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Lattice Mismatch in Crystalline Nanoparticle Thin Films

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† Department of Materials Science and Engineering, Massachusetts Institute of Technology (MIT), 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
‡ § ∥ ⊥ ‡Department of Chemistry, §International Institute for Nanotechnology, ∥Department of Chemical and Biological Engineering, and ⊥Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States
*E-mail: [email protected]
*E-mail: [email protected]
Cite this: Nano Lett. 2018, 18, 1, 579–585
Publication Date (Web):December 22, 2017
https://doi.org/10.1021/acs.nanolett.7b04737
Copyright © 2017 American Chemical Society
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    Abstract

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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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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.7b04737.

    • Experimental procedures, including interaction potential calculations, oligonucleotide sequences, nanoparticle functionalization and assembly, substrate preparation, characterization/analysis techniques (SEM, SAXS, FIB cross-sectioning, and AFM) (PDF), and FIB cross sections (TIF)

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