Anisotropic Confinement of Chromophores Induces Second-Order Nonlinear Optics in a Nanoporous Photonic Metamaterial

Second-order nonlinear optics is the base for a large variety of devices aimed at the active manipulation of light. However, physical principles restrict its occurrence to non-centrosymmetric, anisotropic matter. This significantly limits the number of base materials exhibiting nonlinear optics. Here, we show that embedding chromophores in an array of conical channels 13 nm across in monolithic silica results in mesoscopic anisotropic matter and thus in a hybrid material showing second-harmonic generation (SHG). This non-linear optics is compared to the one achieved in corona-poled polymer films containing the identical chromophores. It originates in confinement-induced orientational order of the elongated guest molecules in the nanochannels. This leads to a non-centrosymmetric dipolar order and hence to a non-linear light-matter interaction on the sub-wavelength, single-pore scale. Our study demonstrates that the advent of large-scale, self-organised nanoporosity in monolithic solids along with confinement-controllable orientational order of chromophores at the single-pore scale provides a reliable and accessible tool to design materials with a nonlinear meta-optics.

Schlagworte

Physics - Optics

Physics - Mesoscopic Systems and Quantum Hall Effect

Physics - Materials Science

physics.app-ph

Physics - Chemical Physics

DDC Class

000: Allgemeines, Wissenschaft

Projekt(e)

SFB 986: Teilprojekt B7 - Polymere in grenzflächenbestimmten Geometrien: Struktur, Dynamik und Funktion an planaren und in porösen Hybridsystemen

SFB 986: Teilprojekt C10 - Photonische Metamaterialien mit anpassbarer und schaltbarer Anisotropie durch Funktionalisierung von porösen Festkörpern mit Flüssigkristallen

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Anisotropic Confinement of Chromophores Induces Second-Order Nonlinear Optics in a Nanoporous Photonic Metamaterial