Modulating the Bond Strength of DNA-Nanoparticle Superlattices

Soyoung E. Seo; Mary X. Wang; Chad M. Shade; Jessica L. Rouge; Keith A. Brown; Chad A. Mirkin

doi:10.1021/acsnano.5b07103

Modulating the Bond Strength of DNA-Nanoparticle Superlattices

Soyoung E. Seo, Mary X. Wang, Chad M. Shade, Jessica L. Rouge, Keith A. Brown, Chad A. Mirkin^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

44 Scopus citations

Abstract

A method is introduced for modulating the bond strength in DNA-programmable nanoparticle (NP) superlattice crystals. This method utilizes noncovalent interactions between a family of [Ru(dipyrido[2,3-a:3′,2′-c]phenazine)(N-N)₂]²⁺-based small molecule intercalators and DNA duplexes to postsynthetically modify DNA-NP superlattices. This dramatically increases the strength of the DNA bonds that hold the nanoparticles together, thereby making the superlattices more resistant to thermal degradation. In this work, we systematically investigate the relationship between the structure of the intercalator and its binding affinity for DNA duplexes and determine how this translates to the increased thermal stability of the intercalated superlattices. We find that intercalator charge and steric profile serve as handles that give us a wide range of tunability and control over DNA-NP bond strength, with the resulting crystal lattices retaining their structure at temperatures more than 50°C above what nonintercalated structures can withstand. This allows us to subject DNA-NP superlattice crystals to conditions under which they would normally melt, enabling the construction of a core-shell (gold NP-quantum dot NP) superlattice crystal.

Original language	English (US)
Pages (from-to)	1771-1779
Number of pages	9
Journal	ACS nano
Volume	10
Issue number	2
DOIs	https://doi.org/10.1021/acsnano.5b07103
State	Published - Feb 23 2016

Funding

We thank J. Griffin for helpful discussions and for providing coding expertise for curve fitting analysis. This material is based upon work supported by AFOSR Award FA9550-11-1-0275, and the Centers of Cancer Nanotechnology Excellence (CCNE) initiative of the National Institutes of Health (NIH) under Award U54 CA151880. SAXS experiments were carried out at Sector 5-ID of the DuPont-Northwestern-Dow Collaborative Access Team at the Advanced Photon Source. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work made use of the EPIC facility (NUANCE Center-Northwestern University), which has received support from the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN); and the State of Illinois, through the IIN. M. Wang gratefully acknowledges a Graduate Research Fellowship from the National Science Foundation (NSFGRFP) and a Northwestern University Ryan Fellowship. J. Rouge acknowledges a postdoctoral fellowship from the PhRMA foundation. K. Brown gratefully acknowledges support from Northwestern University''s International Institute for Nanotechnology.

Keywords

DNA
DNA intercalator
crystallization
nanoparticle
self-assembly

ASJC Scopus subject areas

General Engineering
General Materials Science
General Physics and Astronomy

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10.1021/acsnano.5b07103

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abstract = "A method is introduced for modulating the bond strength in DNA-programmable nanoparticle (NP) superlattice crystals. This method utilizes noncovalent interactions between a family of [Ru(dipyrido[2,3-a:3′,2′-c]phenazine)(N-N)2]2+-based small molecule intercalators and DNA duplexes to postsynthetically modify DNA-NP superlattices. This dramatically increases the strength of the DNA bonds that hold the nanoparticles together, thereby making the superlattices more resistant to thermal degradation. In this work, we systematically investigate the relationship between the structure of the intercalator and its binding affinity for DNA duplexes and determine how this translates to the increased thermal stability of the intercalated superlattices. We find that intercalator charge and steric profile serve as handles that give us a wide range of tunability and control over DNA-NP bond strength, with the resulting crystal lattices retaining their structure at temperatures more than 50°C above what nonintercalated structures can withstand. This allows us to subject DNA-NP superlattice crystals to conditions under which they would normally melt, enabling the construction of a core-shell (gold NP-quantum dot NP) superlattice crystal.",

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Modulating the Bond Strength of DNA-Nanoparticle Superlattices

Abstract

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Keywords

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