Abstract
Colloidal cocrystallization enables the formation of multicomponent materials with unique physicochemical properties, yet the role of nanoparticle (NP) shape and specific ligand interactions to cocrystallize anisotropic and isotropic NPs, with order and correlated disorder, remains underexplored. Here, geometry-inspired strategies along with programmable DNA interactions are combined to achieve structural control of colloidal cocrystal assemblies. Coassembling polyhedral and spherical NPs with complementary DNA yields two classes of cocrystals: one where both components order, and another where polyhedral NPs form a periodic lattice, while spherical NPs remain disordered but spatially correlated with polyhedral edges and corners. The size ratio of the building blocks can be used to control the ordering of spherical NPs—smaller octahedral-to-sphere size ratios favor fully ordered cocrystals. Molecular dynamics simulations further elucidate the role of NP shapes and dimensions in the structural outcome of the cocrystal. This work provides a framework for deliberately targeting and accessing crystals with exotic multicomponent structures.
| Original language | English (US) |
|---|---|
| Article number | eadu4919 |
| Journal | Science Advances |
| Volume | 11 |
| Issue number | 16 |
| DOIs | |
| State | Published - Apr 18 2025 |
Funding
We thank these individuals from the University of Michigan for helpful discussions: K. Je, S.-T . Tsai, A. Lee, and J. A. Anderson. This material is based on work supported by the Air Force Office of Scientific Research award FA9550-22- 1- 0300. This work made use of the EPIC facility (RRID: SCR_026361) of Northwestern University\u2019s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECC S-2025633); the MRSEC program (NSF DMR-2308691) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. This material is based on work supported by the Department of the Navy, Office of Naval Research under ONR award number N00014-18- 1- 2497 (assembly simulations). This research used computational resources and services supported by Advanced Research Computing at the University of Michigan, Ann Arbor, and used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation Grant ACI-1548562 (XSEDE award DMR 140129). This research used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science user facility at Argonne National Laboratory and is based on research supported by the US DOE Office of Science-Basic Energy Sciences, under contract no. DE-AC02- 06CH11357. This work made use of the BioCryo facility (RRID:SCR_021288) of Northwestern University\u2019s NUANCE Center, which has received support from the SHyNE Resource (NSF ECC S-2025633), the IIN, and Northwestern\u2019s MRSEC program (NSF DMR-2308691).
ASJC Scopus subject areas
- General