorption.

In this work, we present a study of the nonlinear absorption properties from different gold nanorod (NR) systems in aqueous suspension. The NRs were obtained with the bottom-up protocol by the seed-mediated growth method (SMG), using Ag(+) ions at different concentrations, and CTAB as surfactant. By using this method, aspect ratios between 2 and 5 were obtained. The transverse surface plasmons (TSP) are located between 514 - 535 nm, while the longitudinal surface plasmons (LSP) are between 639 - 921 nm, for the different samples studied. The Z-scan technique was implemented for open (OA) and closed (CA) aperture at 532 and 1064 nm, with laser pulses of 26 ps, for vertical and horizontal polarizations, with respect to the incidence plane (horizontal). At 532 nm all samples showed saturable absorption (SA), while for samples with LSP near 1064 nm, such effect was observed only at low-energy pulse experimental conditions. In the high-energy pulse regime, an apparent reverse-saturable absorption (RSA) was observed for both wavelengths. However for 532 nm, it was possible to determine that this effect results from structural changes in the samples, which are manifested through the behavior of nonlinear absorption and refraction curves. These results were used to determine the irradiances to which NRs can be modified by photodegradation.

Modulation of the propagation speed of mechanical waves in silicon quantum dots embedded in a silicon-nitride film.

Using a vectorial picosecond self-diffraction method, we evaluate the modification of the speed of the sound in a silicon-nitride film containing silicon quantum dots prepared by remote plasma-enhanced chemical vapor deposition. Our non-contact technique is based on the stimulation of the electrostriction contribution to the nonlinearity of index exhibited by the sample in a multiwave mixing laser experiment. We identified the electronic birefringence using two of the incident beams to generate a self-diffraction signal, then, we modified the third order nonlinear response by means of the optical Kerr effect given by a phase-mismatched third beam which induced electrostriction. Our results indicated that the speed of the sound in a silicon-nitride film can be simultaneously tailored by an electronic nonlinear refractive index, and by an electrostriction effect, both resulting from silicon quantum dots doping.

Ultrafast optical phase modulation with metallic nanoparticles in ion-implanted bilayer silica.

The nonlinear optical response of metallic-nanoparticle-containing composites was studied with picosecond and femtosecond pulses. Two different types of nanocomposites were prepared by an ion-implantation process, one containing Au nanoparticles (NPs) and the other Ag NPs. In order to measure the optical nonlinearities, we used a picosecond self-diffraction experiment and the femtosecond time-resolved optical Kerr gate technique. In both cases, electronic polarization and saturated absorption were identified as the physical mechanisms responsible for the picosecond third-order nonlinear response for a near-resonant 532 nm excitation. In contrast, a purely electronic nonlinearity was detected at 830 nm with non-resonant 80 fs pulses. Regarding the nonlinear optical refractive behavior, the Au nanocomposite presented a self-defocusing effect, while the Ag one presented the opposite, that is, a self-focusing response. But, when evaluating the simultaneous contributions when the samples are tested as a multilayer sample (silica-Au NPs-silica-Ag NPs-silica), we were able to obtain optical phase modulation of ultra-short laser pulses, as a result of a significant optical Kerr effect present in these nanocomposites. This allowed us to implement an ultrafast all-optical phase modulator device by using a combination of two different metallic ion-implanted silica samples. This control of the optical phase is a consequence of the separate excitation of the nonlinear refracting phenomena exhibited by the separate Au and Ag nanocomposites.

Anomalous patterned scattering spectra of one-dimensional porous silicon photonic crystals.

Far-field secondary emission spectra of one-dimensional periodic photonic structures based on porous silicon show characteristic co-focal rings centered close to the structure plane normal. The rings appear when the frequency of picosecond excitation laser pulses is tuned to the edges of the fourth photonic band gap. They can be clearly distinguished from the typical reflected and transmitted light in the oblique incidence geometry. The rings number is dependent on the excitation frequency and the incidence angle. We explain these anomalous spectral features of porous silicon structures by the spectral filtering of light elastically scattered inside the photonic structure by the narrow photonic bands. The elastic scattering of light due to the photonic disorder in the structure causes the appearance of secondary waves propagating in any direction. But only those waves which fall into the allowed photonic bands penetrate through the whole structure and move through its front or back surfaces. The observed patterned secondary emission is an example of efficient photonic engineering by simple means of multilayer porous silicon structures.

Inhibition of the two-photon absorption response exhibited by a bilayer TiO2 film with embedded Au nanoparticles.

We use two different synthesis approaches for the preparation of TiO(2) films in order to study their resulting third order optical nonlinearity, and its modification by the inclusion of Au nanoparticles in one of the samples. An ultrasonic spray pyrolysis method was used for preparing a TiO(2) film in which we found two-photon absorption as a dominant nonlinear effect for 532 nm and 26 ps pulses; and a purely electronic nonlinearity at 830 nm for 80 fs pulses. A strong optical Kerr effect and the inhibition of the nonlinear optical absorption in 532 nm can be obtained for the first sample if Au nanoparticles embedded in a second TiO(2) film prepared by a sol-gel technique are added to it. We used an optical Kerr gate, z-scan, a multi-wave mixing experiment and an input-output transmittance experiment for measuring the optical nonlinearities.

Tuning the aspect ratio of silver nanospheroids embedded in silica.

A method is proposed to control the aspect ratio (epsilon) of elongated nanoparticles obtained by ion implantation in a transparent matrix. The procedure was tested for Ag spheroids in silica and we could accurately change epsilon in the range from the maximum value obtained by the ion implantation (around 3.0 in this case) to 1.0 (spherical shape). The values of epsilon were determined in several steps from optical extinction spectroscopy measurements, by fitting the modification and splitting of the surface plasmon resonance peak, using the T-matrix method. In the initial (maximum deformation) and final (undeformed) states, transmission electron microscopy images were obtained, showing a good agreement with the T-matrix results in both cases.

Modification of the nonlinear optical absorption and optical Kerr response exhibited by nc-Si embedded in a silicon-nitride film.

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.