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Chemical Imaging Initiative

Current Projects

Projects to develop coupled optical, electron, ion, and scanned probe microscopies to understand chemical and biological transformations and mechanisms are as follows.

Science Theme 1: Energy Storage and Conversion Materials

Project 1.5: XES Nanoprobe for Hard X-Ray Region: Mitigating Degradation in Ni-ZEBRA Batteries
Principal Investigator:
Nancy Hess
Team Members: Mark Bowden, Kyle Alvine, John Lemmon
Key Collaborators: Jerry Siedler, Devon Mortensen (University of Washington), Joy Andrews (SSRL)

This project is building a high spatial resolution x-ray emission spectroscopy (XES) capability for in situ analysis of x-ray emission lines in the 5- to 10-keV range. The XES Nanoprobe capability will be demonstrated on two battery systems of scientific interest: sodium/nickel and nickel/lithium. The development of a low-cost, modular XES system at the Advanced Photon Source and ultimately at National Synchrotron Light Source 2 will be widely applicable to fundamental materials chemistry challenges.

Project 1.6: Imaging the Nucleation and Growth of Nanoparticles in Solution
Principal Investigator:
Libor Kovarik
Team Members: Naila Al Hasan, Ryan Kelly, Libor Kovarik
Key Collaborators: Abhaya K. Datye, Angelica Benavidez, Aaron Jenkins (University of New Mexico), Anatoly Frenkel (Yeshiva University and BNL), Sergei Ivanov (Center for Integrated Nanotechnologies, LANL)

This project is developing in situ tools with atomic-scale, millisecond time resolution to image the nucleation and growth of nanoparticles in solution. Atomic-scale, millisecond time-resolution imaging will advance the understanding of particle nucleation and growth mechanisms. This will enable the controlled synthesis and study of nanomaterials of well-defined size, shape and exposed surfaces. These nanomaterials are vital in enabling new material design and exploration.

Project 2.4: Quantitative Imaging of Atomic-Scale Chemistry Changes at Interfaces
Principal Investigator:
Nigel Browning
Team Member: Pinghong Xu
Key Collaborators: Bruce Gates (University of California Davis), Johannes Lercher (Technische Universität München)

This project is developing a robust method to quantify atomic-scale changes in structure, composition, and bonding at interfaces. This research will use the advanced capabilities for chemical imaging under varied environmental conditions afforded by the new generation of aberration-corrected microscopes and in situ stages. The expected outcomes include developing robust statistical methods for reproducible and quantified image analysis/interpretation, applying methods to understand the interplay of structure-composition and properties at interfaces in functional oxides, and applying these statistical methods to investigate heterogeneous catalysts.

Project 2.5: Probing Structural Dynamics with High Spatial and Temporal Resolution
Principal Investigator:
Nigel Browning
Team Members: James Evans, Patricia Abellan, Russell Tonkyn, Naila Al Hasan
Key Collaborators: Ben Torralva (Michigan), Andreas Schroeder (UIC)

This project is conducting the work to understand the structural dynamics in biological and/or nanomaterials systems on the ms to ns timescale. This research will use a unique aberration-corrected Dynamic TEM (DTEM), where a photoemission source will enable time-resolved images at/near atomic resolution. The expected outcomes include developing single-shot imaging with atomic spatial resolution for DTEM with in situ gas and liquid stages, testing the overall limits in spatio-temporal resolution for future ultrafast TEM designs, and developing the capability for imaging biological structures in their "live" hydrated state.

Project 2.6: Probing Structure-Property Relationship of Energy Storage Materials Using Ex Situ and In Situ Dynamic Microscopy and Spectroscopy with High Spatial and Fast Temporal Resolution
Principal Investigator:
Chongmin Wang
Team Members: Meng Gu, Vijay Murugesan, Nigel Browning
Key Collaborators: Ian McNulty, Robert Winarski (APS), Tolek Tyliszczak, David Shuh (ALS)

On this project, the researchers are developing capabilities that drive chemical imaging and spectroscopic analysis of materials under ex situ and in situ conditions with high spatial and fast temporal resolution. They are also establishing the structure-property relationship of energy storage materials and its correlation with charge and ion transport. Finally, they are searching for a general guiding principle for accelerated discovery of new materials for high density and high power energy applications

Project 2.7: Atomic-level Investigation of the Phase Stability of Transition Metals under Reactive Environment
Principal Investigator: Libor Kovarik
Research Team: Zhehao Wei, Janos Szanyi, Charles Peden
Key Collaborators: Ja Hun Kwak (UNIST), Andrey Liyu (PNNL)

The purpose of this project is three-fold: investigate the stability of platinum group catalytic nanoparticles during exposure to elevated temperature and reactive environment; develop capabilities for atomic-level imaging of transition phenomena with environmental transmission electron microscope; and establish guiding principles for accelerated discovery of next-generation catalytic materials. The expected outcome is establishing the mechanisms that govern the stability of supported noble nanoparticles under environmental conditions.

Project 2.8: Atomic-scale Chemical Imaging via Combination of Scanning Tunneling and Electron Energy Loss Spectroscopies
Principal Investigator: Igor Lyubinetsky
Research Team: Rentao Mu, Zhitao Wang, Zdenek Dohnalek, Michael Henderson, Roger Rousseau

The purpose of this project is to develop an atomic-level, mechanistic understanding of catalytically important systems and develop an atomically resolved chemical imaging platform: low-temperature scanning tunneling microscope with in situ molecular beam and ex situ electron spectroscopies. The expected outcomes are a multimodal spectroscopic capability for chemically specific, surface-sensitive imaging at atomic/molecular level and superior spatial resolution compared to tip-enhanced Raman.

Project 3.4: Data Acquisition System for Dynamic Transmission Electron Microscopy
Principal Investigator: Kerstin Kleese-van Dam
Research Team: Mathew Thomas, Malachi Schram, Carina Lansing
Key Collaborators: James Evans, Nigel Browning, Patricia Abellan Baeza, Matthew Olszta, Danny Edwards, Layla Mehdi, Lucas R Parent

The purpose of this project is to improve current transmission electron microscopy (TEM) data acquisition process to support improved analysis capabilities and higher data volumes expected from the dynamic TEM (DTEM) under development at PNNL. The expected outcomes are an acquisition system supporting higher data rates; the ability to capture enhanced metadata; system linked to PNNL Institutional Computing and Analysis in Motion (AIM)/REXAN-based analysis pipelines to provide data streams for evaluating AIM framework efficacy and performance; and hardware/software recommendations for further high-throughput data collection.

Science Theme 2: Biofilm and Cellular Metabolite Expression

Project 1.8: Structure and Dynamics of Biological Systems
Principal Investigator:
James Evans
Team Members: Daniel Perea, Xiao-Ying Yu, Zihua Zhu, Blake Hirschi, Bingwen Liu, Jia Liu, Trevor Moser
Key Collaborators: Nigel Browning, Matt Marshall, Galya Orr, Theva Thevuthasan

This project is integrating five emerging technologies to permit multimodal and multiscale spatial, temporal, and chemical analysis of biofilm organization, cellular nanotoxicology, and enzymatic energy transduction. The five technologies are as follows:

  • Coherent x-ray diffraction at the Linac Coherent Light Source
  • Dynamic transmission electron microscopy
  • Atom probe tomography
  • In situ transmission electron microscopy/scanning electron microscopy/time-of-flight secondary ion mass spectrometry
  • Nano-SISM

Project 1.11: Imaging and Monitoring the Stages of Biofilm Formation
Principal Investigator:
R Shane Addleman
Team Members: George Bonheyo, Erin Miller, Marvin Warner
Key Collaborators: Matt Marshall, Robby Robinson, Kristyn Roscioli, Rob Jeters, Katye Denslow, Jon Suter, Chris Barrett, Curtis Laminer, Jiyeon Park

The team is examining biofilms and biofouling processes from medical and marine environments to understand and compare the basic mechanisms for each type and developing new analytical tools to enable effective measurement of biofilms and support rational development of better antifouling materials. The expected outcomes are

  • Improved and novel analytical methods to study biomolecular processes at the fluid-surface interface.
  • Identify how conditioning film composition and distribution impacts cellular adhesion and colony formation.
  • Improved mechanistic understanding of how surface chemistry and features impact biofilm formation to enable rational development of new antifouling materials.
  • Develop better antifouling surfaces to improve shipping fuel efficiency, reduce invasive species transport, and reduce infections from medical devices.

Science Theme 3: Fundamental Particle Origin and Evolution

Project 1.7: Microscale Reconstruction of Biogeochemical Substrates Using Combined X-Ray Tomography and Scanning Electron Microscope
Principal Investigator:
James McKinley
Team Members: Micah Miller, Erin Miller, Jun Liu

This project is developing a technology for three-dimensional reconstruction of the physical and chemical nature of natural samples at the sub-micrometer scale. The team is also evaluating the ability to combine data across collection methods. With the data they've acquired, they are gaining insights for hydrology, geochemistry, and microbial ecology. These areas rely on the knowledge of phase and pore space distributions to understand contaminant mobility and natural transport and phase transformations.

Project 1.9: Developing Next-Generation Multimodal Chemical Imaging Capability by Combining STEM/APT/STXM/HIM
Principal Investigator:
Theva Thevuthasan
Team Members: Theva Thevuthasan, Arun Devaraj, Craig Szymanski, Birgit Schwenzer, Shuttha Shutthanandan, Zhijie Xu, Gourihar Kulkarni
Key Collaborators: David Shuh (ALS), Tolek Tyliszczak (ALS), Francois Vurpillot (UR)

This project is developing a common platform to obtain three-dimensional analysis with sub-nanometer spatial and chemical resolution and ppm-level mass sensitivity to understand complex energy storage and conversion systems. The platform will integrate aberration-corrected transmission electron microscopy, atom probe tomography, scanning transmission x-ray microscopy, and helium ion microscopy to characterize relevant catalyst materials with metal or metal oxide nanoparticles supported on porous metal oxides and lithium-related energy storage materials.

Project 1.10: Uranium Analysis with X-ray Microscopy
Principal Investigator:
Andrew Duffin
Team Members: Andrew Duffin, Jesse Ward, Gregory Eiden, Steven Smith, Bruce McNamara, Edgar Buck
Key Collaborators: David Prendergast, David Shuh (LBNL)

The purpose of this project is chemical fingerprinting of anthropogenic and mineral uranium leading to chemical age dating of reactive uranium samples and developing x-ray and/or electron microscopy protocol for non-destructive uranium sample analysis.


Chemical Imaging Initiative

Talks, Proposals and Publications

Fundamental & Computational Sciences Directorate


Nigel Browning
Initiative Lead

Lou Terminello
Initiative Advisor

Wayne Hess
Science Theme 1 Co-Lead

Kerstin Kleese van-Dam
Science Theme 1 Co-Lead

Scott E. Baker
Science Theme 2 Co-Lead

Theva Thevuthasan
Science Themes 2 and 3 Co-Lead

Alex Guenther
Science Theme 3 Co-Lead

Edmond Hui
Project Leader


Julie Wiley

Web Publishing

Project Administration


CII Funding