Vibrational Spectroscopy at Atomic Resolution with Electron Impact Scattering

Abstract

Atomic vibrations control all thermally activated processes in materials including diffusion, heat transport, phase transformations, and surface chemistry. Recent developments in monochromated, aberration-corrected scanning transmission electron microscopy (STEM) have enabled nanoscale probing of vibrational modes using a focused electron beam. However, to date, no experimental atomic resolution vibrational spectroscopy has been reported. Here we demonstrate atomic resolution by exploiting localized impact excitations of vibrational modes in materials. We show that the impact signal yields high spatial resolution in both covalent and ionic materials, and atomic resolution is available from both optical and acoustic vibrational modes. We achieve a spatial resolution of better than 2 Å which is an order of magnitude improvement compared to previous work. Our approach represents an important technical advance that can be used to provide new insights into the relationship between the thermal, elastic and kinetic properties of materials and atomic structural heterogeneities.

29 pages main text, 9 figures

References in corpus (2)

• Probing low-energy hyperbolic polaritons in van der Waals crystals with an electron microscope
• Localization of high-energy electron scattering from atomic vibrations

Cited by in corpus (29)

• Light-matter interactions with photonic quasiparticles
• Measuring phonon dispersion at an interface
• Experimental Observation of Localized Interfacial Phonon Modes
• Atomic-scale origin of the low grain-boundary resistance in perovskite solid electrolytes
• Nanoscale Phonon Spectroscopy Reveals Emergent Interface Vibrational Structure of Superlattices
• Physics discovery in nanoplasmonic systems via autonomous experiments in Scanning Transmission Electron Microscopy
• Four-dimensional Vibrational Spectroscopy for Nanoscale Mapping of Phonon Dispersion in BN Nanotubes
• Efficient and versatile model for vibrational STEM-EELS
• Imaging of isotope diffusion using atomic-scale vibrational spectroscopy
• Capturing 3D atomic defects and phonon localization at the 2D heterostructure interface
• Atomic resolution mapping of localized phonon modes at grain boundaries
• Quantum state heralding using photonic integrated circuits with free electrons
• The frequency-resolved frozen phonon multislice method and its application to vibrational EELS using parallel illumination
• Phonon transition across an isotopic interface
• Lossless monochromation for electron microscopy with pulsed photoemission sources and rf cavities
• Magnon diffuse scattering in scanning transmission electron microscopy
• Real-Space Visualization of Frequency-Dependent Anisotropy of Atomic Vibrations
• Simultaneous excitation of phonons at the center and boundaries of Brillouin zones with high energy electron beams
• Simulations of angle- and spatially-resolved vibrational electron energy loss spectroscopy for a system with a planar defect
• Creation and Microscopic Origins of Single-Photon Emitters in Transition Metal Dichalcogenides and Hexagonal Boron Nitride
• Perspective on Atomic-Resolution Vibrational Electron Energy-Loss Spectroscopy
• Atomic-Scale Vibrational Mapping and Isotope Identification with Electron Beams
• Localized Phonon Densities of States at Grain Boundaries in Silicon
• Four-Dimensional Imaging of Lattice Dynamics using Inelastic Scattering
• Electron and Light Induced Stimulated Raman Spectroscopy for Nanoscale Molecular Mapping
• Atomic-Scale Probing of Heterointerface Phonon Bridges in Nitride Semiconductor
• Single-dislocation phonons: atomic-scale measurement and their thermal properties
• Spectroscopic Observation and Modeling of Photonic Modes in CeO2 Nanocubes
• Platform and Framework for Time-Resolved Nanoscale Thermal Transport Measurements in STEM