Kokou D. Dorkenoo

Role of surface plasmon in second harmonic generation from gold nanorods

The role of surface plasmon in second harmonic generation from arrays of gold nanorod particles excited by femtosecond laser pulses is investigated as a function of incident light polarization and irradiation wavelength. In addition to photoluminescence, a peak of second harmonic is observed and is found to depend on the polarization and wavelength of the fundamental frequency laser beam. In particular, the authors found similarities between extinction spectra of the nanoparticles and spectra of emmitted second harmonic. This behavior can be explained by resonant excitation of localized surface plasmon resonances.

Quasi-solitonic behavior of self-written waveguides created by photopolymerization

We investigated the condition of unique self-written channel and multichannel propagation inside bulk photopolymerizable materials. Light was introduced in the medium by a single-mode optical fiber. At a very low beam power of 5 muW , a unique uniform-channel waveguide without any broadening was obtained by polymerization. When the input power is increased to 100 muW , the guide becomes chaotic and multichannel. We connected two fibers separated by a 1-cm distance. The results open the door to studies of the optical and electro-optical properties of photopolymerized guides doped by nonlinear optical chromophores and to possible applications in integrated optical devices.

Rewritable optical data storage in azobenzene copolymers

We propose to encode optical information through the localized depoling of polar chromophores in thin films of grafted polymeric materials with a femtosecond near IR laser source. This disorientation is promoted through the photoisomerization of the azo-dye component induced by a twophoton absorption process. We show that the resulting localized loss in second harmonic generation efficiency can be exploited in data storage applications. The low irradiation powers used allow for a recycling by reheating and repoling the films leading to a rewritable system.

One-step waveguide and optical circuit writing in photopolymerizable materials processed by two-photon absorption

Two-photon absorption process is known to be a convenient tool to create three-dimensional microstructures in photopolymerizable materials. In this context, we have fabricated stable optical waveguides. The features of these waveguides (in particular, transmission losses) have been compared to the results of numerical simulations. We have also demonstrated the possibility of connecting two optical fibers via a curved guide and to realize Y splitters. The technique allows one to fabricate operational integrated optical circuits in photopolymerizable resins.

N,N′-Dibutylbarbituric acid as an acceptor moiety in push–pull chromophores

Twelve novel D–π–A chromophores with the N,N′-dibutylbarbituric acid acceptor, the N,N-dimethylamino donor and a systematically extended π-linker were synthesized. The extent of intramolecular charge-transfer, structure–property relationships and nonlinear optical properties were further investigated by X-ray analysis, electrochemistry, UV/Vis absorption spectra, calculations and EFISH experiments.

Polarization state studies in second harmonic generation signals to trace atherosclerosis lesions

We have performed multi-photon image reconstructions as well as polarization state analyses inside an artery wall affected by atherosclerosis to investigate the changes in collagen structure. Mice, either healthy or affected by spontaneous atherosclerosis, have been used for this purpose. A two-photon imaging system has been used to investigate atherosclerotic lesions in the ascending aorta of mice. Second harmonic imaging has been performed alternatively on healthy samples and on affected region. The reconstructed images show that the spatial distribution of the collagen network seems disorganized by the disease. The polarization state studies reveal however that the apparent disorganization of the collagen is related to its spatially diffuse distribution and that the internal structure of the collagen fibers is not affected by the disease. In addition, a theoretical simulation of the second harmonic polarization states shows that they are consistent with the known 3D structure of the collagen network.

Two-dimensional colloid-based photonic crystals for distributed feedback polymer lasers

We report on a process to design highly ordered monolayers of two-dimensional photonic crystals, made of silica nanoparticules, that can be used for the development of organic optical devices. We have used a photopolymerization process to incorporate a dye gain medium into the nanoparticle layers in order to achieve a laser cavity. The high spatial coherence of the deposits allows for single-mode laser emission in the plane of the layer when the light excitation is perpendicular to the plane. Such periodic films should help in reducing the number of layers needed for future electrically pumped distributed feedback lasers.

Time-resolved measurement of the refractive index for photopolymerization processes

A double-interferometer technique is employed to examine the dynamics of a photopolymerization process. The dye molecule is eosine Y. The refractive index and the thickness of the photopolymerizable film are measured as a function of time. During the photopolymerization process, the first quantity increases by 2%, while the second quantity decreases by more than 4%. Therefore, the refractive index cannot be measured by means of single-interferometer techniques. By fitting our experimental curves to a rate equation, the quantum yield and the absorption coefficient of the sample can be determined with good accuracy.

Image storage through gray-scale encoding of second harmonic signals in azo-dye copolymers

The authors investigated the optical data and image storage in polymeric materials functionalized with azo-dye molecules. Thin films are initially poled to generate a spatially homogeneous second harmonic signal. The information is locally inscribed through the disorientation of the azo chromophores by successive isomerization cycles induced through the two-photon absorption processes. The resulting micron-scale controlled decrease in second harmonic signal can be exploited to perform optical storage. As a demonstration of the proposed method, they store a picture with an 8bit gray-scale encoding. This image can only be retrieved through second harmonic detection and not by linear optical imaging techniques.

Toward submicrometer optical storage through controlled molecular disorder in azo-dye copolymer films

While information encoding through optically induced orientation of azo dyes in organic matrices is being extensively pursued, we propose the alternative of starting out with poled films and to locally reduce their second-harmonic generation capacity by a focused near-infrared femtosecond laser beam of moderate intensity. Arrays of dots irradiated under varying conditions are subsequently imaged in situ as dark spots on a bright background. The samples are also examined through conventional optical microscopy and through atomic force microscopy. We demonstrate that, of these techniques, second-harmonic imaging performs best in the task of information retrieval.