Search NASA⌕ Search
Home/Archive/DOE OSTI

DOE OSTI · 3382429

Atomic Evolution of Hydrogen Intercalation Wave Dynamics in Palladium Nanocrystals Revealed by Liquid-Phase Transmission Electron Microscopy

Lee, Daewon [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0009000038757963)·Oaks-Leaf, Sam [University of California, Berkeley, CA (United States)] (ORCID:0000000326180380)·Betzler, Sophia B. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Shi, Yifeng [Georgia Institute of Technology, Atlanta, GA (United States)]·Zhou, Siyu [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000159590541)·Ophus, Colin [Stanford University, CA (United States)]·Wang, Lin-Wang [Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0000000170612692)·Asta, Mark [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)]·Xia, Younan [Georgia Institute of Technology, Atlanta, GA (United States); Emory University, Atlanta, GA (United States)] (ORCID:0000000324317048)·Limmer, David T. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)] (ORCID:0000000227660688)·Zheng, Haimei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000338134170)
View original source ↗Read source document ↗Export metadata ↓

Abstract

Solute-intercalation-induced phase separation creates spatial heterogeneities in host materials, a phenomenon ubiquitous in batteries, hydrogen storage, and other energy devices. Despite many efforts, probing intercalation processes at the atomic scale has been a significant challenge. By utilizing liquid-phase transmission electron microscopy (TEM), we study hydrogen (de)intercalation in palladium nanocrystals as a model system and have achieved unprecedented atomic-resolution imaging of hydrogen intercalation wave dynamics. Our observations reveal that intercalation wave mechanisms, instead of shrinking-core mechanisms, prevail at ambient temperature for palladium nanocubes ranging from ∼60 nm down to ∼10 nm. Systematic image analysis uncovers the atomic evolution of the hydrogen intercalation wave, transitioning from nonplanar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate that the observed intercalation wave dynamics correspond to sorption pathways minimizing the lattice mismatch strain at the phase boundary. In conclusion, unveiling the atomic intercalation pathways holds profound implications for engineering intercalation-mediated devices and advancements in energy sciences.

Keep this discovery

BibTeXRIS

Lee, Daewon [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0009000038757963), Oaks-Leaf, Sam [University of California, Berkeley, CA (United States)] (ORCID:0000000326180380), Betzler, Sophia B. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Shi, Yifeng [Georgia Institute of Technology, Atlanta, GA (United States)], Zhou, Siyu [Georgia Institute of Technology, Atlanta, GA (United States)] (ORCID:0000000159590541), Ophus, Colin [Stanford University, CA (United States)], Wang, Lin-Wang [Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0000000170612692), Asta, Mark [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)], Xia, Younan [Georgia Institute of Technology, Atlanta, GA (United States); Emory University, Atlanta, GA (United States)] (ORCID:0000000324317048), Limmer, David T. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)] (ORCID:0000000227660688), Zheng, Haimei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000338134170). 2026-06-22. Atomic Evolution of Hydrogen Intercalation Wave Dynamics in Palladium Nanocrystals Revealed by Liquid-Phase Transmission Electron Microscopy. https://doi.org/10.1021/jacs.6c03937

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related discoveries

DOE OSTI2025

Surface deposition of nanometer scale carbon structures on Bi 2 Sr 2 CaCu 2 O 8+δ using a low-cost scanning electron microscope

In this work, we investigate optically active nanostructures on Bi 2 Sr 2 CaCu 2 O 8+δ (BSCCO). The nanostructures are constructed from carbon nanocrystals formed using the electron beam of a scanning electron microscope to locally decompose residual hydrocarbons at the BSCCO surface. Atomic force microscopy is used to characterize the dimensions of these structures as a function of beam exposure time. This technique has been used to induce localized intercalation to form carbon nanoparticles up to tens of nanometers into a variety of 2D materials. Cross-sectional scanning transmission electron microscopy in BSCCO shows the presence of these carbon deposits on the surface, but there is no evidence they penetrate into the BSCCO substrate. Therefore, this technique is not suitable for localized intercalation in BSCCO, and it does have promise as a cost-effective approach to pattern nanometer scale etch stops.

2D materials↗
DOE OSTI2026

Visualizing Millisecond Atomic Dynamics of Nanocrystals in Liquid

Atomic structures of nanomaterials are inherently dynamic and continuously reshaped through interactions with chemical species and external stimuli. Such dynamics are further amplified as the size and dimensionality of nanomaterials decrease. Despite advances in analytical methods, it remains challenging to capture the structural dynamics of nanomaterials in reactive environments with both atomic spatial resolution and commensurate temporal resolution. Here, in this study, we directly visualize atomic-scale dynamics of gold (Au) nanocrystals in reactive liquid environments with millisecond-speed liquid-cell electron microscopy (EM) and deep-learning denoising. We uncover reversible fluctuations in the local crystallinity of Au nanocrystals dependent on the surrounding chemical environment. These transient fluctuations, driven by interactions at nanocrystal–liquid interfaces, critically influence the dissolution kinetics and grain boundary relaxation. By overcoming the spatiotemporal limitations in conventional liquid-cell EM, our findings provide insights into how transient nanoscale structures dictate the stability and reactivity of nanomaterials.

Kang, Sungsu [University of Chicago, IL (United St↗
DOE OSTI2026

The ABCs of phase retrieval: Connecting the acronyms of scanning transmission electron microscopy

High-resolution scanning transmission electron microscopy (S/TEM) is an indispensable tool for characterizing the structure and properties of materials down to the atomic scale. Conventional S/TEM imaging, however, is limited by the phase problem, whereby the phase of the electron exit wave is lost upon detection. Recent advances in diffractive imaging and 4D-STEM have enabled a range of phase-retrieval techniques that computationally reconstruct the missing information encoded in the phase of the transmission function. These approaches offer improved dose efficiency and enhanced sensitivity to weakly scattering signals, extending quantitative imaging to beam-sensitive materials composed of light elements. In this work, we introduce the phase problem in electron microscopy and survey the diverse landscape of phase-retrieval techniques used in the field. Despite their many acronyms and algorithmic variations, these techniques share a common physical and mathematical foundation. We present a unified framework that connects these seemingly distinct methods, from parallax imaging and tilt-corrected bright-field (tcBF-STEM), to aberration-corrected bright-field (acBF-STEM), optimum bright-field (OBF-STEM) and single-sideband (SSB) ptychography, as well as first-moment integrated center of mass techniques (iCOM) and iterative ptychographic algorithms. Based on these insights, we discuss the opportunities and practical limitations of applying these methods across different materials systems, detector designs, and microscope configurations.Graphical abstractRepresentative electron microscopy configurations used for phase retrieval and diffractive imaging in S/TEM: (a) Zernike phase-contrast transmission electron microscopy (TEM), (b) small-convergence-angle four-dimensional scanning transmission electron microscopy (4D-STEM) for nanobeam-based phase reconstruction methods, and (c) large-convergence-angle 4D-STEM for ptychographic and related diffractive imaging techniques reviewed in this work.

36 MATERIALS SCIENCE↗