skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Insights into the physical chemistry of materials from advances in HAADF-STEM

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/C4CP04232H· OSTI ID:1185797
 [1];  [2];  [3];  [4]
  1. Drexel Univ., Philadelphia, PA (United States)
  2. SuperSTEM Lab., Daresbury (United Kingdom); Univ. of Oxford (United Kingdom)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States)

The observation that, ‘‘New tools lead to new science’’[P. S. Weiss, ACS Nano., 2012, 6(3), 1877–1879], is perhaps nowhere more evident than in scanning transmission electron microscopy (STEM). Advances in STEM have endowed this technique with several powerful and complimentary capabilities. For example, the application of high-angle annular dark-field imaging has made possible real-space imaging at subangstrom resolution with Z-contrast (Z = atomic number). Further advances have wrought: simultaneous real-space imaging and elemental identification by using electron energy loss spectroscopy (EELS); 3-dimensional (3D) mapping by depth sectioning; monitoring of surface diffusion by time-sequencing of images; reduced electron energy imaging for probing graphenes; etc. In this paper we review how these advances, often coupled with first-principles theory, have led to interesting and important new insights into the physical chemistry of materials. We then review in detail a few specific applications that highlight some of these STEM capabilities.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1185797
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 17, Issue 6; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 57 works
Citation information provided by
Web of Science

References (119)

Tracking Iridium Atoms with Electron Microscopy: First Steps of Metal Nanocluster Formation in One-Dimensional Zeolite Channels journal December 2011
Atomic-resolution chemical analysis using a scanning transmission electron microscope journal November 1993
Dopants adsorbed as single atoms prevent degradation of catalysts journal February 2004
STEM-EELS imaging of complex oxides and interfaces journal January 2012
Quantized Growth of CdTe Quantum Dots; Observation of Magic-Sized CdTe Quantum Dots journal September 2007
Atomic-Scale Investigation of Two-Component MoVO Complex Oxide Catalysts Using Aberration-Corrected High-Angle Annular Dark-Field Imaging journal March 2010
On the Nanoparticle to Molecular Size Transition:  Fluorescence Quenching Studies journal November 2001
Single Atom Microscopy journal November 2012
Atom-Resolved Imaging of Dynamic Shape Changes in Supported Copper Nanocrystals journal March 2002
Single atom identification by energy dispersive x-ray spectroscopy journal April 2012
Electroluminescence from single monolayers of nanocrystals in molecular organic devices journal December 2002
Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer journal August 1994
Three-dimensional imaging of individual hafnium atoms inside a semiconductor device journal July 2005
Towards a More Accurate Particle Size Distribution of Supported Catalyst by using HAADF-STEM journal May 2011
Mapping titanium and tin oxide phases using EELS: An application of independent component analysis journal January 2011
Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures journal August 2008
On ultrasmall nanocrystals journal September 2010
Optical gaps of free and embedded Si nanoclusters: Density functional theory calculations journal September 2010
Transition Metal Oxides: Extra Thermodynamic Stability as Thin Films journal February 2006
Pd3 and Pt3 species on the α-Al2O3(0001) surface: cluster models embedded in an elastic polarizable environment journal June 2003
Subangstrom Resolution by Underfocused Incoherent Transmission Electron Microscopy journal November 1998
Size and shape of industrial Pd catalyst particles using size-selected clusters as mass standards journal April 2013
Synthesis and Characterization of White-Emitting CdS Quantum Dots Stabilized with Polyethylenimine journal December 2010
Surface Chemistry of Silicon Nanoclusters journal February 2002
Single-Atom Sensitivity for Solving Catalysis Problems journal August 2004
Platinum-Modulated Cobalt Nanocatalysts for Low-Temperature Aqueous-Phase Fischer–Tropsch Synthesis journal March 2013
Atomically localized plasmon enhancement in monolayer graphene journal January 2012
Introducing the Core Concepts of Nanoscience and Nanotechnology: Two Vignettes journal October 2006
Visibility of Single Atoms journal June 1970
Investigation of the Crystallization Process in 2 nm CdSe Quantum Dots journal March 2005
Point Defect Configurations of Supersaturated Au Atoms Inside Si Nanowires journal March 2008
Direct imaging of single metal atoms and clusters in the pores of dealuminated HY zeolite journal May 2010
Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy journal March 2010
Direct Electronic Property Imaging of a Nanocrystal-Based Photovoltaic Device by Electron Beam-Induced Current via Scanning Electron Microscopy journal February 2014
Geometric aberration correction in ion lenses - the Caledonian quadruplet journal September 1983
Dynamic Fluctuations in Ultrasmall Nanocrystals Induce White Light Emission journal May 2012
Pinned emission from ultrasmall cadmium selenide nanocrystals journal September 2008
The Structure of Catalytically Active Gold on Titania journal October 2004
Few-Layer Graphene as a Support Film for Transmission Electron Microscopy Imaging of Nanoparticles journal November 2009
Evidence of High-Pressure Rhodium Sesquioxide in the Rhodium/γ-Alumina Catalytic System journal July 2008
Stimulated Emission by Current Injection from an AlGaN/GaN/GaInN Quantum Well Device journal November 1995
A combined HAADF STEM and density functional theory study of tantalum and niobium locations in the Mo–V–Te–Ta(Nb)–O M1 phases journal December 2012
Semiconductor Nanocrystals as Fluorescent Biological Labels patent September 1998
Characterization of supported catalysts by high-resolution stem journal September 1983
Novel MEMS-Based Gas-Cell/Heating Specimen Holder Provides Advanced Imaging Capabilities for In Situ Reaction Studies journal July 2012
Synthesis, surface studies, composition and structural characterization of CdSe, core/shell and biologically active nanocrystals journal April 2007
White-light-emitting CdSe quantum dots synthesized at room temperature journal July 2006
White-Light Emission from Magic-Sized Cadmium Selenide Nanocrystals journal November 2005
Behavior of Au Species in Au/Fe 2 O 3 Catalysts Characterized by Novel In Situ Heating Techniques and Aberration-Corrected STEM Imaging journal June 2010
Direct Imaging of the Atomic Configuration of Ultradispersed Catalysts journal October 1996
Three-dimensional atomic-scale structure of size-selected gold nanoclusters journal December 2007
Three-Dimensional Tracking and Visualization of Hundreds of Pt−Co Fuel Cell Nanocatalysts During Electrochemical Aging journal January 2012
Atomic Column Resolved Electron Energy-Loss Spectroscopy journal March 1998
Atomic-Resolution Electron Energy Loss Spectroscopy Imaging in Aberration Corrected Scanning Transmission Electron Microscopy journal September 2003
Structures of small Pd–Pt bimetallic clusters by Monte Carlo simulation journal November 2006
Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation journal September 2008
Aberration-corrected ADF-STEM depth sectioning and prospects for reliable 3D imaging in S/TEM journal January 2009
Scanning Electron Microscopes: Is High Resolution Possible? journal November 1966
Advances in the catalysis of Au nanoparticles journal December 2001
Towards sub-Å electron beams journal June 1999
The Merits of Static and Dynamic High-Resolution Electron Microscopy (HREM) for the Study of Solid Catalysts journal July 2010
Size-Dependent Optical Spectroscopy of a Homologous Series of CdSe Cluster Molecules journal March 2001
Origin of Anomalous Pt-Pt Distances in the Pt/Alumina Catalytic System journal December 2004
Z-contrast stem for materials science journal June 1989
Recent conceptual advances in the catalysis science of mixed metal oxide catalytic materials journal February 2005
Nonlinear structured-illumination microscopy: Wide-field fluorescence imaging with theoretically unlimited resolution journal September 2005
Origin of stability of the high-temperature, low-pressure Rh2O3 III form of rhodium sesquioxide journal July 2006
Ultradispersed rhodium rafts: Their existence and topology journal March 1979
Atomically thin hexagonal boron nitride probed by ultrahigh-resolution transmission electron microscopy journal October 2009
Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis journal April 2013
New imaging methods for catalyst particles journal January 1982
Single-atom catalysis of CO oxidation using Pt1/FeOx journal July 2011
Origin of Colossal Ionic Conductivity in Oxide Multilayers: Interface Induced Sublattice Disorder journal March 2010
Z-contrast Imaging in an Aberration-corrected Scanning Transmission Electron Microscope journal July 2000
Encapsulated white-light CdSe nanocrystals as nanophosphors for solid-state lighting journal January 2008
Selective Sputtering and Atomic Resolution Imaging of Atomically Thin Boron Nitride Membranes journal July 2009
Electron–electron and electron‐hole interactions in small semiconductor crystallites: The size dependence of the lowest excited electronic state journal May 1984
Unique Ultrafast Visible Luminescence in Monolayer-Protected Au 25 Clusters journal December 2010
Three-Dimensional Scanning Transmission Electron Microscopy of Biological Specimens journal January 2010
Atomic-Scale Edge Structures on Industrial-Style MoS2 Nanocatalysts journal August 2011
Platinum dioxide phases: Relative thermodynamic stability and kinetics of inter-conversion from first-principles journal May 2006
Nanostructural and chemical characterization of supported metal oxide catalysts by aberration corrected analytical electron microscopy journal February 2012
Electronic structure of tin oxides by electron energy loss spectroscopy and real-space multiple scattering calculations journal January 2005
Seeing the atoms more clearly: STEM imaging from the Crewe era to today journal December 2012
An oxygen reduction electrocatalyst based on carbon nanotube–graphene complexes journal May 2012
Imaging Polymer Systems with High-Angle Annular Dark Field Scanning Transmission Electron Microscopy (HAADF−STEM) journal April 2009
High-resolution Z-contrast imaging of crystals journal August 1991
Hybrid Nanorod-Polymer Solar Cells journal March 2002
Defect-mediated ferromagnetism in insulating Co-doped anatase TiO 2 thin films journal July 2008
Catalytically active single-atom niobium in graphitic layers journal May 2013
Atomic structure of three-layer Au/Pd nanoparticles revealed by aberration-corrected scanning transmission electron microscopy journal January 2008
Historical aspects of aberration correction journal March 2009
Aberration-Corrected Z-Contrast Scanning Transmission Electron Microscopy of CdSe Nanocrystals journal July 2004
Structure of White Light Emitting CdSe Nanocrystals journal July 2011
Direct determination of interface structure and bonding with the scanning transmission electron microscope
  • Pennycook, S. J.; Browning, N. D.; McGibbon, M. M.
  • Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 354, Issue 1719, p. 2619-2634 https://doi.org/10.1098/rsta.1996.0119
journal November 1996
Some Chicago Aberrations journal August 2004
3D electron microscopy in the physical sciences: the development of Z-contrast and EFTEM tomography journal September 2003
A new concept for improved ion and electron lenses — Aberration corrected systems of planar electrostatic deflection elements journal December 1983
Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C journal February 1987
Identification of active Zr–WOx clusters on a ZrO2 support for solid acid catalysts journal November 2009
Differentiation of tin oxides using electron energy-loss spectroscopy journal June 2004
Direct Determination of the Chemical Bonding of Individual Impurities in Graphene journal November 2012
Z-contrast imaging of supported Pt and Pd clusters journal August 1994
New insights into the nature of the acidic catalytic active sites present in ZrO2-supported tungsten oxide catalysts journal May 2008
Depth sectioning with the aberration-corrected scanning transmission electron microscope journal February 2006
Single-Nanocrystal Spectroscopy of White-Light-Emitting CdSe Nanocrystals journal April 2011
Fluorescence microscopy with diffraction resolution barrier broken by stimulated emission journal July 2000
Relating n -Pentane Isomerization Activity to the Tungsten Surface Density of WO x /ZrO 2 journal September 2010
Structure and Ultrafast Dynamics of White-Light-Emitting CdSe Nanocrystals journal April 2009
Recent STM, DFT and HAADF-STEM studies of sulfide-based hydrotreating catalysts: Insight into mechanistic, structural and particle size effects journal January 2008
3 D Characterization of Gold Nanoparticles Supported on Heavy Metal Oxide Catalysts by HAADF-STEM Electron Tomography journal June 2009
Corrected electrostatic lens systems for ion beams journal December 1981
Spectroscopic Imaging of Single Atoms Within a Bulk Solid journal March 2004
Scanning Transmission Electron Microscopy at High Resolution journal January 1974
Towards full-structure determination of bimetallic nanoparticles with an aberration-corrected electron microscope journal November 2010
Sub-ångstrom resolution using aberration corrected electron optics journal August 2002
Microanalysis by Means of Electrons journal September 1944
Standardless Atom Counting in Scanning Transmission Electron Microscopy journal November 2010
Sub-Angstrom Probe Size in HADF-STEM at 120KV journal August 2002

Cited By (7)

The Atomic Circus: Small Electron Beams Spotlight Advanced Materials Down to the Atomic Scale journal October 2018
Earth-Rich Transition Metal Phosphide for Energy Conversion and Storage journal May 2016
Insight by In Situ Gas Electron Microscopy on the Thermal Behaviour and Surface Reactivity of Cobalt Nanoparticles journal July 2018
Generation of subnanometric platinum with high stability during transformation of a 2D zeolite into 3D journal September 2016
Elemental preference and atomic scale site recognition in a Co-Al-W-base superalloy journal December 2017
A facile approach to constructing Pd@PCN–Se nano-composite catalysts for selective alcohol oxidation reactions journal January 2019
Structural properties of sub-nanometer metallic clusters journal January 2019