Two-photon excitation provides a means of activating chemical or physical processes with high spatial resolution in three dimensions and has made possible the development of three-dimensional fluorescence imaging, optical data storage, and lithographic microfabrication. These applications take advantage of the fact that the two-photon absorption probability depends quadratically on intensity, so under tight-focusing conditions, the absorption is confined at the focus to a volume of order λ3 (where λ is the laser wavelength). Any subsequent process, such as fluorescence or a photoinduced chemical reaction, is also localized in this small volume. Although three-dimensional data storage and microfabrication have been illustrated using two-photon-initiated polymerization of resins incorporating conventional ultraviolet-absorbing initiators, such photopolymer systems exhibit low photosensitivity as the initiators have small two-photon absorption cross-sections (δ). Consequently, this approach requires high laser power, and its widespread use remains impractical. Here we report on a class of π;-conjugated compounds that exhibit large δ (as high as 1, 250 × 10−50 cm4 s per photon) and enhanced two-photon sensitivity relative to ultraviolet initiators. Two-photon excitable resins based on these new initiators have been developed and used to demonstrate a scheme for three-dimensional data storage which permits fluorescent and refractive read-out, and the fabrication of three-dimensional micro-optical and micromechanical structures, including photonic-bandgap-type structures.

Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication

We first provide an overview of 3-D shape measurement us- ing various optical methods. Then we focus on structured light tech- niques where various optical configurations, image acquisition tech- niques, data postprocessing and analysis methods and advantages and limitations are presented. Several industrial application examples are presented. Important areas requiring further R&D are discussed. Finally, a comprehensive bibliography on 3-D shape measurement is included, although it is not intended to be exhaustive. © 2000 Society of Photo-Optical Instrumentation Engineers. (S0091-3286(00)00101-X)

Overview of three-dimensional shape measurement using optical methods

Fluorescence is widely used in optical devices, microscopy imaging, biology, medical research and diagnosis. Improving fluorescence sensitivity, all the way to the limit of single-molecular detection needed in many applications, remains a great challenge. The technique of surface enhanced fluorescence (SEF) is based upon the design of surfaces in the vicinity of the emitter. SEF yields an overall improvement in the fluorescence detection efficiency through modification and control of the local electromagnetic environment of the emitter. Near-field coupling between the emitter and surface modes plays a crucial role in SEF. In particular, plasmonic surfaces with localized and propagating surface plasmons are efficient SEF substrates. Recent progress in tailoring surfaces at the nanometre scale extends greatly the realm of SEF applications. This review focuses on the recent advances in the different mechanisms involved in SEF, in each case highlighting the most relevant applications.

http://turroserver.chem.columbia.edu/surfaceplasmons/pdf/53_jpd_41_1_2008_sefsrev.pdf

Surface enhanced fluorescence

This work presents the fabrication of biologically inspired artificial compound eyes The artificial ommatidium, like that of an insect's compound eyes, consists of a refractive polymer microlens, a light-guiding polymer cone, and a self-aligned waveguide to collect light with a small angular acceptance The ommatidia are omnidirectionally arranged along a hemispherical polymer dome such that they provide a wide field of view similar to that of a natural compound eye The spherical configuration of the microlenses is accomplished by reconfigurable microtemplating, that is, polymer replication using the deformed elastomer membrane with microlens patterns The formation of polymer waveguides self-aligned with microlenses is also realized by a self-writing process in a photosensitive polymer resin The angular acceptance is directly measured by three-dimensional optical sectioning with a confocal microscope, and the detailed optical characteristics are studied in comparison with a natural compound eye

http://science.sciencemag.org/content/sci/312/5773/557.full.pdf

Biologically inspired artificial compound eyes.

Modal decomposition of light has been known for a long time, applied mostly to pattern recognition. With the commercialization of liquid-crystal devices, digital holography as an enabling tool has become accessible to all, and with it all-digital tools for the decomposition of light have finally come of age. We review recent advances in unravelling the properties of light, from the modal structure of laser beams to decoding the information stored in orbital angular momentum (OAM)-carrying fields. We show application of these tools to fiber lasers, solid-state lasers, and structured light created in the laboratory by holographic laser beam shaping. We show by experimental implementation how digital holograms may be used to infer the intensity, phase, wavefront, Poynting vector, polarization, and OAM density of some unknown optical field. In particular, we outline how virtually all the previous ISO-standard beam diagnostic techniques may be readily replaced with all-digital equivalents, thus paving the way for unravelling of light in real time. Such tools are highly relevant to the in situ analysis of laser systems, to mode division multiplexing as an emerging tool in optical communication, and for quantum information processing with entangled photons.

Creation and detection of optical modes with spatial light modulators

The development of volume phase gratings written by two-wave-mixing in glass-like polymer storage materials based on poly (methylmethacrylate) and its thermostable derivative (copolymer with acrylic acid) with distributed phenanthrenequinone is investigated experimentally and theoretically. The maximal diffraction efficiency is considered in dependence on the grating period. The redistribution processes of the molecules are described with a one-dimensional diffusion model yielding the existence of a non-local response in the photopolymer layer, and the corresponding non-local response length of phenanthrenequinone is found experimentally.

Non-local response in glass-like polymer storage materials based on poly (methylmethacrylate) with distributed phenanthrenequinone.

For phase holographic gratings in layers of polymethylmethacrylate, containing phenanthrenequinone in high concentration (nearly 3 mol%), a discrepancy between experimental (up to 9) and estimated (∼45) magnitudes of the thermal diffusion amplification coefficient has been revealed. Analysis of plausible reasons of the lower experimental efficiency of the diffusion amplification has been carried out. The influence of material deformations on the reflection grating formation process was investigated experimentally. It is shown that thermoactivated amplification of holograms under high phenanthrenequinone concentration and its profound modulation are depressed by the arising density ‘grating’.

/pdf/phase-hologram-formation-in-highly-concentrated-2r6555eoe5.pdf

Phase hologram formation in highly concentrated phenanthrenequinone-PMMA media

Fluorescence lifetimes of thin, rhodamine 6G-doped polymer layers in front of a mirror have been determined as a function of the emitter-mirror separation and the conditions of excitation and observation. Lifetime is well known to depend on the spatial emitter-mirror separation. The explanation of experimental data needs to consider direction, polarization, and numerical aperture of the experimental system. As predicted theoretically, experimental results depend on the conditions of illumination and observation, because of the different lifetimes of emitters aligned horizontally or vertically with respect to the plane of interfaces and their selection by the experimental system. This effect is not observable when ions are used as a source of fluorescence, because ensemble averaging depends on the properties of sources.

Fluorescence lifetimes of molecular dye ensembles near interfaces

A holographic in-line microscope setup with a glass sample carrier commonly uses a coherent laser light source, with the disadvantage of an incomplete suppression of disturbing interferences and coherence-induced noise. We use temporally partially coherent and spatially partially coherent illumination in the micrometer range of 5 to 100 μm generated by spectrally and spatially filtered light-emitting diodes (LEDs) and tungsten filament lamps. It is shown how errors in reconstructed holograms are decreased by a factor of more than two and the spatial resolution reaches the limit as determined by the numerical aperture. A straightforward model is developed to investigate the effects of partial coherence. The optimization of the coherence parameters improves the imaging quality up to the limit of a conventional microscope.

Optimized coherence parameters for high-resolution holographic microscopy

An analytical description connected with a numerical calculation of the propagation of self-trapped laser beams in a polymethylmethacrylate matrix containing phenanthrenequinone molecules is presented. A theoretical model for the spatial distribution of boundary optical waves is developed in dependence on characteristic beam parameters.

Richard Kowarschik

Papers

Non-local response in glass-like polymer storage materials based on poly (methylmethacrylate) with distributed phenanthrenequinone.

Phase hologram formation in highly concentrated phenanthrenequinone-PMMA media

Fluorescence lifetimes of molecular dye ensembles near interfaces

Optimized coherence parameters for high-resolution holographic microscopy

Numerical investigation of the (1+1)D self-trapping of laser beams in polymeric films based on polymethylmethacrylate and phenanthrenequinone