DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Emerging Electron Microscopy Techniques for Probing Functional Interfaces in Energy Materials

Journal Article · · Angewandte Chemie (International Edition)

Interfaces play a fundamental role in many areas of chemistry. However, their localized nature requires characterization techniques with high spatial resolution in order to fully understand their structure and properties. State-of-the-art atomic resolution or in situ scanning transmission electron microscopy and electron energy-loss spectroscopy are indispensable tools for characterizing the local structure and chemistry of materials with single-atom resolution, but they are not able to measure many properties that dictate function, such as vibrational modes or charge transfer, and are limited to room-temperature samples containing no liquids. Here, we outline emerging electron microscopy techniques that are allowing these limitations to be overcome and highlight several recent studies that were enabled by these techniques. We then provide a vision for how these techniques can be paired with each other and with in situ methods to deliver new insights into the static and dynamic behavior of functional interfaces.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1651402
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 4 Vol. 59; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (166)

Development of a TEM to study in situ structural and chemical changes at an atomic level during gas-solid interactions at elevated temperatures journal September 1998
Controlling Structural Anisotropy of Anisotropic 2D Layers in Pseudo-1D/2D Material Heterojunctions journal July 2017
Integrated Circuits Comprising Patterned Functional Liquids journal July 2018
Vibrational Spectroscopy of Water with High Spatial Resolution journal July 2018
Nanoporous Hybrid Electrolytes for High-Energy Batteries Based on Reactive Metal Anodes journal January 2017
Molecular Recognition at the Gas—Solid Interface: A Powerful Tool for Chemical Sensing journal July 2007
Making the practically impossible “Merely difficult”-Cryogenic FIB lift-out for “Damage free” soft matter imaging: FAST AND EFFICIENT CRYO LIFT-OUT AND TRANSFER TO TEM journal February 2016
Quantitative measurements of internal electric fields with differential phase contrast microscopy on InGaN/GaN quantum well structures: Measurements of internal electric fields journal October 2015
Das Aufl�sungsverm�gen des elektrostatisch-magnetischen Energieanalysators f�r schnelle Elektronen journal August 1964
Tailoring of surface plasmon resonances in TiN/(Al0.72Sc0.28)N multilayers by dielectric layer thickness variation journal November 2017
Ionic conduction in space charge regions journal January 1995
In situ TEM sintering of nano-sized ZrO2 particles journal December 1995
Photocatalytic degradation of volatile organic compounds at the gas–solid interface of a TiO2 photocatalyst journal July 2002
The direct determination of magnetic domain wall profiles by differential phase contrast electron microscopy journal January 1978
Towards sub-Å electron beams journal June 1999
Construction and characterization of the fringe field monochromator for a field emission gun journal April 2000
In situ TEM observations of fast grain-boundary motion in stressed nanocrystalline aluminum films journal August 2008
Probing the light harvesting and charge rectification of bismuth nanoparticles behind the promoted photoreactivity onto Bi/BiOCl catalyst by (in-situ) electron microscopy journal February 2017
Designing Artificial Solid-Electrolyte Interphases for Single-Ion and High-Efficiency Transport in Batteries journal October 2017
Optical properties and biomedical applications of plasmonic nanoparticles journal January 2010
A site-specific focused-ion-beam lift-out method for cryo Transmission Electron Microscopy journal December 2012
A focused ion beam milling and lift-out approach for site-specific preparation of frozen-hydrated lamellas from multicellular organisms journal November 2015
Enhancement of resolution in core-loss and low-loss spectroscopy in a monochromated microscope journal October 2006
Prospects for analyzing the electronic properties in nanoscale systems by VEELS journal February 2008
Energy resolution of an Omega-type monochromator and imaging properties of the MANDOLINE filter journal July 2010
Dynamics of annular bright field imaging in scanning transmission electron microscopy journal June 2010
On the origin of differential phase contrast at a locally charged and globally charge-compensated domain boundary in a polar-ordered material journal July 2015
Sample tilt effects on atom column position determination in ABF–STEM imaging journal January 2016
Phase contrast STEM for thin samples: Integrated differential phase contrast journal January 2016
Pixelated detectors and improved efficiency for magnetic imaging in STEM differential phase contrast journal June 2016
Low magnification differential phase contrast imaging of electric fields in crystals with fine electron probes journal October 2016
Quantitative measurement of mean inner potential and specimen thickness from high-resolution off-axis electron holograms of ultra-thin layered WSe 2 journal July 2017
Scattering delocalization and radiation damage in STEM-EELS journal September 2017
Vibrational and valence aloof beam EELS: A potential tool for nondestructive characterization of nanoparticle surfaces journal September 2017
Cathodoluminescence in the scanning transmission electron microscope journal May 2017
Quantitative comparison of bright field and annular bright field imaging modes for characterization of oxygen octahedral tilts journal October 2017
Optimization of monochromated TEM for ultimate resolution imaging and ultrahigh resolution electron energy loss spectroscopy journal January 2018
Image registration of low signal-to-noise cryo-STEM data journal August 2018
Progress in ultrahigh energy resolution EELS journal August 2019
Comparison of first moment STEM with conventional differential phase contrast and the dependence on electron dose journal August 2019
Inelastic Electron Scattering with Energy Losses in the meV-Region journal August 1981
SESAM: Exploring the Frontiers of Electron Microscopy journal October 2006
In Situ Electron Energy-Loss Spectroscopy in Liquids journal May 2013
In Situ TEM Imaging of Defect Dynamics under Electrical Bias in Resistive Switching Rutile-TiO 2 journal December 2014
High Dynamic Range Pixel Array Detector for Scanning Transmission Electron Microscopy journal January 2016
Site-Specific Preparation of Intact Solid–Liquid Interfaces by Label-Free In Situ Localization and Cryo-Focused Ion Beam Lift-Out journal November 2016
Aberration-Corrected STEM/EELS at Cryogenic Temperatures journal July 2017
Advances in Ultra-High Energy Resolution STEM-EELS journal August 2018
Direct Electron Detection for Atomic-Resolution EELS Mapping at Cryogenic Temperature journal August 2018
Direct Electron Detection for Atomic Resolution in situ EELS journal August 2018
Atomic-Scale Chemical Imaging of Composition and Bonding by Aberration-Corrected Microscopy journal August 2008
Sample Tilt Effects on Atom Column Position Determination in ABF-STEM Imaging journal July 2016
Direct Visualization of Local Electromagnetic Field Structures by Scanning Transmission Electron Microscopy journal July 2017
Role of Akaganeite (β-FeOOH) in the Growth of Hematite (α-Fe 2 O 3 ) in an Inorganic Silica Hydrogel journal June 2015
Stabilizing Protic and Aprotic Liquid Electrolytes at High-Bandgap Oxide Interphases journal July 2018
Hybridization of Single Nanocrystals of Cs 4 PbBr 6 and CsPbBr 3 journal August 2017
Interfacial Challenges in Solid-State Li Ion Batteries journal October 2015
Hot Electron Generation and Cathodoluminescence Nanoscopy of Chiral Split Ring Resonators journal July 2016
In Situ TEM Analysis of Organic–Inorganic Metal-Halide Perovskite Solar Cells under Electrical Bias journal October 2016
Interfacial Stability of Li Metal–Solid Electrolyte Elucidated via in Situ Electron Microscopy journal October 2016
Resonant Coupling between Molecular Vibrations and Localized Surface Plasmon Resonance of Faceted Metal Oxide Nanocrystals journal March 2017
New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM journal November 2017
Low-Dose Aberration-Free Imaging of Li-Rich Cathode Materials at Various States of Charge Using Electron Ptychography journal September 2018
Investigation of the Interaction between Nafion Ionomer and Surface Functionalized Carbon Black Using Both Ultrasmall Angle X-ray Scattering and Cryo-TEM journal February 2017
Cryogenic Focused Ion Beam Characterization of Lithium Metal Anodes journal January 2019
Simultaneous First-Order Valence and Oxygen Vacancy Order/Disorder Transitions in (Pr 0.85 Y 0.15 ) 0.7 Ca 0.3 CoO 3−δ via Analytical Transmission Electron Microscopy journal December 2015
Nanoscale Probing of Local Hydrogen Heterogeneity in Disordered Carbon Nitrides with Vibrational Electron Energy-Loss Spectroscopy journal May 2018
Surface-Enhanced Molecular Electron Energy Loss Spectroscopy journal April 2018
Challenges for Rechargeable Li Batteries journal February 2010
4D Scanning Transmission Ultrafast Electron Microscopy: Single-Particle Imaging and Spectroscopy journal July 2011
Controllable Perovskite Crystallization at a Gas–Solid Interface for Hole Conductor-Free Solar Cells with Steady Power Conversion Efficiency over 10% journal November 2014
Thermal Signatures of Plasmonic Fano Interferences: Toward the Achievement of Nanolocalized Temperature Manipulation journal March 2014
Atomic-Scale Imaging in Real and Energy Space Developed in Ultrafast Electron Microscopy journal September 2007
In Situ TEM Near-Field Optical Probing of Nanoscale Silicon Crystallization journal April 2012
Nanoscale Imaging of Lithium Ion Distribution During In Situ Operation of Battery Electrode and Electrolyte journal February 2014
Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters journal February 2015
In Situ TEM Characterization of Shear-Stress-Induced Interlayer Sliding in the Cross Section View of Molybdenum Disulfide journal December 2014
Electron microscopy image enhanced journal April 1998
Issues and challenges facing rechargeable lithium batteries journal November 2001
Resolution beyond the 'information limit' in transmission electron microscopy journal April 1995
Lithium battery chemistries enabled by solid-state electrolytes journal February 2017
Generation of electron beams carrying orbital angular momentum journal April 2010
Production and application of electron vortex beams journal September 2010
Vibrational spectroscopy in the electron microscope journal October 2014
Mapping vibrational surface and bulk modes in a single nanocube journal March 2017
Damage-free vibrational spectroscopy of biological materials in the electron microscope journal March 2016
Electric field imaging of single atoms journal May 2017
Visualizing the interfacial evolution from charge compensation to metallic screening across the manganite metal–insulator transition journal March 2014
Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction journal December 2014
In situ observation of heat-induced degradation of perovskite solar cells journal January 2016
Plasmonics for improved photovoltaic devices journal February 2010
Direct imaging of hydrogen-atom columns in a crystal by annular bright-field electron microscopy journal February 2011
Probing oxygen vacancy concentration and homogeneity in solid-oxide fuel-cell cathode materials on the subunit-cell level journal August 2012
Origin of additional capacities in metal oxide lithium-ion battery electrodes journal November 2013
Direct observation of ferroelectric field effect and vacancy-controlled screening at the BiFeO3/LaxSr1−xMnO3 interface journal August 2014
Energy and fuels from electrochemical interfaces journal December 2016
Direct observation of chemical reactions on single gold nanocrystals using surface plasmon spectroscopy journal September 2008
Nanoscale optical tomography with cathodoluminescence spectroscopy journal April 2015
Differential phase-contrast microscopy at atomic resolution journal June 2012
Spatially and spectrally resolved orbital angular momentum interactions in plasmonic vortex generators journal March 2019
Probing low-energy hyperbolic polaritons in van der Waals crystals with an electron microscope journal July 2017
Designing solid-liquid interphases for sodium batteries journal October 2017
Fast ion transport at solid–solid interfaces in hybrid battery anodes journal March 2018
Selective breakdown of phonon quasiparticles across superionic transition in CuCrSe2 journal October 2018
Electron ptychography of 2D materials to deep sub-ångström resolution journal July 2018
Cryo-STEM mapping of solid–liquid interfaces and dendrites in lithium-metal batteries journal August 2018
Low-dose cryo electron ptychography via non-convex Bayesian optimization journal August 2017
Direct Detection Electron Energy-Loss Spectroscopy: A Method to Push the Limits of Resolution and Sensitivity journal August 2017
Exploring the capabilities of monochromated electron energy loss spectroscopy in the infrared regime journal April 2018
Imaging of built-in electric field at a p-n junction by scanning transmission electron microscopy journal June 2015
Jointed magnetic skyrmion lattices at a small-angle grain boundary directly visualized by advanced electron microscopy journal October 2016
Molecular recognition at the gas–solid interface: a powerful tool for chemical sensing journal January 2007
Plasmon-enhanced optical sensors: a review journal January 2015
Tuning mobility and stability of lithium ion conductors based on lattice dynamics journal January 2018
Carbon-based materials as supercapacitor electrodes journal January 2009
Direct visualization of initial SEI morphology and growth kinetics during lithium deposition by in situ electrochemical transmission electron microscopy journal January 2014
Atomic-scale origin of the large grain-boundary resistance in perovskite Li-ion-conducting solid electrolytes journal January 2014
Development of a high energy resolution electron energy-loss spectroscopy microscope: HIGH ENERGY RESOLUTION EELS MICROSCOPE journal April 1999
High-κ gate dielectrics: Current status and materials properties considerations journal May 2001
Improvement of windowed type environmental-cell transmission electron microscope for in situ observation of gas-solid interactions journal November 2009
Strain mapping at nanometer resolution using advanced nano-beam electron diffraction journal June 2015
Implementing an accurate and rapid sparse sampling approach for low-dose atomic resolution STEM imaging journal October 2016
Non-spectroscopic composition measurements of SrTiO 3 -La 0.7 Sr 0.3 MnO 3 multilayers using scanning convergent beam electron diffraction journal February 2017
Microscopic origins for stabilizing room-temperature ferromagnetism in ultrathin manganite layers journal June 2010
Atomic lattice disorder in charge-density-wave phases of exfoliated dichalcogenides (1T-TaS 2 ) journal September 2016
Nature and evolution of incommensurate charge order in manganites visualized with cryogenic scanning transmission electron microscopy journal January 2018
On the correlation between self-diffusion and the low-frequency LA ⅔⟨111⟩ phonon mode in b.c.c. metals journal November 1988
A pnCCD-based, fast direct single electron imaging camera for TEM and STEM journal April 2016
Direct imaging of lithium atoms in LiV2O4 by spherical aberration-corrected electron microscopy journal April 2010
Performance of low-voltage STEM/TEM with delta corrector and cold field emission gun journal June 2010
Monochromated STEM with a 30 meV-wide, atom-sized electron probe journal January 2013
The potential for Bayesian compressive sensing to significantly reduce electron dose in high-resolution STEM images journal October 2013
Development of a monochromator for aberration-corrected scanning transmission electron microscopy journal February 2015
Development of high-resolution cathodoluminescence system for STEM and application to plasmonic nanostructures journal July 2016
Theory and practice of electron diffraction from single atoms and extended objects using an EMPAD journal December 2017
The influence of surfaces and interfaces on high spatial resolution vibrational EELS from SiO2 journal February 2018
Electrochemical aspects of the generation of ramified metallic electrodeposits journal December 1990
Roles of phonon amplitude and low-energy optical phonons on superionic conduction journal November 1997
Prospects of spatial resolution in vibrational electron energy loss spectroscopy: Implications of dipolar scattering journal December 2017
Suppression of Octahedral Tilts and Associated Changes in Electronic Properties at Epitaxial Oxide Heterostructure Interfaces journal August 2010
Exciton Mapping at Subwavelength Scales in Two-Dimensional Materials journal March 2015
Atomic-Resolution STEM Imaging of Graphene at Low Voltage of 30 kV with Resolution Enhancement by Using Large Convergence Angle journal April 2015
Electron-Beam Mapping of Vibrational Modes with Nanometer Spatial Resolution journal December 2016
Phonon Spectroscopy at Atomic Resolution journal January 2019
Vitrification of pure Water for Electron Microscopy journal December 1981
Electron microscopy of frozen hydrated sections of vitreous ice and vitrified biological samples journal July 1983
Direct observation of Σ7 domain boundary core structure in magnetic skyrmion lattice journal February 2016
Designer interphases for the lithium-oxygen electrochemical cell journal April 2017
Nanoscale momentum-resolved vibrational spectroscopy journal June 2018
Atomic-Scale Chemical Imaging of Composition and Bonding by Aberration-Corrected Microscopy journal February 2008
Imaging of Transient Structures Using Nanosecond in Situ TEM journal September 2008
4D Nanoscale Diffraction Observed by Convergent-Beam Ultrafast Electron Microscopy journal October 2009
Electron Vortex Beams with High Quanta of Orbital Angular Momentum journal January 2011
Atomic structure of sensitive battery materials and interfaces revealed by cryo–electron microscopy journal October 2017
Identification of site-specific isotopic labels by vibrational spectroscopy in the electron microscope journal January 2019
Plasmonics for improved photovoltaic devices book October 2010
Issues and challenges facing rechargeable lithium batteries book October 2010
Direct Imaging of Hydrogen within a Crystalline Environment journal November 2010
Crystallization Pathways in Biomineralization journal August 2011
Sub-Ångstrom electric field measurements on a universal detector in a scanning transmission electron microscope journal August 2018
In situ and operando transmission electron microscopy of catalytic materials journal January 2015
Resonant Coupling between Molecular Vibrations and Localized Surface Plasmon Resonance of Faceted Metal Oxide Nanocrystals. text January 2017
On the origin of differential phase contrast at a locally charged and globally charge-compensated domain boundary in a polar-ordered material text January 2015
In Situ Electron Energy-Loss Spectroscopy in Liquids text January 2012
Nanoscale Imaging of Lithium Ion Distribution During In Situ Operation of Battery Electrode and Electrolyte text January 2013
Probing low-energy hyperbolic polaritons in van der Waals crystals with an electron microscope text January 2016

Cited By (1)

Characterization of semiconductor photocatalysts journal January 2019