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Atomic resolution mapping of phonon excitations in STEM-EELS experiments

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 Added by Ricardo Egoavil
 Publication date 2014
  fields Physics
and research's language is English




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Atomically resolved electron energy-loss spectroscopy experiments are commonplace in modern aberrationcorrected transmission electron microscopes. Energy resolution has also been increasing steadily with the continuous improvement of electron monochromators. Electronic excitations however are known to be delocalised due to the long range interaction of the charged accelerated electrons with the electrons in a sample. This has made several scientists question the value of combined high spatial and energy resolution for mapping interband transitions and possibly phonon excitation in crystals. In this paper we demonstrate experimentally that atomic resolution information is indeed available at very low energy losses around 100 meV expressed as a modulation of the broadening of the zero loss peak. Careful data analysis allows us to get a glimpse of what are likely phonon excitations with both an energy loss and gain part. These experiments confirm recent theoretical predictions on the strong localisation of phonon excitations as opposed to electronic excitations and show that a combination of atomic resolution and recent developments in increased energy resolution will offer great benefit for mapping phonon modes in real space.



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The high beam current and sub-angstrom resolution of aberration-corrected scanning transmission electron microscopes has enabled electron energy loss spectroscopic (EELS) mapping with atomic resolution. These spectral maps are often dose-limited and spatially oversampled, leading to low counts/channel and are thus highly sensitive to errors in background estimation. However, by taking advantage of redundancy in the dataset map one can improve background estimation and increase chemical sensitivity. We consider two such approaches- linear combination of power laws and local background averaging-that reduce background error and improve signal extraction. Principal components analysis (PCA) can also be used to analyze spectrum images, but the poor peak-to-background ratio in EELS can lead to serious artifacts if raw EELS data is PCA filtered. We identify common artifacts and discuss alternative approaches. These algorithms are implemented within the Cornell Spectrum Imager, an open source software package for spectroscopic analysis.
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3He nanobubbles created by radioactive decay of tritium in palladium tritide are investigated after several years of aging. Scanning Transmission Electron Microscopy Electron Energy-Loss Spectroscopy (STEM-EELS) has been used to measure helium density from the helium K-edge around 23 eV. Helium densities were found between 20 and 140 (+/-30) He/nm3 and the corresponding nanobubble pressures range between 0.1 and 3 (+/-0.2) GPa. Measuring helium density and mapping He atoms by STEM-EELS enables to differentiate bubbles from empty cavities in the palladium tritide matrix.
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