Journal
NANO LETTERS
Volume 18, Issue 1, Pages 579-585Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b04737
Keywords
Nanoparticle; self-assembly; epitaxy; thin film; lattice mismatch
Categories
Funding
- Air Force Office of Scientific Research [FA9550-16-1-0150, FA9950-17-1-0348, FA9550-17-1-0288]
- Vannevar Bush Faculty Fellowship program - Basic Research Office of the Assistant Secretary of Defense for Research and Engineering
- Office of Naval Research [N00014-15-1-0043]
- Center for Bio-Inspired Energy Science, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0000989]
- U.S. DOE Office of Science User Facility [DE-AC02-06CH11357]
- MRSEC Program under National Science Foundation [DMR-1419807]
- National Science Foundation [DMR-1121262]
- NSF Graduate Research Fellowship Program [NSF 1122374]
- Center for Computation and Theory of Soft Materials Fellowship
- NSF Graduate Research Fellowship
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For atomic thin films, lattice mismatch during heteroepitaxy leads to an accumulation of strain energy, generally causing the films to irreversibly deform and generate defects. In contrast, more elastically malleable building blocks should be better able to accommodate this mismatch and the resulting strain. Herein, that hypothesis is tested by utilizing DNA-modified nanoparticles as soft, programmable atom equivalents to grow a heteroepitaxial colloidal thin film. Calculations of interaction potentials, small-angle X-ray scattering data, and electron microscopy images show that the oligomer corona surrounding a particle core can deform and rearrange to store elastic strain up to +/- 7.7% lattice mismatch, substantially exceeding the +/- 1% mismatch tolerated by atomic thin films. Importantly, these DNA-coated particles dissipate strain both elastically through a gradual and coherent relaxation/broadening of the mismatched lattice parameter and plastically (irreversibly) through the formation of dislocations or vacancies. These data also suggest that the DNA cannot be extended as readily as compressed, and thus the thin films exhibit distinctly different relaxation behavior in the positive and negative lattice mismatch regimes. These observations provide a more general understanding of how utilizing rigid building blocks coated with soft compressible polymeric materials can be used to control nano- and microstructure.
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