Topological Engineering of Metal-Organic Architectures for Tunable Ultrafast Nonlinear Optical Responses
Abstract
Advances in nonlinear optical (NLO) materials are central to the development of ultrafast photonic and optoelectronic technologies, where macroscopic response is strongly governed by chromophore geometry and orientational order. Here, we employ mechanically non-trivial metal-organic architectures as a molecular engineering strategy to impose and stabilize threedimensional chromophore arrangements, enabling systematic tuning of ultrafast second-and third-order NLO responses. The NLO response of two types of topologically non-trivial complexes, namely [2]catenates ([2]C) and trefoil knots (TK), based on Zn(II) and Cd(II) centers are investigated in guest-host PMMA thin films and nanoconfined environments. Pyrene-functionalized Zn(II)-based architectures exhibit pronounced second-and thirdharmonic generation (SHG and THG, respectively), reaching first and second hyperpolarizabilities up to β of 43.66 × 10 -38 m 4 V -1 and 102.67 × 10 -47 m 5 V -2 highlighting the role of extended π-conjugation and intramolecular charge transfer. Z-scan measurements reveal self-focusing behavior and architecture-dependent refractive index modulation. Incorporation of these architectures into nanoporous alumina membranes leads to a marked enhancement of SHG relative to thin films, consistent with the combined effects of nanoscale confinement and partial orientational ordering induced within the nanoporous environment. These results establish mechanically non-trivial metal-organic architectures as versatile platforms in which molecular topology, metal coordination, and ligand-centered electronic structure collectively govern ultrafast NLO response.
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BibTeX
@article{waszkowska2026topological,
title = {{Topological Engineering of Metal-Organic Architectures for Tunable Ultrafast Nonlinear Optical Responses}},
author = {Karolina Waszkowska and Thirumurugan Prakasam and Nowshin Kabir and Abdelkrim El-Ghayoury and Anna Zawadzka and Monika Lelonek and Carlos Platas-Iglesias and Mourad Elhabiri and Ali Trabolsi and Bouchta Sahraoui},
journal = {Advanced Optical Materials},
year = {2026},
month = aug,
doi = {10.1002/adom.71518},
url = {https://hal.science/hal-05839614v1},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Topological Engineering of Metal-Organic Architectures for Tunable Ultrafast Nonlinear Optical Responses
AU - Karolina Waszkowska
AU - Thirumurugan Prakasam
AU - Nowshin Kabir
AU - Abdelkrim El-Ghayoury
AU - Anna Zawadzka
AU - Monika Lelonek
AU - Carlos Platas-Iglesias
AU - Mourad Elhabiri
AU - Ali Trabolsi
AU - Bouchta Sahraoui
PY - 2026
DA - 2026/08/08
JO - Advanced Optical Materials
DO - 10.1002/adom.71518
UR - https://hal.science/hal-05839614v1
AB - Advances in nonlinear optical (NLO) materials are central to the development of ultrafast photonic and optoelectronic technologies, where macroscopic response is strongly governed by chromophore geometry and orientational order. Here, we employ mechanically non-trivial metal-organic architectures as a molecular engineering strategy to impose and stabilize threedimensional chromophore arrangements, enabling systematic tuning of ultrafast second-and third-order NLO responses. The NLO response of two types of topologically non-trivial complexes, namely [2]catenates ([2]C) and trefoil knots (TK), based on Zn(II) and Cd(II) centers are investigated in guest-host PMMA thin films and nanoconfined environments. Pyrene-functionalized Zn(II)-based architectures exhibit pronounced second-and thirdharmonic generation (SHG and THG, respectively), reaching first and second hyperpolarizabilities up to β of 43.66 × 10 -38 m 4 V -1 and 102.67 × 10 -47 m 5 V -2 highlighting the role of extended π-conjugation and intramolecular charge transfer. Z-scan measurements reveal self-focusing behavior and architecture-dependent refractive index modulation. Incorporation of these architectures into nanoporous alumina membranes leads to a marked enhancement of SHG relative to thin films, consistent with the combined effects of nanoscale confinement and partial orientational ordering induced within the nanoporous environment. These results establish mechanically non-trivial metal-organic architectures as versatile platforms in which molecular topology, metal coordination, and ligand-centered electronic structure collectively govern ultrafast NLO response.
SN - 2195-1071
ER -