Strong nonlinear absorption is observed in nanocomposite films containing PbS nanocrystals of mean size of 3.3 nm stabilized in a commercial poly(vinyl acetate) glue by a novel and simple chemical route of synthesis. A significant blueshift of the optical absorption edge indicates strong quantum confinement. The mean nanocrystal size was characterized by x-ray diffraction and transmission electron microscopy. The surface structure of nanocrystals is analysed using infrared spectroscopy. The excitonic transitions are probed by photoacoustic spectroscopy and the results are analysed on the basis of theoretical calculations using envelope function formalism. Results of open aperture z-scan experiments suggest a model involving saturable absorption followed by two-photon absorption at a lower concentration while the data for a higher concentration fitted saturable absorption followed by three-photon absorption. Free carrier absorption due to two-photon-assisted excited state absorption appears to be the predominant mechanism of optical nonlinearity.
Stable films containing CdS quantum dots of mean size 3.4 nm embedded in a solid host matrix are prepared using a room temperature chemical route of synthesis. CdS/synthetic glue nanocomposites are characterized using high resolution transmission electron microscopy, infrared spectroscopy, differential scanning calorimetry and thermogravimetric analysis. Significant blue shift from the bulk absorption edge is observed in optical absorption as well as photoacoustic spectra indicating strong quantum confinement. The exciton transitions are better resolved in photoacoustic spectroscopy compared to optical absorption spectroscopy. We assign the first four bands observed in photoacoustic spectroscopy to 1se–1sh, 1pe–1ph, 1de–1dhand 2pe–2phtransitions using a non interacting particle model. Nonlinear absorption studies are done using z-scan technique with nanosecond pulses in the off resonant regime. The origin of optical limiting is predominantly two photon absorption mechanism.
We demonstrate the use of stable films containing PbS nanocrystals as media for self-adaptive phase filtering in phase contrast imaging of transparent objects by a cost-effective exploitation of nonlinear optical refraction in a simple, all-optical, and self-adjusting 4f imaging system. The optical nonlinearity is characterized by z-scan technique using a continuous wave He-Ne laser as the excitation source. The mechanism of nonlinearity in this case is mainly due to the nonlocal thermo-optical interaction between the laser beam and the sample. The value of nonlinear refractive index coefficient is found to be -3.5x10(-7) cm(2)/W. The nanocomposite material shows a thermal lens effect and is a potential candidate for phase contrast imaging.
Devices based on optical technology for high speed communication networks require materials with large nonlinear optical response in the ultrafast regime. Nonlinear optical materials have also attracted wide attention as potential candidates for the protection of optical sensors and eyes while handling lasers. Optical limiters have a constant transmittance at low input influence and a decrease in transmittance at higher fluences and are based on a variety of mechanisms such as nonlinear refraction, nonlinear scattering, multiphoton absorption and free carrier absorption. As we go from bulk to nanosized materials especially in the strong quantum confinement regime where radius of the nanoparticle is less than the bulk exciton Bohr radius, the optical nonlinearity is enhanced due to quantum confinement effect. This paper is on the ultrafast nonresonant nonlinearity in free standing films of PbS quantum dots stabilized in a synthetic glue matrix by a simple chemical route which provides flexibility of processing in a variety of physical forms. Optical absorption spectrum shows significant blue shift from the bulk absorption onset indicating strong quantum confinement. PbS quantumdots of mean size 3.3nm are characterized by X-ray diffraction and transmission electron microscopy. The mechanism of nonlinear absorption giving rise to optical limiting is probed using open z-scan technique with laser pulses of 150 fs pulse duration at 780 nm and the results are presented in the nonresonant femtosecond regime. Irradiance dependence on nonlinear absorption are discussed. KeywordsPbS quantum dots; femtosecond z-scan; non resonant optical nonlinearity; optical limiting 1.INTRODUCTIONBoth the linear and nonlinear optical properties of semiconductor nanocrystals are known to differ appreciably from those of the bulk semiconductor 1,2 , particularly in the regime of strong quantum confinement, when the cluster sizes are below a critical size called bulk exciton Bohr radius. In this regime, the bulk semiconductor energy bands are split into discrete energy levels with an increase in the effective bandgap. Materials with large optical nonlinearities have immense potential in various photonics device applications like optical switching and optical limiting. This has led to a lot of interest in exploring the linear as well as nonlinear optical processes and mechanisms in these materials. PbS is a direct band gap material with bulk bandgap of 0.41eV and exciton bohr radius of 9nm.
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