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PreprintCC BY 4.0arXiv

5DSTEM of Liquid-Phase Nanocrystal Growth Bridges Ensemble Kinetics and Nanoscale Dynamics

Abstract

Resolving how ensemble growth kinetics emerge from particle- and grain-level dynamics is essential for predictive control of nanocrystal synthesis. Here, time-resolved four-dimensional scanning transmission electron microscopy (4DSTEM), extended into five dimensions (5DSTEM) through continuous acquisition, is used to simultaneously resolve morphology, crystallographic orientation, and lattice strain during Au nanocrystal growth in aqueous HAuCl4. Although ensemble growth follows surface-reaction-limited kinetics, individual nanoparticles exhibit distinct pathways, including continuous growth and discrete coalescence through oriented attachment. These pathways display characteristic orientation dynamics, with stable or gradually selected orientations during continuous growth and abrupt reconfiguration followed by alignment during coalescence. At the ensemble level, the out-of-plane orientation distribution is established early and remains stable, whereas in-plane orientations remain broadly distributed without global alignment. Tensile strain develops progressively from particle surfaces and interfaces, directly linking lattice distortion with evolving morphology and crystallographic structure. By connecting ensemble kinetics with particle- and grain-resolved structural evolution, 5DSTEM provides a general framework for uncovering heterogeneous growth mechanisms and for relating synthesis pathways to structure-dependent properties in functional nanomaterials.

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BibTeX
@misc{lee20265dstem,
  title = {{5DSTEM of Liquid-Phase Nanocrystal Growth Bridges Ensemble Kinetics and Nanoscale Dynamics}},
  author = {Serin Lee and Colin Ophus and Jennifer Dionne},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.25549},
  eprint = {2609.25549},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.25549},
  note = {CC BY 4.0},
}
RIS
TY  - UNPB
TI  - 5DSTEM of Liquid-Phase Nanocrystal Growth Bridges Ensemble Kinetics and Nanoscale Dynamics
AU  - Serin Lee
AU  - Colin Ophus
AU  - Jennifer Dionne
PY  - 2026
DA  - 2026/09/22
PB  - arXiv
DO  - 10.48550/arxiv.2609.25549
UR  - https://arxiv.org/abs/2609.25549
AB  - Resolving how ensemble growth kinetics emerge from particle- and grain-level dynamics is essential for predictive control of nanocrystal synthesis. Here, time-resolved four-dimensional scanning transmission electron microscopy (4DSTEM), extended into five dimensions (5DSTEM) through continuous acquisition, is used to simultaneously resolve morphology, crystallographic orientation, and lattice strain during Au nanocrystal growth in aqueous HAuCl4. Although ensemble growth follows surface-reaction-limited kinetics, individual nanoparticles exhibit distinct pathways, including continuous growth and discrete coalescence through oriented attachment. These pathways display characteristic orientation dynamics, with stable or gradually selected orientations during continuous growth and abrupt reconfiguration followed by alignment during coalescence. At the ensemble level, the out-of-plane orientation distribution is established early and remains stable, whereas in-plane orientations remain broadly distributed without global alignment. Tensile strain develops progressively from particle surfaces and interfaces, directly linking lattice distortion with evolving morphology and crystallographic structure. By connecting ensemble kinetics with particle- and grain-resolved structural evolution, 5DSTEM provides a general framework for uncovering heterogeneous growth mechanisms and for relating synthesis pathways to structure-dependent properties in functional nanomaterials.
ER  -