TY - JOUR
T1 - Comprehensive view of microscopic interactions between DNA-coated colloids
AU - Cui, Fan
AU - Marbach, Sophie
AU - Zheng, Jeana Aojie
AU - Holmes-Cerfon, Miranda
AU - Pine, David J.
N1 - Funding Information:
We gratefully acknowledge Dr. Kaiyuan Yao for his help in the designing and building of our microscope. The authors are also indebted to Alexandre Morin for his guidance on zeta potential measurements to evaluate the thickness of polymer brushes, and to Stefano Angioletti-Uberti for numerous discussions on the binding part of the energy of interaction. The authors would further like to acknowledge fruitful discussions with Guillaume Dubach, Daan Frenkel, Jaeup Kim, Madhavi Krishnan, Bartolo M. Mognetti, and Shura Grosberg. S.M. acknowledges funding from the MolecularControl project, European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant award number 839225. S.M., M.H.-C., J.A.Z., and F.C. were supported in part by the MRSEC Program of the National Science Foundation under Award Number DMR-1420073. The research of F.C. and D.J.P. was primarily supported by the US Department of Energy DE-SC0007991 for the initiation and design of the TIRM experiments. Additional support for F.C. and D.J.P. was provided by the US Army Research Office under award number W911NF-17-1-0328. M.H.-C. was partially supported by the US Department of Energy under Award No. DE-SC0012296, and acknowledges support from the Alfred P. Sloan Foundation.
Publisher Copyright:
© 2022, The Author(s).
PY - 2022/12
Y1 - 2022/12
N2 - The self-assembly of DNA-coated colloids into highly-ordered structures offers great promise for advanced optical materials. However, control of disorder, defects, melting, and crystal growth is hindered by the lack of a microscopic understanding of DNA-mediated colloidal interactions. Here we use total internal reflection microscopy to measure in situ the interaction potential between DNA-coated colloids with nanometer resolution and the macroscopic melting behavior. The range and strength of the interaction are measured and linked to key material design parameters, including DNA sequence, polymer length, grafting density, and complementary fraction. We present a first-principles model that screens and combines existing theories into one coherent framework and quantitatively reproduces our experimental data without fitting parameters over a wide range of DNA ligand designs. Our theory identifies a subtle competition between DNA binding and steric repulsion and accurately predicts adhesion and melting at a molecular level. Combining experimental and theoretical results, our work provides a quantitative and predictive approach for guiding material design with DNA-nanotechnology and can be further extended to a diversity of colloidal and biological systems.
AB - The self-assembly of DNA-coated colloids into highly-ordered structures offers great promise for advanced optical materials. However, control of disorder, defects, melting, and crystal growth is hindered by the lack of a microscopic understanding of DNA-mediated colloidal interactions. Here we use total internal reflection microscopy to measure in situ the interaction potential between DNA-coated colloids with nanometer resolution and the macroscopic melting behavior. The range and strength of the interaction are measured and linked to key material design parameters, including DNA sequence, polymer length, grafting density, and complementary fraction. We present a first-principles model that screens and combines existing theories into one coherent framework and quantitatively reproduces our experimental data without fitting parameters over a wide range of DNA ligand designs. Our theory identifies a subtle competition between DNA binding and steric repulsion and accurately predicts adhesion and melting at a molecular level. Combining experimental and theoretical results, our work provides a quantitative and predictive approach for guiding material design with DNA-nanotechnology and can be further extended to a diversity of colloidal and biological systems.
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U2 - 10.1038/s41467-022-29853-w
DO - 10.1038/s41467-022-29853-w
M3 - Article
C2 - 35484104
AN - SCOPUS:85128948711
VL - 13
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 2304
ER -