Spontaneous pattern formation due to modulation instability of incoherent white light in a photopolymerizable medium

Spontaneous pattern formation due to modulation instability was observed in a broad uniform beam of incoherent white light propagating in an optically isotropic, photopolymerizable organosiloxane. Pattern formation originates from intensity-dependent refractive index changes due to polymerization, which cause competition between the natural diffraction (broadening) and self-induced refraction of the beam. Under these nonlinear conditions, weak intensity modulations in the beam, noise, that would be negligible under linear conditions are amplified. The amplified patterns become unstable over time and spontaneously divide into individual self-trapped filaments of white light of essentially identical diameter (76 +/- 3 microm), which propagate through the medium without diffracting. In the case of noise with a weak 1-D periodic modulation, for example, the uniform beam transformed into a 1-D periodic array of self-trapped lamellae, which in turn formed a 2-D array of self-trapped cylindrical filaments. Although the rate of pattern formation varied inversely with optical power (measured from 8.4 to 59.8 mW), the uniform beam always split into discrete filaments, demonstrating that they are the most stable form of light propagation under the nonlinear conditions created by polymerization. Each filament of light retained the spectral composition and incoherence of white light, which showed that the entire polychromatic, incoherent and unpolarized wavepacket collectively participated in pattern formation. These findings are consistent with recent theoretical models of nonlinear white light propagation and with experimental observations of pattern formation in coherent and partially coherent light. Because refractive index changes due to polymerization are permanent, pattern formation imparts microstructure to the organosiloxane. Optical micrographs revealed that, after pattern formation, the initially homogeneous medium consisted entirely of a closely packed array of narrow channel waveguides induced by self-trapped filaments.     

The dynamics of self-trapped beams of incoherent white light in a free-radical photopolymerizable medium

Detailed experimental studies of the dynamics of self-trapped beams of white light (400-800 nm) in a photosensitive organosiloxane medium are presented. Self-trapped white light beams with similar spatial profiles formed in the organosiloxane at intensities ranging across an order of magnitude (2.7-22.0 W.cm-2). Beam-profiling measurements showed that these spatially and temporally incoherent wave packets propagate without diffracting (broadening) by initiating free-radical polymerization of methacrylate groups and corresponding refractive index changes in the organosiloxane medium. Analyses of their temporal evolution showed that the intensity-dependent behavior of self-trapped white light is similar to that of self-trapped laser light despite the extreme differences in their phase structure and chromaticity; the self-trapped incoherent beams even show the complementary oscillations of width and intensity that is characteristic of self-trapped coherent light. Furthermore, the dynamics of the self-trapped white light beams was found to be strongly correlated to the kinetics of free-radical polymerization and corresponding rates of refractive index changes in the organosiloxane. These studies provide accessible photochemical routes to self-trapped incoherent wave packets, which are extremely difficult to generate in conventional nonlinear optical media that owe their responses to higher-order dielectric susceptibility tensors. This could enable the experimental verification of theoretical models developed for the nonlinear propagation of white light and stimulate research into more complex self-trapping phenomena such as the interactions of self-trapped incoherent beams and spontaneous pattern formation due to modulation instability in a uniform incoherent optical field. These findings also carry potential for the development of self-induced waveguide, optical solder and interconnect technology for incoherent light emitted by incandescent sources or LEDs.     

Self-trapping of spatially and temporally incoherent white light in a photochemical medium

We report that a beam of spatially and temporally incoherent white light self-traps by initiating free-radical polymerization in an organosiloxane medium. Refractive index changes due to polymerization lead to the formation of a narrow channel waveguide that traps and guides the entire multimode, broadband beam without diffraction. The response time of the system, which is determined by the inherently slow rate of free-radical polymerization, exceeds by several orders of magnitude the femtosecond-scale random phase fluctuations that characterize white light. Self-trapping of incoherent light is possible in the photochemical medium because it responds to the time-averaged intensity profile of the white light beam.     

Epoxy-based Polymer Containing Imidazole-type Azo Chromophores for Integrated Waveguide Applications

In this work, an epoxy-based polymer containing 2-phenylazo-4, 5-dicyanoimidazole chromophores (BP-IZ-DC) was synthesized and characterized by spectroscopic methods. The polymer showed unusual photo-bleachable property and the refractive index of the polymer could be readily modified by irradiation with a laser beam at visible wavelength. The irradiation with a laser beam at 488 nm caused a much more significant change of the refractive index than irradiation with 532 nm laser light. Upon the irradiation with the laser beam (488 nm, 100 mW/cm²) for 1 h, the refractive index decreased from 1.6512 to 1.5802. By using the photo-bleachable azo polymer, channel waveguide was fabricated by light irradiation through a mask and the light-transmission ability of the waveguide was evaluated.     

Doped colloidal photonic crystal structure with refractive index chirping to the [111] crystallographic axis

A three-dimensionally ordered array of close-packed colloidal spheres, a photonic crystal structure in which the refractive index of the medium interstitial lattice in a colloidal crystal spatially changes in the [111] crystallographic axis, is demonstrated. The colloidal photonic crystal structure with refractive index chirping was produced by infiltration of a monomer and organic dopants with a high refractive index into a silica opal, followed by interfacial gel polymerization. The resulting photonic crystal structure has a gradually varying stop band at each different (111) plane in the face-centered cubic (fcc) crystal structure at a normal incidence. This novel structure exhibited optical characteristics that have band-gap broadening by the superposition of stop bands at each plane of the crystal with different dielectric functions. Moreover, the refractive index perturbation in the [111] fcc opal also showed a defect state within a pseudo-photonic band gap. This new type of photonic crystal structure should be useful for the band-gap engineering of photonic-band-gap materials.     

Large Photoinduced Refractive Index Change in a Polyimide Film by Charge‐Transfer Complex Formation with a Polymer‐Bound Phenylazide Fragment

A large photo‐induced refractive index change as large as 0.014 at 632.8 nm in thermostable transparent polymer films has been realized for the first time by using photoirradiation of polyimide precursor films containing a phenylazide and successive imidization. The phenylazide fragment forms a charge‐transfer complex with imide moiety. The films maintained high transmittance in a wide visible region in contrast to usual polyimide films. This value of refractive index change is sufficient to make thermostable channel waveguides and other optical devices.     

ADDITIVE-INDUCED ENHANCEMENT OF OPTICAL CLARITY OF POLYACRYLAMIDE HYDROGEL

The aqueous polymerization of acrylamide and crosslinking with N,N-methylenebisacrylamide afforded hydrogelsdisplaying high levels of light scattering (poor optical clarity). Enhancement of the optical clarity within a polyacrylamide(PAm) hydrogel was accomplished through the implementation of "refractive index matching". Water-soluble additives wereutilised to better match the refractive index inhomogeneities throughout a given hydrogel. This resulted in lower lightscattering within the system and hence improved clarity. Amino acids, sugars, polymers, and other water-soluble additivessuch as glycerol were investigated by this methodology. Most additives investigaed displayed potential for effectivelyreducing the light scattering within a PAm hydrogel as a function of increased additive concentration. On increasing therefractive index of the water medium, the overall refractive index of a PAm hydrogel was also observed to increase. Thisprovided a quantitative means of determining the effectiveness of a given additive for improving the optical clarity within ahydrogel.     

Synthesis of silyl-functionalized oligothiophene-based polymers with bright blue light-emission and high refractive index

In this paper, we report the synthesis of partially conjugated polymers with a silyl-group-substituted oligothiophene and a short alkyl chain in the main chain by hydrosilylation polymerization and describe their optical properties such as luminescence and refractive index. The obtained polymers are found to have good solubility and processability. Moreover, the high steric hindrance of the silyl-group can inhibit the π-π interaction and intermolecular aggregation of the polymers. Hence, the emission of the obtained polymers was similar to that of the corresponding silyl-group-substituted oligothiophene. The polymers exhibit intense light blue fluorescence under UV irradiation and a high refractive index in the visible light region.     

Responsive photonic crystal for the sensing of environmental pollutants

This review covers the concepts of photonic crystal (PhC) and its usage for the sensing of environmental pollutants. PhCs are composed of periodic and ordered nanostructures which can manipulate the diffraction or reflection of light propagation through the structures. If the light spectra locate in the visible range, the color of materials can be observed by naked eye. The optical properties of PhCs are determined by the lattice constant of the crystal or by the refractive index contrast between the colloids and the surrounding medium. Based on these features, responsive PhCs can be designed to detect the environmental pollutants. In this review, we primarily described the photonic crystals for the sensing of volatile organic compounds (VOCs), organophosphates (OPs), heavy metal ions and endocrine disrupting chemicals (EDCs), and these sensors exhibited excellent sensitivity and are promising for the on-site monitoring of pollutants.     

Noninvasive picoliter volume thermometry based on backscatter interferometry

Using the on-chip refractive index (RI) detector based on backscatter interferometry, sensitive, small volume, noninvasive thermometry can be performed. The current optical configuration for the on-chip interferometric backscatter detector (OCIBD) is quite simple and consists of an unfocused laser, an unaltered chip with a hemispherical channel and a photodetector. Alignment is straightforward with the only requirement being that the beam fully fills the channel. The interaction of an unfocused laser beam with the uncoated etched channel with a curvature within the silica plate (chip) produces fringes whose positional changes scale with respect to the refractive index (RI), n, of the fluid in the channel. Due to the inherently high value of dn/dT for most fluids and the high sensitivity of OCIBD to RI changes, the measurement of small temperature variations in sub-nanoliter volumes is possible. Performing OCIBD with a 75 microm diameter laser beam on a silica chip that contains an etched channel with a 40 microm radius facilitates noninvasive thermometry on a N-(2-hydroxyethyl)piperazine-(2-ethanesulfonic acid) (HEPES) solution in a 188 x 10(-12) L probe volume with a temperature resolution of 9.9 x 10(-4) degrees C, at the 99% confidence level.     

A chip-scale universal detector for electrophoresis based on backscattering interferometry

An on-chip detector based on backscatter interferometry has been developed to perform sub-nanoliter volume refractive index measurements. The detection system consists of a simple, folded optical train based on the interaction of a laser beam and an etched channel in a silica (glass) plate. This etched channel is composed of two radii joined by a flat portion which define a curved surface in the shape of a half cylinder in a silica (glass) plate. The backscattered light from the channel takes on the form of a high contrast interference pattern that contains information related to the bulk properties of the fluid located within the probe volume. Positional changes of the interference pattern extrema (fringes) allow for the determination of refractive index changes at the 10(-6) level in a detection volume of 188 x 10(-12) L. Under capillary electrophoresis (CE) conditions, the injected mass detection limits for small molecules with little native absorption ranges from 530 fmol (0.18 ng) for sucrose to 720 fmol (0.43 nanograms) for raffinose. Fluorescein was also used to evaluate the technique for universal CE and under further optimized conditions can be quantified at the 150 microM level. Separation performance for the solutes tested ranged from about 2300 to 15,500 plates or 61,000 to 400,000 N m-1. The results presented here indicate there is potential for using the simple optical train of backscattering interferometry for on-chip universal solute analysis.     

Design of new integrated optical substrates for immuno-analytical applications

Integrated optical Mach-Zehnder interferometers supply information on changes in refractive index and/or thickness of a film placed as a superstrate on top of one of its surface wave-guides. The internal propagation of light is influenced by the evanescent field reaching into the superstrate. This propagating light interferes with an uninfluenced wave in the second arm after recombination. The result is an intensity modulation depending on the refractive index parameters of the substrate, the waveguide itself and the properties of the superstrate. Taking an antigen layer as the superstrate, its interaction with antibodies changes its thickness by several nanometers. This can be observed by recording the change in intensity of the signal of the interferometer. The sensitivity of such a device depends on particular values of the optical parameters of substrate and waveguide with respect to the given superstrate properties. Computer calculations help to select optimum glass and waveguide fabrication conditions. The numerical results of a variety of assumed conditions have been tested experimentally. The application to the improved detection of triazines is discussed.     

Fluorescent liquid-core/air-cladding waveguides towards integrated optofluidic light sources

We have demonstrated fluorescent liquid-core/air-cladding (LA) waveguides suitable for use as integrated optofluidic light sources. These waveguides were fabricated by conventional soft lithography using poly(dimethylsiloxane) (PDMS). Two-phase stratified flows of air and ethylene glycol with fluorescent dye were generated along the PDMS channel. Compared to the liquid-core/liquid-cladding (L(2)) waveguide, the larger refractive index contrast of the LA waveguide resulted in stronger optical confinement. Specifically, the larger refractive index contrast led to experimentally achievable captured fractions (the amount of light to be coupled into the liquid core) as high as 22.8% and the measured propagation losses as low as 0.14 dB cm(-1). Furthermore, in our LA waveguides, diffusional mixing of the core and cladding fluids did not occur and the size of the core stream could be reversibly tuned simply by adjusting the flow rates of the two contiguous phases.     

Optical imaging in tissue with X-ray excited luminescent sensors

We report a high-spatial resolution imaging technique to measure optical absorption and detect chemical and physical changes on surfaces embedded in thick tissue. Developing sensors to measure chemical concentrations on implanted surfaces through tissue is an important challenge for analytical chemistry and biomedical imaging. Tissue scattering dramatically reduces the resolution of optical imaging. In contrast, X-rays provide high spatial resolution imaging through tissue but do not measure chemical concentrations. We describe a hybrid technique which uses a scanning X-ray beam to irradiate Gd(2)O(2)S scintillators and detect the resulting visible luminescence through the tissue. The amount of light collected is modulated by optical absorption in close proximity to the luminescence source. By scanning the X-ray beam, and measuring total amount of light collected, one can measure the local absorption near scintillators at a resolution limited by the width of luminescence source (i.e. the width of the X-ray excitation beam). For proof of principle, a rectangular 1.7 mm scanning X-ray beam was used to excite a single layer of 8 μm Gd(2)O(2)S particles, and detect the absorption of 5 nm thick silver island film through 10 mm of pork. Lifetime and spectroscopic measurements, as well changing the refractive index of the surroundings indicate that the silver reduces the optical signal through attenuated total internal reflection. The technique was used to image the dissolution of regions of the silver island film which were exposed to 1 mM of H(2)O(2) through 1 cm of pork tissue.     

Dynamically reconfigurable liquid-core liquid-cladding lens in a microfluidic channel

This paper describes the design and operation of a liquid-core liquid-cladding (L(2)) lens formed by the laminar flow of three streams of liquids in a microchannel whose width expands laterally in the region where the lens forms. Two streams of liquid with a lower refractive index (the cladding) sandwich a stream of liquid with a higher refractive index (the core). As the core stream enters the expansion chamber, it widens and becomes biconvex in shape, for some rates of flow. This biconvex fluidic element focuses light. Manipulating the relative rates of flow of the streams reconfigures the shape, and therefore the focal distance, of the L(2) lens. This paper also describes a technique for beam tracing, and for characterization of a lens in an enclosed micro-scale optical system. The use of a cladding liquid with refractive index matched to that of the material used in the fabrication of the microfluidic system (here, poly(dimethylsiloxane)) improves the quality of the focused beam.     

Photochemically-induced refractive index and fluoresence patterning on polymer films

The molecular design for large photo-induced refractive index changes in transparent visible light region was proposed and realized with norbornadiene polymers and poly(vinyl cinnamate). The patterning of pure refractive-index contract on their transparent films was made with near-field scanning optical microscopy (NSOM). Reversible fluorescence patterning on polymer films is also presented by using controlled energy transfer from a fluorescent pyromethene to a photochromic diarylethene.     

Observation of spatial distribution of laser-induced refractive index change in dye-doped liquid crystals

Spatial distributions of photothermal refractive index changes in dye-doped liquid crystals were determined by an optical interferometric method. The refractive index change of the order of 10^-1, including spatial distribution, was estimated by the described experimental technique. The absolute value of the refractive index change was proportional to the pump beam power, and the diameter of the index distribution was slightly larger than that of the pump laser beam due to heat conduction.     

含硫高折射率光学树脂合成及性能研究进展

作为无机玻璃的替代品,有机光学树脂具有轻质、抗冲击性好、易加工和可调性强等优点。折射率是光学树脂的主要参数之一,折射率的高低可直接影响成品镜片的厚度、美观性和舒适度。在不降低光学树脂综合性能的基础上提升光学树脂折射率一直是该领域的热点和难点,在光学树脂中引入高摩尔折射率的硫元素被认为是最有效和常用的方法之一。本文将含硫光学树脂分为烯烃类、环氧类、环硫类、多环类和聚氨酯类,简要综述了国内外近几年的研究进展,涉及单体合成、单体聚合以及单体结构对光学树脂综合性能影响,系统总结了以上材料的特性及发展。     

Graphene-Based Waveguides: Novel Method for Detecting Biological Activity

We demonstrate the fabrication of a biosensor based on graphene coupled with polydimethylsiloxane (PDMS) waveguide. Biosensors work on the principle of local evanescent graphene-coupled wave sensor. It is observed that the evanescent field shifts in the presence of chemical or biological species as evanescent waves are extremely sensitive to a change in refractive index. This method helps to monitor the target analyte by attaching the selective receptor molecules to the surface of the PDMS optical waveguide resulting in its optical intensity distribution shift. We monitor the electrical properties of graphene in the dark and under illumination of PDMS waveguide. The changes in photocurrent through the graphene film were monitored for blue, green, and red light. We observed that the fabricated graphene-coupled PDMS optical waveguide sensor is sensitive to visible light for the used bioanalytes.     

High-refractive index acrylate polymers for applications in nanoimprint lithography

The development of polymeric optical materials with a higher refractive index,transparency in the visible spectrum region and easier processability is increasingly desirable for advanced optical applications such as microlenses,image sensors,and organic light-emitting diodes.Most acrylates have a low refractive index(around 1.50)which does not meet the high perfo rmance requirements of advanced optical materials.In this research,three novel acrylates were synthesized via a facile one-step approach and used to fabricate optical transparent polymers.All of the polymers reveal good optical properties including high transparency(≥90%)in the visible spectrum region and high refractive index values(1.6363)at 550 nm.Moreover,nanostructures of these acrylate polymers with various feature sizes including nanogratings and photonic crystals were successfully fabricated using nanoimprint lithography.These results indicate that these acrylates can be used in a wide range of optical and optoelectronic devices where nanopatterned films with high refractive index and transparency are required.