Cornell University
Library
Cornell UniversityLibrary

eCommons

Help
Log In(current)
  1. Home
  2. Cornell University Graduate School
  3. Cornell Theses and Dissertations
  4. Atomic-scale Analysis of Defects in Battery Materials through Bayesian-Optimized Electron Ptychography

Atomic-scale Analysis of Defects in Battery Materials through Bayesian-Optimized Electron Ptychography

Access Restricted

Access to this document is restricted. Some items have been embargoed at the request of the author, but will be made publicly available after the "No Access Until" date.

During the embargo period, you may request access to the item by clicking the link to the restricted file(s) and completing the request form. If we have contact information for a Cornell author, we will contact the author and request permission to provide access. If we do not have contact information for a Cornell author, or the author denies or does not respond to our inquiry, we will not be able to provide access. For more information, review our policies for restricted content.

File(s)
Yoon_cornellgrad_0058F_15308.pdf (18.24 MB)
No Access Until
2028-01-08
Permanent Link(s)
https://doi.org/10.7298/3wbm-ps17
https://hdl.handle.net/1813/121014
Collections
Cornell Theses and Dissertations
Author
Yoon, Dasol
Abstract

A long-standing challenge in battery research is understanding lithium diffusion mechanisms at the atomic scale. Direct imaging of lithium is difficult because it is a light element and highly sensitive to radiation damage. Yet, atomic-resolution imaging is essential for identifying local defects and structural variations that strongly influence battery performance. While some conventional scanning transmission electron microscopy (STEM) methods can resolve both light and heavy elements in such materials, they are generally limited to two-dimensional projections. In this work, we demonstrate that multislice electron ptychography (MEP) captures three-dimensional structural information in a dose-efficient manner, while also providing higher resolution imaging of both light and heavy elements in a lithium-ion cathode. Using the depth-sectioning capability of MEP, we directly visualize lithium vacancy clusters buried within the cathode at the level of individual lithium columns. This capability to track lithium distributions in three dimensions will be crucial for advancing our understanding of battery charging mechanisms and guiding future material improvements. While these results highlight the potential of MEP for studying battery materials, practical challenges remain in its application. For beam-sensitive battery materials, conventional tilting to crystallographic zone axes is taxing and often impractical, particularly when samples contain multiple grains or drift due to instabilities of cryogenic holders. Small mistilts can, in principle, be corrected during MEP reconstruction, but solving for tilt alongside hundreds of other reconstruction parameters frequently leads to convergence failures or requires extensive simulations. Because MEP reconstruction is already computationally intensive, this creates a significant bottleneck. To address this challenge, we developed a workflow that incorporates Bayesian optimization of composite functions (BOCF) to robustly estimate specimen tilt and thickness from position-averaged convergent beam electron diffraction (PACBED) patterns. BOCF reliably converges in the complex three-parameter space and achieves objective values that are orders of magnitude better than conventional BO strategies. Notably, it reduces the computational demand to only several tens of simulations, in contrast to convolutional neural networks that require thousands that are restricted to specific experimental conditions and material systems. We also demonstrate that the optimized parameters can indeed correct specimen mistilts in MEP reconstructions, resulting in clearly resolved atom columns. By making previously unusable tilted datasets accessible, the method enhances the overall throughput of MEP and relaxes experimental constraints not only for beam-sensitive materials but also for other systems in general.

Description
73 pages
Date Issued
2025-12
Keywords
Battery
•
Bayesian Optimization
•
Defect Analysis
•
Electron Microscopy
•
Ptychography
•
Vacancy
Committee Chair
Muller, David
Committee Member
Abruna, Hector
Matteson, David
Degree Discipline
Materials Science and Engineering
Degree Name
Ph. D., Materials Science and Engineering
Degree Level
Doctor of Philosophy
Type
dissertation or thesis

Site Statistics | Help

About eCommons | Policies | Terms of use | Contact Us

copyright © 2002-2026 Cornell University Library | Privacy | Web Accessibility Assistance