Abstract
Colloidal crystal engineering with DNA allows one to design diverse superlattices with tunable lattice symmetry, composition, and spacing. Most of these structures follow the complementary contact model, maximizing DNA hybridization on building blocks and producing relatively close-packed lattices. Here, low-symmetry kagome superlattices are assembled from DNA-modified gold bipyramids that can engage only in partial DNA surface matching. The bipyramid dimensions and DNA length can be engineered for two different superlattices with rhombohedral unit cells, including one composed of a periodic stacking of kagome lattices. Enabled by the partial facet alignment, the kagome lattices exhibit lattice distortion, bipyramid twisting, and planar chirality. When conjugated with Cy-5 dyes, the kagome lattices serve as cavities with high-density optical states and large Purcell factors along lateral directions, leading to strong dipole radiation along the z axis and facet-dependent light emission. Such complex optical properties make these materials attractive for lasers, displays, and quantum sensing constructs.
| Original language | English (US) |
|---|---|
| Article number | eadp3756 |
| Journal | Science Advances |
| Volume | 10 |
| Issue number | 29 |
| DOIs | |
| State | Published - Jul 2024 |
Funding
We acknowledge E. W. Roth (NU) for ultramicrotomy. This work used the EPIC and BioCryo facility of Northwestern University's 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. Leica SP8 confocal microscopy was used at the Biological Imaging Facility at Northwestern University (RRID:SCR_017767), supported by the Chemistry for Life Processes Institute, the NU Office for Research, the Department of Molecular Biosciences and the Rice Foundation. Funding: This material is based on work supported by the Air Force Office of Scientific Research under award FA9550-22- 1- 0300 (Au bipyramids synthesis and DNA functionalization, C.A.M. and K.A.) and as part of the Center for Bio-Inspired Energy Science, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC0000989 (assembly of Au bipyramids, modeling and simulation of bipyramid assembly, C.A.M. and S.C.G.). The assembly simulations were conducted on NCSA Delta and SDSC Expanse through allocation DMR 140129 (S.C.G.) from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCE SS) program, which is supported by National Science Foundation grant numbers 2138259, 2138286, 2138307, 2137603, and 2138296. S.C.G. was supported by a Vannevar Bush Faculty Fellowship sponsored by the Department of the Navy, Office of Naval Research under ONR award number N00014-22- 1- 2821. Author contributions: Z.L. synthesized and characterized the Au bipyramids, synthesized and purified the DNA strands, and assembled the nanoparticles and characterized the colloidal crystals; Y. Lim performed MD simulations of nanoparticle assembly and constructed the 3D models; I.T. performed the optical experiments and optical simulation. Z.L., W.Z., Y. Li and Y.Z. analyzed the colloidal crystals. Z.L., Y. Lim, I.T., S.C.G., K.A., and C.A.M. wrote the paper. S.C.G., K.A., and C.A.M. supervised the research. Competing interests: The authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Acknowledgments: We acknowledge e. W. Roth (nU) for ultramicrotomy. this work used the ePic and Biocryo facility of northwestern University\u2019s nUAnce center, which has received support from the Soft and hybrid nanotechnology experimental (Shyne) Resource (nSF eccS-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. Leica SP8 confocal microscopy was used at the Biological imaging Facility at northwestern University (RRid:ScR_017767), supported by the chemistry for Life Processes institute, the nU Office for Research, the department of Molecular Biosciences and the Rice Foundation. Funding: this material is based on work supported by the Air Force Office of Scientific Research under award FA9550-22-1-0300 (Au bipyramids synthesis and dnA functionalization, c.A.M. and K.A.) and as part of the center for Bio-inspired energy Science, an energy Frontier Research center funded by the U.S. department of energy, Office of Science, Basic energy Sciences under Award de-Sc0000989 (assembly of Au bipyramids, modeling and simulation of bipyramid assembly, c.A.M. and S.c.G.). the assembly simulations were conducted on ncSA delta and SdSc expanse through allocation dMR 140129 (S.c.G.) from the Advanced cyberinfrastructure coordination ecosystem: Services & Support (AcceSS) program, which is supported by national Science Foundation grant numbers 2138259, 2138286, 2138307, 2137603, and 2138296. S.c.G. was supported by a vannevar Bush Faculty Fellowship sponsored by the department of the navy, Office of naval Research under OnR award number n00014-22-1-2821. Author contributions: Z.L. synthesized and characterized the Au bipyramids, synthesized and purified the dnA strands, and assembled the nanoparticles and characterized the colloidal crystals; Y. Lim performed Md simulations of nanoparticle assembly and constructed the 3d models; i.t. performed the optical experiments and optical simulation. Z.L., W.Z., Y. Li and Y.Z. analyzed the colloidal crystals. Z.L., Y. Lim, i.t., S.c.G., K.A., and c.A.M. wrote the paper. S.c.G., K.A., and c.A.M. supervised the research. Competing interests: the authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials.
ASJC Scopus subject areas
- General