Multivalent Cation-Induced Actuation of DNA-Mediated Colloidal Superlattices
Nanoparticles functionalized with DNA can assemble into ordered superlattices with defined crystal habits through programmable DNA “bonds”. Here, we examine the interactions of multivalent cations with these DNA bonds as a chemical approach for actuating colloidal superlattices. Multivalent cations alter DNA structure on the molecular scale, enabling the DNA “bond length” to be reversibly altered between 17 and 3 nm, ultimately leading to changes in the overall dimensions of the micrometer-sized superlattice. The identity, charge, and concentration of the cations each control the extent of actuation, with Ni2+ capable of inducing a remarkable >65% reversible change in crystal volume. In addition, these cations can increase “bond strength”, as evidenced by superlattice thermal stability enhancements of >60 °C relative to systems without multivalent cations. Molecular dynamics simulations provide insight into the conformational changes in DNA structure as the bond length approaches 3 nm and show that cations that screen the negative charge on the DNA backbone more effectively cause greater crystal contraction. Finally, taken together, the use of multivalent cations represents a powerful strategy to alter superlattice structure and stability, which can impact diverse applications through dynamic control of material properties, including the optical, magnetic, and mechanical properties.
- Research Organization:
- Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES); Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); AUS Air Force Office of Scientific Research (AFOSR); US Department of the Navy, Office of Naval Research (ONR); National Institutes of Health (NIH)
- Grant/Contract Number:
- SC0000989; AC02-06CH11357; N00014-15-1-0043; U54CA199091; FA8650-15-2-5518; FA9550-17-1-0348; ECCS-1542205
- OSTI ID:
- 1767664
- Journal Information:
- Journal of the American Chemical Society, Vol. 141, Issue 51; ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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