Resolving the Atomic Structure of Sequential Infiltration Synthesis Derived Inorganic Clusters.
basic_science · Level V
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- Record sourced from PubMed, PMID 33170644.
- Also identified by DOI 10.1021/acsnano.0c03848.
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Abstract
Sequential infiltration synthesis (SIS) is a route to the precision deposition of inorganic solids in analogy to atomic layer deposition but occurs within (vs upon) a soft material template. SIS has enabled exquisite nanoscale morphological complexity in various oxides through selective nucleation in block copolymers templates. However, the earliest stages of SIS growth remain unresolved, including the atomic structure of nuclei and the evolution of local coordination environments, before and after polymer template removal. We employed In K-edge extended X-ray absorption fine structure and atomic pair distribution function analysis of high-energy X-ray scattering to unravel (1) the structural evolution of InO<sub><i>x</i></sub>H<sub><i>y</i></sub> clusters inside a poly(methyl methacrylate) (PMMA) host matrix and (2) the formation of porous In<sub>2</sub>O<sub>3</sub> solids (obtained after annealing) as a function of SIS cycle number. Early SIS cycles result in InO<sub><i>x</i></sub>H<sub><i>y</i></sub> cluster growth with high aspect ratio, followed by the formation of a three-dimensional network with additional SIS cycles. That the atomic structures of the InO<sub><i>x</i></sub>H<sub><i>y</i></sub> clusters can be modeled as multinuclear clusters with bonding patterns related to those in In<sub>2</sub>O<sub>3</sub> and In(OH)<sub>3</sub> crystal structures suggests that SIS may be an efficient route to 3D arrays of discrete-atom-number clusters. Annealing the mixed inorganic/polymer films in air removes the PMMA template and consolidates the as-grown clusters into cubic In<sub>2</sub>O<sub>3</sub> nanocrystals with structural details that also depend on SIS cycle number.