Ad-hoc design of temporally shaped fs laser pulses based on plasma dynamics for deep ablation in fused silica

We have analyzed the ablation depth yield of fused silica irradiated with shaped pulse trains with a separation of 500 fs and increasing or decreasing intensity envelopes. This temporal separation value is extracted from previous studies on ablation dynamics upon irradiation with transform-limited 100 fs laser pulses. The use of decreasing intensity pulse trains leads to a strong increase of the induced ablation depth when compared to the behavior, at the same pulse fluence, of intensity increasing pulse trains. In addition, we have studied the material response under stretched (500 fs, FWHM) and transform-limited (100 fs, FWHM) pulses, for which avalanche or multiphoton ionization respectively dominates the carrier generation process. The comparison of the corresponding evolution of the ablated depth vs. fluence suggests that the use of pulse trains with decreasing intensity at high fluences should lead to enhanced single exposure ablation depths, beyond the limits corresponding to MPI- or AI-alone dominated processes.     

Reversible and Irreversible Chemisorption in Nonporous‐Crystalline Hybrids

The tools of synthetic chemistry allow us to fine‐tune the reactivity of molecules at a level of precision not yet accessible with inorganic solids. We have investigated hybrids that couple molecules to the superior thermal and mechanical properties of solids. Herein we present, to the best of our knowledge, the first demonstration of reactivity between hybrid perovskites and substrates. Reaction with iodine vapor results in a remarkable expansion of these materials (up to 36 % in volume) where new covalent C? I bonds are formed with retention of crystallinity. These hybrids also show unusual examples of reversible chemisorption. Here, solid‐state interactions extend the lifetime of molecules that cannot be isolated in solution. We have tuned the half‐lives of the iodinated structures from 3 h to 3 days. These nonporous hybrids drive substrate capture and controlled release through chemical reactivity. We illustrate the strengths of the hybrid by considering radioactive iodine capture.     

Optical contrast by laser-induced phase changes: Real time optical measurement of fast transformation times

Real time optical measurements are used to analyse two different kinds of phase changes which generate optical contrast in (In₄₃Sb₅₇)₈₇Ge₁₃ thin films. Amorphous to crystalline and amorphous to amorphous structural transformations are induced by pulsed laser irradiation in micron-sized regions. A two beam configuration is used to follow the evolution of the optical properties of the films in real time. It is shown that real time optical measurements provide a unique tool to analyse laser-induced fast structural transformations leading to optical contrast. Processes occurring via relaxation, solid state crystallization or melting-solidification are clearly distinguished. From the analysis of the optical transients the minimum transformation times are directly determined.On Sabbatical leave from IBM Almaden Research Center, San Jose, CA, USA     

Discretizations of nonlinear differential equations using explicit finite order methods

In this work we study the appearance of spurious solutions when first-order differential equations with unimodal right-hand sides are discretized using Runge-Kutta schemes. These spurious solutions are explained in terms of the iteration functions. Schemes that produce good approximating solutions for much longer times are given.     

The influence of the ethanol-water molar ratio in the precursor solution on morphology and photocatalytic activity of pyrolytic ZnO films

Zinc oxide films were fabricated by a homemade spray pyrolysis system equipped with an optical setup ensuring the in situ control of the film growth. Zinc acetate (0.1 M) diluted in a mixture of ethanol and water was used as the precursor solution. The ethanol-water molar ratio, gamma, in the precursor solution was varied from 0 to 0.92. The deposition temperature and the pH of the precursor solution were kept at 350 degrees C and 4.5, respectively. X-ray diffraction patterns revealed that films were zincitelike with a grain size depending on the ethanol-water molar ratio in the precursor solution. The interference pattern obtained during film deposition was used to monitor the film roughness; it was found that this is related with those results of surfaces and optical analysis obtained by scanning electron microscopy and spectrophotometric measurements, respectively. The morphology of the ZnO films obtained from gamma equal to either 0 or 0.92 are dense with agglomerates uniformly distributed, whereas the films obtained from gamma equal to either 0.03 or 0.06 are very rough with irregular agglomerates. The films obtained from gamma equal to 0.12, 0.18 and 0.31 are rough. Photoelectrocatalytic results indicated that there is a correlation of the partial molar volume of ethanol with respect to water in the spraying solution, with the photocatalytic efficiency of the ZnO films. We found that the maximum photodegradation of methyl orange in the solution occurs using ZnO films obtained with gamma = 0.12.     

Dye-sensitized solar cells based on nanocrystalline TiO2 films surface treated with Al3+ ions: photovoltage and electron transport studies

Nanocrystalline TiO2 films, surface modified with Al3+, were manufactured by depositing a TiO2 suspension containing small amounts of aluminum nitrate or aluminum chloride onto conducting glass substrates, followed by drying, compression, and finally heating to 530 degrees C. Electrodes prepared with TiO2 nanoparticles coated with less than 0.3 wt % aluminum oxide with respect to TiO2 improved the efficiency of the dye sensitized solar cell. This amount corresponds to less than a monolayer of aluminum oxide. Thus, the Al ions terminate the TiO2 surface rather than form a distinct aluminum oxide layer. The aluminum ion surface treatment affects the solar cell in different ways: the potential of the conduction band is shifted, the electron lifetime is increased, and the electron transport is slower when aluminum ions are present between interconnected TiO2 particles.     

Chain-length dependent nematic ordering of conjugated polymers in a liquid crystal solvent

In this communication we demonstrate the dependence of the solute order parameter on the solute molecular weight for polymer solutes dissolved in liquid crystalline solvents. Using ensemble absorption polarization spectroscopy together with single molecule fluorescence polarization measurements, we have determined the order parameter of the conjugated polymer MEH-PPV (poly[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene vinylene]) in the liquid crystal 5CB (4-cyano-4-n-pentylbiphenyl) as a function of polymer chain length. Ensemble absorption polarization measurements agree well with results obtained by single molecule fluorescence polarization spectroscopy, indicating a large-scale ordering of the MEH-PPV solute in 5CB. These results demonstrate that the increasing number of defects for larger polymer weights inherently limits the alignment of the polymer solute.     

Threshold intensity and coefficient of raman scattering amplification in a high-<Emphasis Type="Italic">Q</Emphasis> bilayer microresonator during the formation of internal and external submicron photonic jets: A photonic nanojet in the near field

Using quantum and semiclassical approaches, the energy excitation threshold for induced Raman scattering is estimated and a relationship between the excitation threshold and the concentration of optically active molecules in a bilayer microresonator is established. Estimates are made during the formation of specially configured optical fields: internal and external photonic nanojets. Based on the amount of stored energy per mode and the value of the threshold intensity, an additional generalized selection rule for whispering gallery modes is suggested. It is shown that the bilayer microresonator can focus incident radiation (laser pumping) into a submicron focal volume at a low threshold intensity.     

Dynamical properties of families of discrete delay advection–reaction operators

A family of discrete delay advection–reaction operators is introduced along with an infinite matrix formulation in order to investigate the asymptotic behaviour of the orbits of their iterates. The infinite matrices obtained are triangular matrices with only one non-zero subdiagonal. We show that the elements of powers of these matrices can be written as distinctive products of two factors, one of them involving derivatives of the Lagrange polynomials of basic functions with the diagonal elements as nodes. The other factor consists of products of the subdiagonal elements. Consequently the convergence of the iterates of the operators depends on their eigenvalues and the products of their subdiagonal elements.