10 Microsc. Microanal. 27 (Suppl 1), 2021
doi:10.1017/S1431927621000611 © Microscopy Society of America 2021
Quantification of Structural Heterogeneities and Morphologies in Ultrathin Au-based
Nanowire Systems using 4D STEM and Electron Tomography
Alexandra Bruefach
1
, Audrey Von Raesfeld
1
and Mary Scott
2
1
Materials Science and Engineering, University of California, Berkeley, United States,
2
UC Berkeley,
Berkeley, California, United States
Hierarchical nanomaterial design has led to advances in numerous fields, including medicine, optics, and
catalysis [1,2,3]. Local crystallographic structures and morphologies govern these behaviors, thus
warranting deep investigation into how these structural variations impact these properties. Four-
dimensional scanning transmission electron microscopy (4D-STEM) provides a unique opportunity to
probe local crystal structure in diffraction space. This technique has the ability to provide a wealth of
information on materials with complex arrangements.
There have been several reports of metallic nanowires taking on complex structures based on the Boerdijk-
Coxeter-Bernal (BCB) helix [4,5,6]. These structures are comprised of multiple tetrahedral units packed
on their faces into an aperiodic helical structure. Most notably is the ultrathin (~2nm) Au-Ag based system
that rapidly twists into double helices upon induction with Pd, Pt, or Au salt [7]. These Au-Ag seed
structures are purported to exhibit a double-stranded BCB helical lattice, which shows indicative fan-like
contrast in EM imaging due to the presence of icosahedral packing [4,7]. Initially, it was proposed that
this material exhibits this mechanical response due to a lattice transformation from the BCB-type structure
to FCC, caused by the strain buildup of interfacial Pd deposition [7]. Recent reports show crystalline and
polycrystalline FCC Au-based nanowires with similar diameters also twist into double helices upon
induction with Ag or Pd salt [6,7]. Although the behavior is similar, these systems were proposed to twist
due to alloying effects leading to a lattice transformation towards the BCB-type structure. This intriguing
behavior and argued reaction mechanisms across multiple ultrathin Au-based systems warrants further
structural investigation. We demonstrate how this technique can be utilized to reveal population
differences between morphologically similar structures.
However, 4D STEM alone does not provide insight on 3-dimensional (3D) morphologies of
nanostructures, which is crucial for understanding catalytic behavior and unique optical behaviors, such
as circular dichroism [8]. Instead, Electron Tomography (ET) provides necessary information regarding
these 3D features such as curvature and surface morphology. Understanding these qualities is essential in
understanding and interpreting the diffraction data, which is dependent on 3D structure.
We use statistical measurements from 4D STEM scans to understand crystallographic information that is
not obtainable through nanoscale electron tomography, while recovering important morphological
information such as curvature using nanoscale tomography. These two techniques, when interpreted
collectively, provide a wealth of information revealing the crystal structure and morphology of the
underlying twisted wire. These results allow for the mechanical transformation to be understood.
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