Thin films of metal-organic compounds and metal nanoparticle-embedded polymers for nonlinear optical applications

Thin films based on two very different metal-organic systems are developed and some nonlinear optical applications are explored. A family of zinc complexes which form perfectly polar assemblies in their crystalline state are found to organize as uniaxially oriented crystallites in vapor deposited thin films on glass substrate. Optical second harmonic generation from these films is investigated. A simple protocol is developed for thein-situ fabrication of highly monodisperse silver nanoparticles in a polymer film matrix. The methodology can be used to produce free-standing films. Optical limiting capability of the nanoparticle-embedded polymer film is demonstrated     

Proton beam writing of Nd:GGG crystals as new waveguide laser sources

Focused proton beam writing has been utilized to fabricate optical channel waveguides in Nd:GGG crystals. The 1?MeV proton beam irradiation creates a local modified region with positive refractive index changes at the end of the proton trajectory, in which the channel waveguide could confine the light field in a symmetric way. Room-temperature laser emission has been achieved at 1063.7?nm, with absorbed pump power of 61?mW (at 808?nm). The obtained slope efficiency of the Nd:GGG waveguide laser system is as high as 66%, which is, to our best knowledge, the highest value for integrated lasers from ion beam processed channel waveguide systems.     

Soft X‐ray absorption spectroscopy and resonant inelastic X‐ray scattering spectroscopy below 100 eV: probing first‐row transition‐metal M‐edges in chemical complexes

X‐ray absorption and scattering spectroscopies involving the 3d transition‐metal K‐ and L‐edges have a long history in studying inorganic and bioinorganic molecules. However, there have been very few studies using the M‐edges, which are below 100 eV. Synchrotron‐based X‐ray sources can have higher energy resolution at M‐edges. M‐edge X‐ray absorption spectroscopy (XAS) and resonant inelastic X‐ray scattering (RIXS) could therefore provide complementary information to K‐ and L‐edge spectroscopies. In this study, M_2,3‐edge XAS on several Co, Ni and Cu complexes are measured and their spectral information, such as chemical shifts and covalency effects, are analyzed and discussed. In addition, M_2,3‐edge RIXS on NiO, NiF₂ and two other covalent complexes have been performed and different d–d transition patterns have been observed. Although still preliminary, this work on 3d metal complexes demonstrates the potential to use M‐edge XAS and RIXS on more complicated 3d metal complexes in the future. The potential for using high‐sensitivity and high‐resolution superconducting tunnel junction X‐ray detectors below 100 eV is also illustrated and discussed.     

Electrophoresis of sheared polyelectrolytes

ABSTRACT

A shear flow breaks the spherical symmetry of a flexible polymer, which has some interesting consequences for the electrophoresis of polyelectrolytes. In addition to introducing a chain-length dependence of the electrophoretic velocity, there is also the possibility of migration of the molecule perpendicular to the direction of coaxial gradients in pressure and electric potential. This has been shown to produce a rapid and highly localised concentration of DNA within a microfluidic capillary, with a number of potential applications to on-chip preparation and analysis of genomic DNA. In this paper, dedicated to Prof. Daan Frenkel, I will describe a calculation of the electrophoretic motion of a long polyelectrolyte under a coaxial flow and electric field.     

Visualising many-body electron dynamics using one-body densities and orbitals

As experimental techniques begin to probe electronic motions in increasing detail, the need is arising for compact and informative visualisations of simulations of such processes. The inherent challenge is that a full many-electron wavefunction is a high-dimensional object, representing the complicated correlations of strongly repulsive bodies in a small molecular volume. A general procedure is needed to distill this to a smaller amount of information that does not rely on any specific level of approximation. The result should allow for easy and intuitive interpretation while drawing out nontrivial aspects of the underlying many-body dynamics, such as the complex phase information inherent of a nonstationary state. Current visualisation schemes based on physical observables or the qualitative information contained in simple wavefunctions, such as time-dependent configuration-interaction-singles (TD-CIS) and time-dependent self-consistent-field (TD-SCF), are discussed. This information is compared to an analysis based on the one-body reduced density operator (1-RDO), which is well-defined for general wavefunctions. It is seen that the distinction between two paradigms of many-body dynamics, electron transport and energy transport, is reflected in the coherences of a difference-1-RDO, or lack thereof.     

Power spectra and spatial pattern dynamics of a ring laser

Experimental measurements of power spectra of a single longitudinal and transverse mode ring dye laser are presented that reveal the critical slowing down of the laser near threshold. External pump noise serves as a probe of the frequency response of the dye laser. Detailed comparisons of the spectral characteristics with computer simulations and an approximate analytic theory are given. The dynamics of spatial pattern formation in a multimode dye laser is examined through measurements of first-passage-time distributions. A comparison of the experiments with computer simulations based on a simple theoretical model of the two-mode laser shows qualitative agreement. These measurements indicate that there are a variety of complex phenomena associated with the transverse mode pattern formation dynamics that need to be addressed theoretically and studied further experimentally.     

Binaural prediction of speech intelligibility in reverberant rooms with multiple noise sources

When speech is in competition with interfering sources in rooms, monaural indicators of intelligibility fail to take account of the listener's abilities to separate target speech from interfering sounds using the binaural system. In order to incorporate these segregation abilities and their susceptibility to reverberation, Lavandier and Culling [J. Acoust. Soc. Am. 127, 387-399 (2010)] proposed a model which combines effects of better-ear listening and binaural unmasking. A computationally efficient version of this model is evaluated here under more realistic conditions that include head shadow, multiple stationary noise sources, and real-room acoustics. Three experiments are presented in which speech reception thresholds were measured in the presence of one to three interferers using real-room listening over headphones, simulated by convolving anechoic stimuli with binaural room impulse-responses measured with dummy-head transducers in five rooms. Without fitting any parameter of the model, there was close correspondence between measured and predicted differences in threshold across all tested conditions. The model's components of better-ear listening and binaural unmasking were validated both in isolation and in combination. The computational efficiency of this prediction method allows the generation of complex "intelligibility maps" from room designs.