Chiral assemblies of pinwheel superlattices on substrates

Shan Zhou, Jiahui Li, Jun Lu, Haihua Liu, Ji-Young Kim, Ahyoung Kim, Lehan Yao, Chang Liu, Chang Qian, Zachary D. Hood, Xiaoying Lin, Wenxiang Chen, Thomas E. Gage, Ilke Arslan, Alex Travesset, Kai Sun, Nicholas A. Kotov () and Qian Chen ()
Additional contact information
Shan Zhou: University of Illinois at Urbana-Champaign
Jiahui Li: University of Illinois at Urbana-Champaign
Jun Lu: University of Michigan
Haihua Liu: Argonne National Laboratory
Ji-Young Kim: University of Michigan
Ahyoung Kim: University of Illinois at Urbana-Champaign
Lehan Yao: University of Illinois at Urbana-Champaign
Chang Liu: University of Illinois at Urbana-Champaign
Chang Qian: University of Illinois at Urbana-Champaign
Zachary D. Hood: Argonne National Laboratory
Xiaoying Lin: University of Illinois at Urbana-Champaign
Wenxiang Chen: University of Illinois at Urbana-Champaign
Thomas E. Gage: Argonne National Laboratory
Ilke Arslan: Argonne National Laboratory
Alex Travesset: Iowa State University and Ames Lab
Kai Sun: University of Michigan
Nicholas A. Kotov: University of Michigan
Qian Chen: University of Illinois at Urbana-Champaign

Nature, 2022, vol. 612, issue 7939, 259-265

Abstract: Abstract The unique topology and physics of chiral superlattices make their self-assembly from nanoparticles highly sought after yet challenging in regard to (meta)materials1–3. Here we show that tetrahedral gold nanoparticles can transform from a perovskite-like, low-density phase with corner-to-corner connections into pinwheel assemblies with corner-to-edge connections and denser packing. Whereas corner-sharing assemblies are achiral, pinwheel superlattices become strongly mirror asymmetric on solid substrates as demonstrated by chirality measures. Liquid-phase transmission electron microscopy and computational models show that van der Waals and electrostatic interactions between nanoparticles control thermodynamic equilibrium. Variable corner-to-edge connections among tetrahedra enable fine-tuning of chirality. The domains of the bilayer superlattices show strong chiroptical activity as identified by photon-induced near-field electron microscopy and finite-difference time-domain simulations. The simplicity and versatility of substrate-supported chiral superlattices facilitate the manufacture of metastructured coatings with unusual optical, mechanical and electronic characteristics.

Date: 2022
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DOI: 10.1038/s41586-022-05384-8

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