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


EMSL Project ID
47296

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
2012-02-09
End Date
2014-09-30
Status
Closed

Team

Principal Investigator

Nigel Browning
Institution
University of Liverpool

Team Members

Ryan Hufschmid
Institution
University of Washington

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, C Park, BL Mehdi, W Xu, Y Zhang, LR Parent, M Gu, I Arslan, J Zhang, CM Wang, JE Evans, and ND Browning. 2014. "Probing the Degradation Mechanisms in Electrolyte Solutions for Li-ion Batteries by In-Situ TEM." Nano Letters 14(3):1293-1299. doi:10.1021/nl404271k
Abellan Baeza P, TJ Woehl, LR Parent, ND Browning, JE Evans, and I Arslan. 2014. "Factors influencing quantitative liquid (scanning) transmission electron microscopy." Chemical Communications 50(38):4873-80. doi:10.1039/c3cc48479c
Chambers SA, M Gu, PV Sushko, H Yang, CM Wang, and ND Browning. 2013. "Ultra-low contact resistance at an epitaxial metal/oxide heterojunction through interstitial site doping." Advanced Materials 25(29):4001–4005. doi:10.1002/adma.201301030
Evans JE, and ND Browning. 2013. "Enabling direct nanoscale observations of biological reactions with dynamic TEM." Microscopy 62(1):147-156. doi:10.1093/jmicro/dfs081
Martinez-Macias C ,Xu P ,Hwang SJ ,Lu J ,Chen CY ,Browning N D,Gates B C 2014. "Iridium Complexes and Clusters in Dealuminated Zeolite HY: Distribution between Crystalline and Impurity Amorphous Regions" ACS Catalysis 4(8):2662?2666. 10.1021/cs5006426
Mehraeen S ,McKeown J ,Deshmukh P V,Evans J E,Abellan Baeza P ,Xu P ,Reed B W,Taheri M L,Fischione P E,Browning N D 2013. "A (S)TEM Gas Cell Holder with Localized Laser Heating for In Situ Experiments" Microscopy and Microanalysis 19(2):470-478. 10.1017/S1431927612014419
Melzer D ,Xu P ,Hartmann D ,Zhu Y ,Browning N D,Sanchez-Sanchez M ,Lercher J A 2016. "Atomic-scale determination of active facets on the MoVTeNb oxide M1 phase and their intrinsic catalytic activity for ethane oxidative dehydrogenation " Angewandte Chemie International Edition
Moeck P ,York B W,Browning N D 2014. "Symmetries of migration related segments of all [001] coincidence site lattice tilt boundaries in (001) projections for all holohedral cubic materials" Crystal Research & Technology 49(9):708-720. 10.1002/crat.201400071
Muntifering B R,Kovarik L ,Browning N D,Pond R C,Knowlton W B,Mullner P 2016. "Stress assisted removal of conjugation boundaries in non-modulated Ni-Mn-Ga by coordinated secondary twinning" Journal of Materials Science 51(1):457-466. 10.1007/s10853-015-9236-1
Muntifering BR, RC Pond, L Kovarik, ND Browning, and P Muller. 2014. "Intra-variant Substructure in Ni-Mn-Ga Martensite: Conjugation Boundaries ." Acta Materialia 71:255-263. doi:10.1016/j.actamat.2014.03.018
Parent L R,Cheng Y ,Sushko P ,Shao Y ,Liu J ,Wang C M,Browning N D 2015. "Realizing the Full Potential of Insertion Anodes for Mg-ion Batteries Through the Nano-Structuring of Sn" Nano Letters 15(2):1177-1182. 10.1021/nl5042534
Parent LR, DB Robinson, PJ Cappillino, RJ Hartnett, P Abellan, ND Browning, and I Arslan. 2014. "In Situ Observation of Directed Nanoparticle Aggregation During the Synthesis of Ordered Nanoporous Metal in Soft Templates." Chemistry of Materials 26(3):1426-1433. doi:10.1021/cm4035209
Price PM, ND Browning, and DP Butt. 2014. "Microdomain Formation, Oxidation, and Cation Ordering in LaCa2Fe3O8+y." PNNL-SA-103675, Pacific Northwest National Laboratory, Richland, WA. [Submitted]
Sacci R L,Dudney N J,More K L,Parent L R,Arslan I ,Browning N D,Unocic R R 2013. "Direct Visualization of Initial SEI Morphology and Growth Kinetics During Lithium Deposition by in situ Electrochemical Transmission Electron Microscopy" Chemical Communications 50(17):2104-2107. 10.1039/c3cc49029g
Wang J ,Ganguly S ,Sen S ,Browning N D,Kauzlarich S M 2013. "Synthesis and characterization of P-doped amorphous and nanocrystalline Si" Polyhedron 58(Special Issue):156?161. 10.1016/j.poly.2012.10.011
Welch DA, TJ Woehl, C Park, R Faller, JE Evans, and ND Browning. 2016. "Understanding the Role of Solvation Forces on the Preferential Attachment of Nanoparticles in Liquid." ACS Nano 10(1):181-187. doi:10.1021/acsnano.5b06632
Woehl TJ, C Park, JE Evans, I Arslan, WD Ristenpart, and ND Browning. 2013. "Direct Observation of Aggregative Nanoparticle Growth: Kinetic Modeling of the Size Distribution and Growth Rate." ACS Nano 14(1):373-378. doi:10.1021/nl4043328
Woehl TJ, JE Evans, I Arslan, WD Ristenpart, and ND Browning. 2012. "Direct in Situ Determination of the Mechanisms Controlling Nanoparticle Nucleation and Growth." ACS Nano 6(10):8599–8610. doi:10.1021/nn303371y
Xu P ,Lu J ,Aydin C ,Debefve L M,Browning N D,Chen CY ,Gates B C 2015. "Imaging individual lanthanum atoms in zeolite Y by scanning transmission electron microscopy: evidence of lanthanum pair sites" Microporous and Mesoporous Materials 213():95-99. 10.1016/j.micromeso.2015.04.008
Yang H ,Kotula P G,Sato Y ,Chi M ,Ikuhara Y ,Browning N D 2014. "Segregation of Mn2+ Dopants as Interstitials in SrTiO3 Grain Boundaries" Materials Research Letters 2(1):16-22. 10.1080/21663831.2013.856815
Yang H ,Lee H S,Kotula P G,Sato Y ,Ikuhara Y ,Browning N D 2015. "Amphoteric Doping of Praseodymium Pr3+ in SrTiO3 Grain Boundaries" Applied Physics Letters 106(12):Article No. 121904. 10.1063/1.4916223