Science - USA (2022-04-08)

complex organization where 15-nm AuNPs
were encapsulated in tetrahedra that were as-
sembled in a diamond lattice (Fig. 4A) through
inter-vertex bonds ( 14 ). We used this super-
lattice to create a multimaterial (iron/silica/
platinum) continuous framework based on
the tetrahedron motif while preserving nano-
particle placements. Such complex inorganic
structures are desirable for diverse material
applications and present an important chal-
lenge for visualization. After assembling the
diamond lattice, we templated the DNA frame-
work by absorption of iron ions into the
charged DNA backbone, followed by silicifica-
tion and platinum coating. The elemental sen-
sitivity and spatial acuity of our imaging
allowed us to produce gold, iron, and platinum
maps (Fig. 4B) of the continuous framework.
We then reconstructed these 3D multimaterial
frameworks and AuNP lattice (Fig. 4C), where
a close correspondence to a model structure
was observed. This approach clearly shows the
relation between the nanoparticles and the
tetrahedra motif, for both global and local
arrangements. The platinum and iron coat-
ings offer a complete view into the framework
and complement each other where either plat-
inum or iron did not coat fully (movie S6 and
figs. S19 and S20).
The developed methods make it possible to
create DNA-prescribed discrete and continuous
inorganic lattices that can find use in catalyt-
ical, optical, and energy material applications.
The demonstrated characterization approach
will provide unprecedented opportunities to

understand and perfect a broad range of self-

assembled nanomaterials.

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ACKNOWLEDGMENTS

We thank the Imaging Facility of CUNY Advanced Science Research

Center for instrument use and technical assistance. This research

used resources of the Center for Functional Nanomaterials and

the Hard X-ray Nanoprobe Beamline (HXN) at 3-ID. Small-angle

scattering was collected at the Complex Matter Scattering (CMS)

instrument at 11-BM and Soft Matter Interfaces (SMI) at 12-ID of the

National Synchrotron Light Source II, which are part of the US

Department of Energy, Office of Science facilities at Brookhaven

National Laboratory under contract DE-SC0012704.Funding:The

DNA-assembly work and defect analysis were supported by the

US Department of Energy, Office of Basic Energy Sciences, grant

DE-SC0008772. The inorganic templating and structural analysis

work were supported by the US Department of Defense, Army

Research Office, W911NF-19-1-0395.Author contributions:A.M.,

H.Y., and O.G. conceived and designed the experiments. A.M.

performed the assembly and mineralization experiments. A.M., B.M.,

H.Y., and X.H. prepared and contributed to sample preparation

for the beamline. A.M., H.Y., X.H., and Y.S.C. performed SHXM

experiments and assisted in data preparation. A.M., H.Y., and H.E.

performed data processing and analysis. A.M., H.Y., and O.G.

wrote the paper. O.G. and H.Y. supervised the project. All authors

discussed the results, assisted with assembling figures, and

reviewed or edited the manuscript.Competing interests:The

authors claim no competing InterestsData and materials

availability:Synchrotron data files will be made available upon

reasonable request to the corresponding authors. Ptychography

( 26 ) and PyXRF ( 31 ) software packages are available via GitHub

https://github.com/NSLS-II/ptycho_gui, https://github.com/

NSLS-II/PyXRF. All data needed to evaluate the conclusions are

present in the paper and the supplementary materials.

SUPPLEMENTARY MATERIALS

science.org/doi/10.1126/science.abk0463

Materials and Methods

Supplementary Text

Figs. S1 to S25

Movies S1 to S6

References ( 32 – 35 )

28 June 2021; accepted 8 March 2022

10.1126/science.abk0463

SCIENCEscience.org 8 APRIL 2022¥VOL 376 ISSUE 6589 207

Fig. 4. Multielement continuous
framework with embedded nano-
particles based on a diamond
superlattice assembled from tetra-
hedron motifs.(A) Model of a
diamond unit cell with
complementary DNA–encoded tetra-
hedra in red and gray with nano-
particles inset, multielement
templated (teal) framework of tetra-
hedra, and zoom-in of the templated
tetrahedra with iron internal along
the DNA structure, silica and
platinum outer coating. (B) 3D
reconstructed slice with Au, Fe, and
Pt channels along with a composite
image demonstrating the particle/
matrix visibility, directly showing
particle-to-particle bonds. Scale bars,
100 nm. (C) 3D model alongside
3D reconstructed data with
segmented representation of the
continuous framework formed
by Fe/silica/Pt tetrahedra and
Au nanoparticles.

Au

Fe

Pt

Fe Au Pt

Fe/DNA

Silica

Pt

Fe Au Pt

100nm

B

C

A

86 nm

Framework templating

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