Modeling the optical properties of self-organized arrays of liquid crystal defects

International audienceLocal full Mueller matrix measurements in the Fourier plane of a microscope lens were used to determine the internal anisotropic ordering in periodic linear arrays of smectic liquid crystal defects, known as 'oily streaks'. We propose a single microstructure-dependent model taking into account the anisotropic dielectric function of the liquid crystal that reproduces the smectic layers orientation and organization in the oily streaks. The calculated Mueller matrix elements are compared to the measured data to reveal the anchoring mechanism of the smectic oily streaks on the substrate and evidence the presence of new type of defect arrangement. Beyond the scientific inquiry, the understanding and control of the internal structure of such arrays offer technological opportunities for developing liquid-crystal based sensors and self-assembled nanostructures

Self-organized arrays of dislocations in thin smectic liquid crystal films

International audienceCombining optical microscopy, synchrotron X-ray diffraction and ellipsometry, we studied the internal structure of linear defect domains (oily streaks) in films of smectic liquid crystal 8CB with thickness 100-300 nm confined between air and a rubbed PVA polymer substrate which impose hybrid anchoring conditions (normal and unidirectional planar, respectively). We show how the presence or absence of dislocations control the structure of highly deformed thin smectic films. Each domain contains smectic layers curved in the shape of flattened hemicylinders to satisfy both anchoring conditions, together with grain boundaries whose size and shape are controlled by the presence of dislocation lines. A flat grain boundary normal to the interface connects neighboring hemicylinders, while a rotating grain boundary (RGB) is located near the axis of curvature of the cylinders. The RGB shape appears such that dislocation lines are concentrated at its summit close to the air interface. The smectic layers reach the polymer substrate via a transition region where the smectic layer orientation satisfies the planar anchoring condition over the entire polymer substrate and whose thickness does not depend on the one of the film. The strength of the planar anchoring appears to be high, larger than 10 −2 J/m 2 , compensating for the high energy cost of creating an additional 2D defect between an horizontal smectic layer and perpendicular ones. This 2D defect may be melted, in order to avoid the creation of a transition region structure composed of a large number of dislocations. As a result, linear defect domains can be considered as arrays of oriented defects, straight dislocations of various Burger vectors, whose location is now known and 2D nematic defects. The possibility of easy variation between the present structure with a moderate amount of dislocations and a structure with a large number of dislocations is also demonstrated

Organization and assembly of semi-conducting nanoparticles in networks of smectic topological defects

Nous présentons dans cette thèse une utilisation de la structure dite de stries huileuses présente lors de la compétition entre deux ancrages antagonistes de part et d’autre d’un film sub-micrométrique de cristal liquide en phase smectique pour réaliser le contrôle à l’échelle individuelle de l’orientation d’émetteurs de photons unique ainsi que de l’auto-organisation ultérieure lorsque la concentration est augmentée. La morphologie interne de cette structure est étudiée à l’aide d’observations en microscopie optique polarisée, d’ellipsométrie et de diffraction de rayons X. L’analyse de ces résultats mène au modèle présenté en fin de chapitre 2 caractérisé par la formation d’un réseau de défauts topologiques orientés. Ces stries huileuses sont ensuite utilisées pour permettre l’alignement à l’échelle individuelle de particules semi-conductrices, des dots-in-rods de CdSe:CdS, suivant l’axe principal des défauts. Le chapitre 3 présente l’insertion des particules et la mesure de l’orientation de leur dipôle associé ainsi que celle du degré de polarisation. Le chapitre 4 discute du comportement des particules pour une concentration élevée, avec outre leur orientation leur auto-organisation au sein des stries huileuses. Nous faisons une analyse statistique de la densité des amas formés à la surface d’un échantillon et des informations résultant de la structure des amas sur l’organisation des défauts dans différentes situations. On observe un alignement des nanoparticules à l’échelle unique et en amas, ainsi qu’un maintien ou un renforcement du degré de polarisation mesuré, montrant une auto-organisation des amas favorisant l’interaction entre les dipôles des particules.This thesis discusses the use of a liquid crystal structure, called oily streaks, formed by the competition of two antagonist anchoring on each side of a submicrometric liquid crystal layer, to achieve the self-alignment and, for higher concentration, the organization, of single photon emitters on an individual scale. We discuss the internal layout of these oily streaks through measurements done in polarized optical microscopy, ellipsometry and X-ray diffraction analysis. These data sets are correlated in chapter 2 into a description of the internal structure of the oily streaks, characterized by the formation of a pattern of oriented topological defects, and an analysis of their behaviour. These streaks are then used as a template to align single photon emitters, CdSe:CdS dot-in-rods, on an individual scale alongside the main axis of the defects. We measure the alignment of their dipoles as well as their degree of polarization in order to discuss the behaviour of the particles in the topological defects of the oily streaks. The last chapter presents a statistical analysis of the behaviour of nanoparticles in oily streaks once their concentration is increased, depending on their size in number of particles as well as the characteristics of the structure in which the single particles or the clusters are trapped. We use these elements to further our understanding of the layout of oily streaks in different thicknesses and configurations as we observe the alignment phenomenon both with single particles and clusters, as well as, for the clusters, a similar or superior degree of polarization compared to single particles, indicating an interaction between the particles’ dipoles

Assemblage et organisation de nanoparticules semi-conductrices dans des réseaux de défauts topologiques smectiques

This thesis discusses the use of a liquid crystal structure, called oily streaks, formed by the competition of two antagonist anchoring on each side of a submicrometric liquid crystal layer, to achieve the self-alignment and, for higher concentration, the organization, of single photon emitters on an individual scale. We discuss the internal layout of these oily streaks through measurements done in polarized optical microscopy, ellipsometry and X-ray diffraction analysis. These data sets are correlated in chapter 2 into a description of the internal structure of the oily streaks, characterized by the formation of a pattern of oriented topological defects, and an analysis of their behaviour. These streaks are then used as a template to align single photon emitters, CdSe:CdS dot-in-rods, on an individual scale alongside the main axis of the defects. We measure the alignment of their dipoles as well as their degree of polarization in order to discuss the behaviour of the particles in the topological defects of the oily streaks. The last chapter presents a statistical analysis of the behaviour of nanoparticles in oily streaks once their concentration is increased, depending on their size in number of particles as well as the characteristics of the structure in which the single particles or the clusters are trapped. We use these elements to further our understanding of the layout of oily streaks in different thicknesses and configurations as we observe the alignment phenomenon both with single particles and clusters, as well as, for the clusters, a similar or superior degree of polarization compared to single particles, indicating an interaction between the particles’ dipoles.Nous présentons dans cette thèse une utilisation de la structure dite de stries huileuses présente lors de la compétition entre deux ancrages antagonistes de part et d’autre d’un film sub-micrométrique de cristal liquide en phase smectique pour réaliser le contrôle à l’échelle individuelle de l’orientation d’émetteurs de photons unique ainsi que de l’auto-organisation ultérieure lorsque la concentration est augmentée. La morphologie interne de cette structure est étudiée à l’aide d’observations en microscopie optique polarisée, d’ellipsométrie et de diffraction de rayons X. L’analyse de ces résultats mène au modèle présenté en fin de chapitre 2 caractérisé par la formation d’un réseau de défauts topologiques orientés. Ces stries huileuses sont ensuite utilisées pour permettre l’alignement à l’échelle individuelle de particules semi-conductrices, des dots-in-rods de CdSe:CdS, suivant l’axe principal des défauts. Le chapitre 3 présente l’insertion des particules et la mesure de l’orientation de leur dipôle associé ainsi que celle du degré de polarisation. Le chapitre 4 discute du comportement des particules pour une concentration élevée, avec outre leur orientation leur auto-organisation au sein des stries huileuses. Nous faisons une analyse statistique de la densité des amas formés à la surface d’un échantillon et des informations résultant de la structure des amas sur l’organisation des défauts dans différentes situations. On observe un alignement des nanoparticules à l’échelle unique et en amas, ainsi qu’un maintien ou un renforcement du degré de polarisation mesuré, montrant une auto-organisation des amas favorisant l’interaction entre les dipôles des particules