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We report on the first DNA-based route towards monolayered free-standing nanoparticle superlattices

Free-standing nanoparticle superlattice sheets controlled by DNA.

NATURE MATERIALS, no. 6 (2009): 519.0-525

Cited by: 310|Views63
WOS NATURE

Abstract

Free-standing nanoparticle superlattices (suspended highly ordered nanoparticle arrays) are ideal for designing metamaterials and nanodevices free of substrate-induced electromagnetic interference. Here, we report on the first DNA-based route towards monolayered free-standing nanoparticle superlattices. In an unconventional way, DNA was u...More

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Introduction
  • Free-standing nanoparticle superlattices are ideal for designing metamaterials and nanodevices free of substrate-induced electromagnetic interference.
  • Structural characterization by transmission electron microscopy (TEM) revealed a smaller inter-particle spacing along the axis of stress relaxation than elsewhere in the sheets (Fig. 3b and Supplementary Fig. S3.1).
  • The authors further established that DNA number density and length are the dominant factors influencing inter-particle spacing—a key parameter that determines the collective properties of nanoparticle superlattices.
Highlights
  • Free-standing nanoparticle superlattices are ideal for designing metamaterials and nanodevices free of substrate-induced electromagnetic interference
  • The retained satellite microdroplets thinned, forming water films in which the motions of nanoparticles were spatially confined to two dimensions. This confinement, conceptually similar to our micromoulding approach[25], greatly improved the formation of high-quality nanoparticle superlattices with boundaries attached to the microhole edges
  • Sheets were formed exclusively in the microholes, with nanoparticles rarely observed on the surrounding substrate, as confirmed by further transmission electron microscopy (TEM) characterization. b, A higher-magnification TEM micrograph of a free-standing, monolayered sheet (DNA-T70) shows that nanoparticles are highly ordered yet well spaced, occupying only 18.53% of the total area
  • The inset shows a fast Fourier transform (FFT) of the image. c,d, 3D scanning TEM (STEM) tomography of a free-standing superlattice sheet (DNA-R) reveals that the sheet is both monolayered and flat. e, Characteristic AFM height image showing the presence of fully attached sheets (DNA-T70) and empty holes in the silicon nitride substrate. f, High-resolution AFM image of the surface of a fully attached sheet showing highly ordered nanoparticles. g, Cross-sectional height plot, corresponding to the dashed line in e, showing recessed sheets and an immeasurably deep hole in which no sheet formed
  • Structural characterization by transmission electron microscopy (TEM) revealed a smaller inter-particle spacing along the axis of stress relaxation than elsewhere in the sheets (Fig. 3b and Supplementary Fig. S3.1)
  • Each data point for the spring constant was the mean of force measurements on six different superlattice sheets for each DNA strand, with the standard deviation shown as error bars
Results
  • For both fully and partially attached monolayered sheets, a densely packed DNA corona is a prerequisite to obtain highly ordered arrays.
  • Green circles: measured DNA height between neighbouring nanoparticles in fully attached sheets.
  • Blue circles: measured DNA height along the axis of stress relaxation in partially attached sheets.
  • Free-standing nanoparticle superlattices in the fully dried state despite the absence of base-pairing forces.
  • Taking advantage of the wide-ranging length controllability of DNA, the authors demonstrated that inter-particle spacing for both the fully and partially attached sheets can be precisely and widely tuned by changing DNA length (Fig. 4a–f).
  • It seems that the inter-particle spacing increases linearly with DNA length in both fully and partially attached sheets (Fig. 5).
  • Owing to the highly flexible nature of ssDNA, the compliant DNA corona was substantially deformed in the interstices between nanoparticles during the formation of superlattice sheets.
  • For gold nanoparticles the authors observed colour variations of sheets from blue to pink under white light illumination (Fig. 6a, b) as inter-particle spacing was varied.
  • Inter-particle spacing a,b, Representative photographic images of different sheets formed using ligands DNA-T5 and DNA-T30, which were acquired in transmission mode under white light illumination.
  • Each data point for the spring constant was the mean of force measurements on six different superlattice sheets for each DNA strand, with the standard deviation shown as error bars.
Conclusion
  • The authors plotted the plasmon shift versus inter-particle spacing along the axis of stress relaxation, which resembled an exponential decay (Fig. 6e).
  • The authors compared the spring constants in the linear regime, k = dF /dδ, of pre-strained superlattice sheets with different DNA length.
  • The partially attached sheets in micrometre-sized holes exhibited slight deformation at higher magnifications owing to high beam currents.
Funding
  • This work is partially supported by NYSTAR and the NSF CAREER award (grant number: 0547330)
  • We acknowledge the use of the facilities of the Cornell Centre for Materials Research, which is supported through NSF Grant DMR 0520404, part of the NSF MRSEC Program
  • D.A.M. and J.J.C. acknowledge financial support from IRG-1 of NSF-MRSEC (CCMR)
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