van der Waals-Guided Nanopatterning Perovskite Nanocrystal Superlattices for Active Light-Emitting Metasurfaces
7 affiliations
- 1Institute for Chemical and Bioengineering
- 2ETH Zürich
- 3Department of Chemical Engineering
- 4Indian Institute of Science
- 5Laboratory for Nanometallurgy
- 6School of Integrated Circuits
- 7Huazhong University of Science and Technology
Abstract
High-resolution nanopatterning of self-assembled colloidal nanocrystal superlattices is crucial for their integration into miniaturized devices and integrated photonics. However, conventional top-down lithography often compromises supercrystallinity and dissolves constituent nanocrystals. Here, we introduce a non-destructive, bottom-up approach for the site-specific nucleation and growth of perovskite superlattices. Guided by the Lifshitz theory of van der Waals forces, we engineer a sharp permittivity contrast within nanotemplates to manipulate localized dewetting dynamics. This tailored interaction landscape establishes deep thermodynamic sinks that selectively drive the site-specific nucleation of CsPbBr3 nanocrystals. Corroborated by molecular dynamics simulations, we reveal that these dynamic energy sinks strictly restrict the rotational degrees of freedom of incoming nanocrystals, ultimately promoting highly ordered, face-to-face superlattice packing. This approach yields uniform, large-area arrays with subwavelength feature sizes and periodicities down to 200 and 350 nanometers, respectively, achieving an unprecedented array density exceeding 8 x 106 mm-2. Deterministic control over superlattice dimensions and array periodicity enables precise momentum-space engineering of radiation patterns, realizing highly directional light-emitting metasurfaces with an ultranarrow beam divergence of only 8.5°. Finally, we demonstrate the monolithic integration of these arrays into subwavelength electrically-driven active light-emitting metasurfaces, unlocking robust on-chip light modulation. This work establishes a robust pathway for translating the extraordinary properties of perovskite superlattices into next-generation on-chip nanophotonics.
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BibTeX
@misc{carretta2026waalsguided,
title = {{van der Waals-Guided Nanopatterning Perovskite Nanocrystal Superlattices for Active Light-Emitting Metasurfaces}},
author = {Donato Maria Carretta and Zhan-Hong Lin and Gianluca Vagli and Sunil B. Shivarudraiah and Jiwoo Oh and Abhijit Gogoi and Marcello Pozzi and Tommaso Marcato and Shuangshuang Zeng and Ananth Govind Rajan and Chih-Jen Shih},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15008892/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008892/v1},
note = {CC BY-NC-ND},
}
RIS
TY - UNPB
TI - van der Waals-Guided Nanopatterning Perovskite Nanocrystal Superlattices for Active Light-Emitting Metasurfaces
AU - Donato Maria Carretta
AU - Zhan-Hong Lin
AU - Gianluca Vagli
AU - Sunil B. Shivarudraiah
AU - Jiwoo Oh
AU - Abhijit Gogoi
AU - Marcello Pozzi
AU - Tommaso Marcato
AU - Shuangshuang Zeng
AU - Ananth Govind Rajan
AU - Chih-Jen Shih
PY - 2026
DA - 2026/09/15
PB - ChemRxiv
DO - 10.26434/chemrxiv.15008892/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008892/v1
AB - High-resolution nanopatterning of self-assembled colloidal nanocrystal superlattices is crucial for their integration into miniaturized devices and integrated photonics. However, conventional top-down lithography often compromises supercrystallinity and dissolves constituent nanocrystals. Here, we introduce a non-destructive, bottom-up approach for the site-specific nucleation and growth of perovskite superlattices. Guided by the Lifshitz theory of van der Waals forces, we engineer a sharp permittivity contrast within nanotemplates to manipulate localized dewetting dynamics. This tailored interaction landscape establishes deep thermodynamic sinks that selectively drive the site-specific nucleation of CsPbBr3 nanocrystals. Corroborated by molecular dynamics simulations, we reveal that these dynamic energy sinks strictly restrict the rotational degrees of freedom of incoming nanocrystals, ultimately promoting highly ordered, face-to-face superlattice packing. This approach yields uniform, large-area arrays with subwavelength feature sizes and periodicities down to 200 and 350 nanometers, respectively, achieving an unprecedented array density exceeding 8 x 106 mm-2. Deterministic control over superlattice dimensions and array periodicity enables precise momentum-space engineering of radiation patterns, realizing highly directional light-emitting metasurfaces with an ultranarrow beam divergence of only 8.5°. Finally, we demonstrate the monolithic integration of these arrays into subwavelength electrically-driven active light-emitting metasurfaces, unlocking robust on-chip light modulation. This work establishes a robust pathway for translating the extraordinary properties of perovskite superlattices into next-generation on-chip nanophotonics.
ER -