Skip to main content

Advanced High Resolution and Dynamic in-situ TEM/STEM Observations of Materials Processes


EMSL Project ID
48583

Abstract

The first goal of this research program is to develop a robust method to quantify the atomic scale changes in structure, composition and bonding that occur at interfaces under a variety of environmental conditions. Although (scanning) transmission electron microscopy has long had the ability to deliver atomic resolution Z-contrast images, interpretation of the image contrast and subsequently the properties of the material being studied, has primarily been on an image by image basis -- in some cases extrapolating a single image to represent the properties of all interfaces in a materials system. However, to truly quantify the properties of interfaces, any atomic scale study must give statistical relevance to the analysis. In addition to an increase in spatial resolution, the advent of aberration correctors has provided a stability and robustness of experimental approach that means the statistical variations across many images can be correlated and quantified. This research will use these features of aberration correction to build on the statistical crystallography methods developed for structural biology and applied previously in materials science to study doping changes in bulk materials. Analysis will focus specifically on oxide interfaces and heterogeneous catalysts under environmental conditions ranging from high vacuum through atmospheric pressure gases to liquids with the ultimate goal of understanding how structures evolve under different operating conditions.

The second goal of this project is to develop a fundamental understanding of materials dynamics (from microseconds to nanoseconds) in systems where the required combination of spatial and temporal resolution can only be reached by the dynamic transmission electron microscope (DTEM). In this temporal regime, the DTEM is expected to have atomic spatial resolution, providing an in-situ TEM capable of studying nanoscale dynamic phenomena with several orders of magnitude time resolution advantage over any existing in-situ TEM. For the routine interpretation of DTEM images it will be essential to also perform detailed experiments on the environmental TEM. This capability will be used to study the mechanism of sintering and growth for nanoparticles in and around electrodes and the observation of live organic systems in their hydrated states. The aim for both of these projects is to develop new insights into long-standing scientific problems related to the identification and control of the active sites that are responsible for the selectivity of chemical reactions and the nucleation/growth of nanostructures. In addition to providing time resolved imaging, short pulses of electrons may significantly enhance the capabilities of static bioimaging by mitigating damage and sample deformation issues which limit state-of-the-art bioimaging. This program is expected to involve many graduate students and postdocs, rapidly leading to the education of a new generation of scientists capable of employing the latest dynamic characterization methods.

Project Details

Start Date
2014-10-01
End Date
2017-09-30
Status
Closed

Team

Principal Investigator

Nigel Browning
Institution
University of Liverpool

Team Members

Hao Su
Institution
Eindhoven University of Technology

Eric Jensen
Institution
Pacific Northwest National Laboratory

Ryan Hufschmid
Institution
University of Washington

Jeffrey Ditto
Institution
University of Oregon

Joseph Patterson
Institution
University of California, San Diego

Yu Gong
Institution
College of Charleston

Hee Joon Jung
Institution
Northwestern University

Louise Debefve
Institution
University of California, Davis

Trevor Moser
Institution
Environmental Molecular Sciences Laboratory

Beata Mehdi
Institution
University of Liverpool

Patrick El-Khoury
Institution
Pacific Northwest National Laboratory

James Evans
Institution
Environmental Molecular Sciences Laboratory

David Welch
Institution
University of California, Davis

Jean Futrell
Institution
Pacific Northwest National Laboratory

Alan Joly
Institution
Pacific Northwest National Laboratory

Related Publications

Abellan Baeza P, LR Parent, NM Al Hasan, C Park, I Arslan, AM Karim, JE Evans, and ND Browning. 2016. "Gaining Control over Radiolytic Synthesis of Uniform Sub-3-nanometer Palladium Nanoparticles: Use of Aromatic Liquids in the Electron Microscope." Langmuir 32(6):1468-1477. doi:10. 1021/acs. langmuir. 5b04200
Berto TF, KE Sanwald, JP Byers, ND Browning, OY Gutierrez, and JA Lercher. 2016. "Enabling Overall Water Splitting on Photocatalysts by CO-Covered Noble Metal Co-catalysts." Journal of Physical Chemistry Letters 7(21):4358-4362. doi:10.1021/acs.jpclett.6b02151
Buru C, P Li, BL Mehdi, A Dohnalkova, AE Platero-Prats, ND Browning, KW Chapman, J Hupp, and O Farha. 2017. "Adsorption of a Catalytically Accessible Polyoxometalate in a Mesoporous Channel-type Metal–Organic Framework." Chemistry of Materials. doi:10.1021/acs.chemmater.7b00750
Falmbigl M, D Putzky, JJ Ditto, and DC Johnson. 2015. "Influence of Interstitial V on Structure and Properties of Ferecrystalline ([SnSe]1. 15)1(V1+xSe2)n for n=1, 2, 3, 4, 5, and 6." Journal of Solid State Chemistry 231:101–107. doi:10. 1016/j. jssc. 2015. 08. 013
Falmbigl M ,Putzky D ,Ditto J J,Esters M ,Bauers S R,Ronning F ,Johnson D C 2015. "Influence of Defects on the Charge Density Wave of ([SnSe]1þ?)1(VSe2)1 Ferecrystals" ACS Nano 9(8):8440–8448. 10.1021/acsnano.5b03361
Falmbigl M, Z Hay, JJ Ditto, GA Mitchson, and DC Johnson. 2015. "Modifying a charge density wave transition by modulation doping: ferecrystalline compounds ([Sn1?xBixSe]1. 15)1(VSe2)1 with 0 ? x ? 0. 66." Journal of Materials Chemistry C 3:12308-12315. doi:10. 1039/C5TC03130C
Fan Y, AW Robertson, Y Zhou, Q Chen, X Zhang, ND Browning, H Zheng, MH Rümmeli, and JH Warner. 2017. "Electrical Breakdown of Suspended Mono- and Few-Layer Tungsten Disulfide." PNNL-SA-127585, Pacific Northwest National Laboratory, Richland, WA. [Unpublished]
Hite O K,Nellist M ,Ditto J J,Falmbigl M ,Johnson D C 2016. "Transport Properties of VSe2 Monolayers Separated by Bilayers of BiSe" Journal of Materials Research 31(07):886-892. 10.1557/jmr.2015.354
Li B, RV Chopdekar, AT N'Diaye, A Mehta, JP Byers, ND Browning, E Arenholz, and Y Takamura. 2016. "Tuning Interfacial Exchange Interactions via Electronic Reconstruction in Transition-Metal Oxide Heterostructures." Applied Physics Letters 109(15):2401. doi:10.1063/1.4964407
Li P, N Vermeulen, C Malliakas, DA Gomez-Gualdron, AJ Howarth, BL Mehdi, A Dohnalkova, ND Browning, M O'Keeffe, and O Farha. 2017. "Bottom-up construction of a superstructure in a porous uranium-organic crystal." Science 356(6338):624-627. doi:10.1126/science.aam7851
Mills EM, M Kleine-Boymann, J Janek, H Yang, ND Browning, Y Takamura, and S Kim. 2016. "YSZ thin films with minimized grain boundary resistivity." Energy and Environmental Science 18:10486-10491. doi:10. 1039/C5CP08032K
Mitchson GA, M Falmbigl, JJ Ditto, and DC Johnson. 2015. "Antiphase Boundaries in the Turbostratically Disordered Misfit Compound (BiSe)1+?NbSe2." Inorganic Chemistry 54(21):10309–10315.
Sadeghi O, C Falaise, PI Molina, RD Hufschmid, CF Campana, BC Noll, ND Browning, and M Nyman. 2016. "Chemical stabilization and electrochemical destabilization of the iron Keggin ion in water." Inorganic Chemistry 55(21):11078-11088. doi:10.1021/acs.inorgchem.6b01694
Westover R ,Atkins R ,Falmbigl M ,Ditto J J,Johnson D C 2016. "Self-assembly of Designed Precursors: A Route to Crystallographically Aligned New Materials with Controlled Nanoarchitecture" Journal of Solid State Chemistry 236():173–185. 10.1016/j.jssc.2015.08.018
Westover R D,Mitchson G A,Ditto J J,Johnson D C 2016. "Synthesis of a Family of ([SnSe]1+?)m([{MoxNb1x}Se2]1+?)1" European Journal of Inorganic Chemistry 2016(8):1225–1231. 10.1002/ejic.201501324
Zhu Y, and ND Browning. 2017. "The Role of Gas in Determining Image Quality and Resolution During In Situ Scanning Transmission Electron Microscopy Experiments." ChemCatChem 9(18):3478-3485. doi:10.1002/cctc.201700474
Zhu Y, P Sushko, D Melzer, E Jensen, L Kovarik, C Ophus, M Sanchez-Sanchez, JA Lercher, and ND Browning. 2017. "Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution." Journal of the American Chemical Society 139(36):12342-12345. doi:10.1021/jacs.7b05240