Programming the Nonlinear Optics of a Nanoporous Photonic Metamaterial by Confined Crystallization
Abstract
A membrane traversed by a dense array of nanochannels acts as a photonic metamaterial: with channels far smaller than the wavelength of light, the optical response is set by the architecture rather than by the constituent materials. Here each nanochannel is turned into a nonlinear optical meta-atom by filling anodic aluminum oxide (AAO) with benzil (BZL), a noncentrosymmetric molecular crystal, and the crystallization pathway programs their orientation. In free-standing membranes every channel solidifies independently, the orientations remain uncorrelated, and the effective second-harmonic generation (SHG) response is nearly polarization isotropic; its magnitude follows a core - shell model in which an optically inactive interfacial layer of 2.6 nm reduces the active volume of each meta-atom, reproducing on bare alumina the value previously found on alkyl-grafted silica and indicating a host-insensitive limit. Seeding crystallization from a bulk benzil layer instead aligns the meta-atoms over submillimeter domains and produces a macroscopically anisotropic effective susceptibility. Channel diameters from 32 to 270 nm span the transition out of the subwavelength regime, and the anomalous directional SHG emission reported here is confined to the metamaterial limit. Confined crystallization thus offers a route to nonlinear optical metamaterials whose effective susceptibility tensor is written during processing.
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BibTeX
@misc{maxym2026programming,
title = {{Programming the Nonlinear Optics of a Nanoporous Photonic Metamaterial by Confined Crystallization}},
author = {Andrii Z. Maxym and Junhui Lang and Bouchta Sahraoui and Anatoliy S. Andrushchak and Yaroslav Shchur and Olha Kityk and Robert Wielgosz and Monika Lelonek and Piotr Pawlik and Patrick Huber and Jaroslaw Jedryka and Andriy V. Kityk},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.22801},
eprint = {2610.22801},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.22801},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Programming the Nonlinear Optics of a Nanoporous Photonic Metamaterial by Confined Crystallization
AU - Andrii Z. Maxym
AU - Junhui Lang
AU - Bouchta Sahraoui
AU - Anatoliy S. Andrushchak
AU - Yaroslav Shchur
AU - Olha Kityk
AU - Robert Wielgosz
AU - Monika Lelonek
AU - Piotr Pawlik
AU - Patrick Huber
AU - Jaroslaw Jedryka
AU - Andriy V. Kityk
PY - 2026
DA - 2026/10/16
PB - arXiv
DO - 10.48550/arxiv.2610.22801
UR - https://arxiv.org/abs/2610.22801
AB - A membrane traversed by a dense array of nanochannels acts as a photonic metamaterial: with channels far smaller than the wavelength of light, the optical response is set by the architecture rather than by the constituent materials. Here each nanochannel is turned into a nonlinear optical meta-atom by filling anodic aluminum oxide (AAO) with benzil (BZL), a noncentrosymmetric molecular crystal, and the crystallization pathway programs their orientation. In free-standing membranes every channel solidifies independently, the orientations remain uncorrelated, and the effective second-harmonic generation (SHG) response is nearly polarization isotropic; its magnitude follows a core - shell model in which an optically inactive interfacial layer of 2.6 nm reduces the active volume of each meta-atom, reproducing on bare alumina the value previously found on alkyl-grafted silica and indicating a host-insensitive limit. Seeding crystallization from a bulk benzil layer instead aligns the meta-atoms over submillimeter domains and produces a macroscopically anisotropic effective susceptibility. Channel diameters from 32 to 270 nm span the transition out of the subwavelength regime, and the anomalous directional SHG emission reported here is confined to the metamaterial limit. Confined crystallization thus offers a route to nonlinear optical metamaterials whose effective susceptibility tensor is written during processing.
ER -