[Polarimétrie non-linéaire sur des cristaux moléculaires jusqu'à l'échelle nanométrique]
L'optique non-linéaire en milieux moléculaires est actuellement en phase de renouvellement au débouché de la possibilité nouvelle d'accéder aux échelles nanométriques grâce à une instrumentation nano-photonique de pointe et aux modèles associés. Nous nous proposons dans cet article de passer en revue et de discuter des développements en cours dans ce domaine dans notre laboratoire, en mettant particulièrement en exergue les propriétés tensorielles de dépendance en polarisations résolues à une échelle submicronique, aux fins d'une meilleure compréhension des architectures de nanostructures, de l'ordre et des propriétés dynamiques de cristallisation jusqu'à la résolution de la microscopie confocale à deux photons. L'intérêt de combiner les effets non-linéaires cohérents (i.e. génération de second harmonique) et incohérents (i.e. fluorescence à deux photons) tous deux résolus en polarisation apparaît dans la possibilité de déterminer l'orientation et la qualité cristalline de nano-cristaux (depuis des cristaux mono-moléculaires jusqu'à des cristaux binaires de type hôte-matrice). Le modèle de gaz orienté, interprété de la façon la plus générale en symétries multipolaires grâce au formalisme des tenseurs irréductibles, permet d'identifier des formes génériques de réponses angulaires en polarisation dont l'allure renseigne qualitativement et quantitativement sur les propriétés structurelles d'une large variété de nanomatériaux organiques et inorganiques.
Molecular nonlinear optics is currently experiencing a fruitful revival as a result of the unprecedented possibility to experimentally access the nanoscale through adequate nanophotonics instrumentation and modelling. It is the purpose of this article to survey and discuss some ongoing developments in this domain within our laboratory, with special emphasis on polarization dependent tensorial properties read-out at submicron scale, to be exploited towards a better understanding of nanostructured architectures, ordering as well as dynamical crystallization properties of a variety of samples, down to the spatial resolution of two-photon nonlinear confocal microscopy. The advantages of combining coherent (e.g. second harmonic generation) and incoherent (e.g. two photon induced fluorescence) phenomena, moreover with polarization resolution, will be shown to open-up a new and unique pathway onto the orientation as well as crystalline quality of different types of nanocrystals (from one component molecular to mixed guest–host binary crystals). The oriented gas model, expressed in its most general invariant form by way of irreducible multipolar decomposition permits to identify generic types of nonlinear polarization patterns which potentially provide both qualitative and quantitative insight onto the structural properties of a broad variety of molecular as well as inorganic nanomaterials.
Mot clés : Nanoparticule, Optique non-linéaire
Sophie Brasselet 1 ; Joseph Zyss 1
@article{CRPHYS_2007__8_2_165_0,
author = {Sophie Brasselet and Joseph Zyss},
title = {Nonlinear polarimetry of molecular crystals down to the nanoscale},
journal = {Comptes Rendus. Physique},
pages = {165--179},
publisher = {Elsevier},
volume = {8},
number = {2},
year = {2007},
doi = {10.1016/j.crhy.2006.07.015},
language = {en},
}
Sophie Brasselet; Joseph Zyss. Nonlinear polarimetry of molecular crystals down to the nanoscale. Comptes Rendus. Physique, Volume 8 (2007) no. 2, pp. 165-179. doi : 10.1016/j.crhy.2006.07.015. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/j.crhy.2006.07.015/
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