Abstract

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. This nonlinear optics is compared to the one achieved in corona-poled polymer films containing the identical chromophores. It originates in the confinement-induced orientational order of the elongated guest molecules in the nanochannels. This leads to a non-centrosymmetric dipolar order and hence to a nonlinear light–matter interaction on the sub-wavelength, single-pore scale. Our study demonstrates that the advent of large-scale, self-organized nanoporosity in monolithic solids along with the 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.

© 2021 Optical Society of America

Enhanced nonlinearities in hybrid structure based on nanoporous membrane and a metallohelicate with promising application in nanophotonics and NLO

Karolina Waszkowska, Yohan Cheret, Dominique Guichaoua, Théo Travers, Abdelkrim El-Ghayoury, Denis Gindre, Petra Göring, Monika Lelonek, Anatoliy Andrushchak, Irina Goncharova, and Bouchta Sahraoui
Opt. Lett. 48(11) 2897-2900 (2023)

Anisotropic second-harmonic generation from monocrystalline gold flakes

Sergejs Boroviks, Torgom Yezekyan, Álvaro Rodríguez Echarri, F. Javier García de Abajo, Joel D. Cox, Sergey I. Bozhevolnyi, N. Asger Mortensen, and Christian Wolff
Opt. Lett. 46(4) 833-836 (2021)

Electrically poled vapor-deposited organic glasses for integrated electro-optics

Lauren Dallachiesa and Ivan Biaggio
Opt. Lett. 47(8) 1924-1927 (2022)

Atomic layer deposited second-order nonlinear optical metamaterial for back-end integration with CMOS-compatible nanophotonic circuitry

Stéphane Clemmen, Artur Hermans, Eduardo Solano, Jolien Dendooven, Kalle Koskinen, Martti Kauranen, Edouard Brainis, Christophe Detavernier, and Roel Baets
Opt. Lett. 40(22) 5371-5374 (2015)

Second-order nonlinearity induced transparency

Y. H. Zhou, S. S. Zhang, H. Z. Shen, and X. X. Yi
Opt. Lett. 42(7) 1289-1292 (2017)