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We report on sub-wavelength structuring of photosensitive azo-containing polymer films induced by a surface plasmon interference intensity pattern. The two surface plasmon waves generated at neighboring nano-slits in the metal layer during irradiation interfere constructively, resulting in an intensity pattern with a periodicity three times smaller than the wavelength of the incoming light. The near field pattern interacts with the photosensitive polymer film placed above it, leading to a topography change which follows the intensity pattern exactly, resulting in the formation of surface relief gratings of a size below the diffraction limit. We analyze numerically and experimentally how the depth of the nano-slit alters the interference pattern of surface plasmons and find that the sub-wavelength patterning of the polymer surface could be optimized by modifying the geometry and the size of the nano-slit.
We report on reversible structuring of photosensitive azo-containing polymer films induced by near-field intensity patterns emanating from illuminated nano-scale metal structures fabricated by colloidal lithography. Two different sets of these nano-antennas, consisting of either gold or silver, were investigated with respect to their ability to induce topography changes in a photosensitive polymer film placed above. Using in situ recorded atomic force microscopy micrographs of polymer topography changes during UV irradiation, we find that the response of the polymer film differs for the two metals at similar geometries of the metal nanostructures. The maximum topography change is stronger for Ag antennas as compared to the Au pattern, whereas the latter material revealed a pronounced splitting of topography maxima into two, a phenomenon less visible in the case of Ag. Finite difference time domain simulations of the electromagnetic field distribution in the vicinity of the metal structures confirm this remarkable observation. The local intensity is twice as large for the Ag as compared to the Au structures, and in each case, a splitting of the intensity pattern results, with a stronger modulation for Au. For both metals, the topography change was found to be reversible between a patterned and a flat by repeated change of irradiation conditions.
It is well-known that surface plasmon generated near fields of suitably irradiated metal nano-structures can induce a patterning in an azobenzene-modified photosensitive polymer film placed on top. The change in the topography usually follows closely and permanently the underlying near field intensity pattern. With this approach, one can achieve a multitude of morphologies by additionally changing light intensity, polarization and the kind of metal used for nano-structuring. In this paper, we demonstrate that below a critical value of the polymer film thickness, the receding polymer material induces a change in refractive index of the glass-metal-polymer system, modifying the near field intensity distribution and causing a back-reaction on the flow of polymer material. This has a profound influence on the smallest size of topographical features that can be imprinted into the polymer.
Here we demonstrate how a surface plasmon (SP) generated near field pattern in the vicinity of a nano-scale pin hole can be used to generate reversible topography changes in a photosensitive polymer film above the opening. This can be achieved by simply changing the polarization state of the plasmon generating incoming light. In the case of linear polarization, the near field intensity pattern causes the film to laterally expand/contract according to the direction of the polarization. For circular polarization, two pronounced rims corresponding to maxima in the topography are observed. In all cases, the topographical variation is in close agreement with the SP intensity distribution computed from finite difference time domain simulation. Our results demonstrate the versatility of using SP near fields to imprint a variety of structures into photosensitive polymer films using only a single metallic mask.
Nanogradient polymer brushes
(2012)
We have used polarized confocal Raman microspectroscopy and scanning near-field optical microscopy with a resolution of 60 nm to characterize photoinscribed grating structures of azobenzene doped polymer films on a glass support. Polarized Raman microscopy allowed determining the reorientation of the chromophores as a function of the grating phase and penetration depth of the inscribing laser in three dimensions. We found periodic patterns, which are not restricted to the surface alone, but appear also well below the surface in the bulk of the material. Near-field optical microscopy with nanoscale resolution revealed lateral two-dimensional optical contrast, which is not observable by atomic force and Raman microscopy.
In this paper, we report on in-situ atomic force microscopy (AFM) studies of topographical changes in azobenzene-containing photosensitive polymer films that are irradiated with light interference patterns. We have developed an experimental setup consisting of an AFM combined with two-beam interferometry that permits us to switch between different polarization states of the two interfering beams while scanning the illuminated area of the polymer film, acquiring corresponding changes in topography in-situ. This way, we are able to analyze how the change in topography is related to the variation of the electrical field vector within the interference pattern. It is for the first time that with a rather simple experimental approach a rigorous assignment can be achieved. By performing in-situ measurements we found that for a certain polarization combination of two interfering beams [namely for the SP (a dagger center dot, a dagger") polarization pattern] the topography forms surface relief grating with only half the period of the interference patterns. Exploiting this phenomenon we are able to fabricate surface relief structures with characteristic features measuring only 140 nm, by using far field optics with a wavelength of 491 nm. We believe that this relatively simple method could be extremely valuable to, for instance, produce structural features below the diffraction limit at high-throughput, and this could significantly contribute to the search of new fabrication strategies in electronics and photonics industry.
In this paper we report on an opto-mechanical scission of polymer chains within photosensitive diblock-copolymer brushes grafted to flat solid substrates. We employ surface-initiated polymerization of methylmethacrylate (MMA) and t-butyl methacrylate (tBMA) to grow diblock-copolymer brushes of poly(methylmethacrylate-b-t-butyl methacrylate) following the atom transfer polymerization (ATRP) scheme. After the synthesis, deprotection of the PtBMA block yields poly(methacrylic acid) (PMAA). To render PMMA-b-PMAA copolymers photosensitive, cationic azobenzene containing surfactants are attached to the negatively charged outer PMAA block. During irradiation with an ultraviolet (UV) interference pattern, the extent of photoisomerization of the azobenzene groups varies spatially and results in a topography change of the brush, i.e., formation of surface relief gratings (SRG). The SRG formation is accompanied by local rupturing of the polymer chains in areas from which the polymer material recedes. This opto-mechanically induced scission of the polymer chains takes place at the interfaces of the two blocks and depends strongly on the UV irradiation intensity. Our results indicate that this process may be explained by employing classical continuum fracture mechanics, which might be important for tailoring the phenomenon for applying it to poststructuring of polymer brushes.
We report on conductivity behavior of very thin gold layer deposited on a photosensitive polymer film. Under irradiation with light interference pattern, the azobenzene containing photosensitive polymer film undergoes deformation at which topography follows a distribution of intensity, resulting in the formation of a surface relief grating. This process is accompanied by a change in the shape of the polymer surface from flat to sinusoidal together with a corresponding increase in surface area. The gold layer placed above deforms along with the polymer and ruptures at a strain of 4%. The rupturing is spatially well defined, occurring at the topographic maxima and minima resulting in periodic cracks across the whole irradiated area. We have shown that this periodic micro-rupturing of a thin metal film has no significant impact on the electrical conductivity of the films. We suggest a model to explain this phenomenon and support this by additional experiments where the conductivity is measured in a process when a single nanoscopic scratch is formed with an AFM tip. Our results indicate that in flexible electronic materials consisting of a polymer support and an integrated metal circuit, nano-and micro cracks do not alter significantly the behavior of the conductivity unless the metal is disrupted completely. (C) 2013 AIP Publishing LLC.
We report on a change in the properties of monomolecular films of polyelectrolyte molecules, induced by illuminating the silicon substrate on which they adsorb. It was found that under illumination the thickness of the adsorbed layer decreases by at least 27% and at the same time the roughness is significantly reduced in comparison to a layer adsorbed without irradiation. Furthermore, the homogeneity of the film topography and the surface potential is shown to be improved by illumination. The effect is explained by a change in surface charge density under irradiation of n- and p-type silicon wafers. The altered charge density in turn induces conformational changes of the adsorbing polyelectrolyte molecules. Their photocontrolled adsorption opens new possibilities for selective manipulation of adsorbed films. This possibility is of potential importance for many applications such as the production of well-defined coatings in biosensors or microelectronics.