Experimental determination of nanocomposite grating structures by light- and neutron-diffraction in the multi-wave-coupling regime.

We experimentally demonstrate how to accurately retrieve the refractive index profile of photonic structures by standard diffraction experiments and use of the rigorous coupled-wave analysis in the multi-wave coupling regime, without the need for taking any auxiliary data. In particular, we show how the phases of the Fourier components of a periodic structure can be fully recovered by deliberately choosing a probe wavelength of the diffracting radiation much smaller than the lattice constant of the structure. In the course of our demonstration, we accurately determine the slight asymmetry of the structure of nanocomposite phase gratings by light and neutron diffraction measurements.

Light- and Neutron-Optical Properties of Holographic Transmission Gratings from Polymer-Ionic Liquid Composites with Submicron Grating Spacing.

We investigate the applicability of polymer-ionic liquid composites as optical elements for light, as well as for slow neutrons. The gratings are recorded using two-beam mixing and are characterized experimentally based on their diffraction properties. We produced a set of samples differing in their thickness, ranging from 10 m - 100 m . We demonstrate that it is possible to prepare transmission gratings with a lattice constant of Λ = 480 n m , resulting in thick gratings for light, as well as neutrons. The presented samples show low optical losses in the Vis-UV spectrum and exhibit refractive index modulations of about 10 - 3 at λ = 543 n m . However, further improvements have to be made to obtain efficient neutron optical components.

Photopolymerizable nanocomposite photonic materials and their holographic applications in light and neutron optics.

We present an overview of recent investigations of photopolymerizable nanocomposite photonic materials in which, thanks to their high degree of material selectivity, recorded volume gratings possess high refractive index modulation amplitude and high mechanical/thermal stability at the same time, providing versatile applications in light and neutron optics. We discuss the mechanism of grating formation in holographically exposed nanocomposite materials, based on a model of the photopolymerization-driven mutual diffusion of monomer and nanoparticles. Experimental inspection of the recorded grating's morphology by various physicochemical and optical methods is described. We then outline the holographic recording properties of volume gratings recorded in photopolymerizable nanocomposite materials consisting of inorganic/organic nanoparticles and monomers having various photopolymerization mechanisms. Finally, we show two examples of our holographic applications, holographic digital data storage and slow-neutron beam control.

A Comprehensive Study of Photorefractive Properties in Poly(ethylene glycol) Dimethacrylate- Ionic Liquid Composites.

A detailed investigation of the recording, as well as the readout of transmission gratings in composites of poly(ethylene glycol) dimethacrylate (PEGDMA) and ionic liquids is presented. Gratings with a period of about 5.8 micrometers were recorded using a two-wave mixing technique with a coherent laser beam of a 355-nm wavelength. A series of samples with grating thicknesses d 0 = 10 … 150 micrometers, each for two different exposure times, was prepared. The recording kinetics, as well as the post-exposure properties of the gratings were monitored by diffracting a low intensity probe beam at a wavelength of 633 nm for Bragg incidence. To obtain a complete characterization, two-beam coupling experiments were conducted to clarify the type and the strength of the recorded gratings. Finally, the diffraction efficiency was measured as a function of the readout angle at different post-exposure times. We found that, depending on the parameters, different grating types (pure phase and/or mixed) are generated, and at elevated thicknesses, strong light-induced scattering develops. The measured angular dependence of the diffraction efficiency can be fitted using a five-wave coupling theory assuming an attenuation of the gratings along the thickness. For grating thicknesses larger than 85 microns, light-induced scattering becomes increasingly important. The latter is an obstacle for recording thicker holograms, as it destroys the recording interference pattern with increasing sample depth. The obtained results are valuable in particular when considering PEGDMA-ionic liquid composites in the synthesis of advanced polymer composites for applications, such as biomaterials, conductive polymers and holographic storage materials.

Effects of chain-transferring thiol functionalities on the performance of nanoparticle-polymer composite volume gratings.

We report influences of varying functionalities of thiols as chain transfer agents on the spatial frequency response, polymerization shrinkage, and thermal stability of a volume grating recorded in a photopolymerizable ZrO2 nanoparticle-polymer composite film. It is shown that a substantial increase in the saturated refractive index modulation is realized at high spatial frequencies by doping with multifunctional thiols. Moreover, the incorporation of multifunctional thiols considerably suppresses polymerization shrinkage of recorded volume gratings and thermal changes in refractive index and film thickness as compared with the case of mono-thiol. These results indicate that multifunctional thiols provide effective control of the properties of nanoparticle-polymer composite volume gratings for various applications in light and neutron optics.

Nanoparticle polymer composite volume gratings incorporating chain transfer agents for holography and slow-neutron optics.

We demonstrate twofold enhancement of the saturated refractive index modulation (Δn(sat)) recorded in a photopolymerizable nanoparticle-acrylate polymer composite film by incorporating thiols acting as chain transfer agents. The chain transfer reaction of thiols with (meth)acrylate monomer reduces the polymer crosslinking density and facilitates the mutual diffusion of nanoparticles and monomer during holographic exposure. These modifications provide increased density modulations of nanoparticles and the formed polymer, resulting in the enhancement of Δn(sat) as high as 1.6×10(-2) at a wavelength of 532 nm. The incorporation of thiols also leads to shrinkage suppression and to improvement of the grating's spatial frequency response. Such simultaneous improvement is very useful for holographic applications in light and neutron optics.

Two glass transitions of polyurea networks: effect of the segmental molecular weight.

Polymer-nanoparticle composites (PNCs) play an increasing role in technology. Inorganic or organic nanoparticles are usually incorporated into a polymer matrix to improve material properties. Polyurea is a spontaneously occurring PNC, exhibiting a phase segregated structure with hard nanodomains embedded in a soft (elastically compliant) matrix. This system shows two glass transitions at Tg1 and Tg2. It has been argued that they are related to the freezing of motion of molecular segments in the soft matrix (usual polymer α-glass transition at Tg1) and to regions of restricted mobility near the hard nanodomains (α'-process) at Tg2, respectively. We present detailed dynamic mechanical analysis (DMA) measurements for polyurea networks with different segmental lengths l(c) (2.5, 12.1, 24.5 nm) of the polymer chains, i.e. different volume fractions ϕ(x) (0.39, 0.12, 0.07) of the hard domains. The two glass transitions show up in two distinct peaks in tan δ at Tα and Tα'. Analysing the data using a Havriliak-Negami term for the α- and α'-relaxation, as well as Vogel-Fulcher dependencies for the corresponding relaxation times, it is found that the α-glass transition at Tg1 increases strongly (up to ΔT = 70 K) with increasing ϕ(x), whereas the α'-transition at Tg2 remains unchanged. At ϕ(x)(c) ≈ 0.19 the two curves intersect, i.e. Tg1 = Tg2. This value of ϕ(x)(c) is very close to the percolation threshold of randomly oriented overlapping ellipsoids of revolution with an aspect ratio of about 1 : 4-1 : 5. We therefore conclude that around 19% of the hard nanodomains polyurea changes from a system of hard nanoparticles embedded in a soft matrix (ϕ(x) ≤ ϕ(x)(c)) to a system of soft domains confined in a network of percolated hard domains at ϕ(x) ≥ ϕ(x)(c).

Depth profile of optically recorded patterns in light-sensitive liquid-crystal elastomers.

We investigated nonlinear absorption and photobleaching processes in a liquid-crystal elastomer doped with light-sensitive azobenzene moiety. A conventional one-dimensional holographic grating was recorded in the material with the use of two crossed UV laser beams and the angular dependence of the diffraction efficiency in the vicinity of the Bragg peak was analyzed. These measurements gave information on the depth to which trans to cis isomerization had progressed into the sample as a function of the UV irradiation time. Using a numerical model that takes into account the propagation of writing beams and rate equations for the local concentration of the absorbing trans conformer, we computed the expected spatial distribution of the trans and cis conformers and the shape of the corresponding Bragg diffraction peak for different irradiation doses. Due to residual absorption of the cis conformers the depth of the recording progresses logarithmically with time and is limited by the thermal relaxation from the cis to trans conformation.

Out-of-phase mixed holographic gratings: a quantative analysis.

We show, that by performing a simultaneous analysis of the angular dependencies of the +/- first and the zeroth diffraction orders of mixed holographic gratings, each of the relevant parameters can be obtained: the strength of the phase grating and the amplitude grating, respectively, as well as a potential phase between them. Experiments on a pure lithium niobate crystal are used to demonstrate the applicability of the analysis.

Colossal light-induced refractive-index modulation for neutrons in holographic polymer-dispersed liquid crystals.

We report strong diffraction of cold neutrons from an only 30 micro m thick holographic polymer-dispersed liquid crystal (H-PDLC) transmission grating. The light-induced refractive-index modulation for neutrons is about 10(-6), i.e., nearly 2 orders of magnitude larger than in the best photo-neutron-refractive materials probed up to now. This makes H-PDLCs a promising candidate for fabricating neutron-optical devices.

Separate and simultaneous investigation of absorption gratings and refractive-index gratings by beam-coupling analysis: comment.

We correct a fundamental error occurring in the paper by F. Kahmann [J. Opt. Soc. Am. A10, 1562 (1993)] leading to a different value for the parameter varphi(p,0), i.e., the initial phase shift for the complex grating.

Light-induced phase and amplitude gratings in centrosymmetric Gadolinium Gallium garnet doped with calcium.

The photosensitive properties of a centrosymmetric gadolinium gallium garnet crystal doped with calcium are investigated at room temperature. Elementary holograms can be recorded over a wide range of wavelengths in the visible spectral range. The photosensitive properties are studied experimentally using beam coupling and angular response experiments. Mixed absorption and refractive-index gratings are observed and their amplitudes and relative phases determined. Moreover, the candidate centers that are responsible for the photorefractive effect are discussed.

Specific recording kinetics as a general property of unconventional photorefractive media.

We introduce a model for the kinetics of grating formation during holographic recording in optically excitable two-state systems. An unexpected characteristic time dependence of the diffraction efficiency is found. We show that it originates from a nonlinear transformation of the light interference pattern into a refractive-index profile. Our findings strongly resemble and explain by nature the experimental data of two-state systems in general, here represented by two examples: sodium nitroprusside and terbium gallium garnet.