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Femtosecond photoexcitation of semiconducting materials leads to the generation of coherent acoustic phonons (CAPs), the behaviours of which are linked to intrinsic and engineered electronic, optical and structural properties. While often studied with pump-probe spectroscopic techniques, the influence of nanoscale structure and morphology on CAP dynamics can be challenging to resolve with these all-optical methods. Here, we used ultrafast electron microscopy (UEM) to resolve variations in CAP dynamics caused by differences in the degree of crystallinity in as-prepared and annealed GaAs lamellae. Following in situ femtosecond photoexcitation, we directly imaged the generation and propagation dynamics of hypersonic CAPs in a mostly amorphous and, following an in situ photothermal anneal, a mostly crystalline lamella. Subtle differences in both the initial hypersonic velocities and the asymptotic relaxation behaviours were resolved via construction of space-time contour plots from phonon wavefronts. Comparison to bulk sound velocities in crystalline and amorphous GaAs reveals the influence of the mixed amorphous-crystalline morphology on CAP dispersion behaviours. Further, an increase in the asymptotic velocity following annealing establishes the sensitivity of quantitative UEM imaging to both structural and compositional variations through differences in bonding and elasticity. Implications of extending the methods and results reported here to elucidating correlated electronic, optical and structural behaviours in semiconducting materials are discussed. This article is part of a discussion meeting issue 'Dynamic in situ microscopy relating structure and function'.
|Original language||English (US)|
|Journal||Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences|
|State||Published - Dec 11 2020|
Bibliographical noteFunding Information:
Data accessibility. Data has been uploaded to the Data Repository of the University of Minnesota and can be freely accessed at this link: http://hdl.handle.net/11299/212097 or via the https://doi.org/10.13020/36wa-rj64. Authors’ contributions. E.J.V. contributions were formal analysis, investigation, methodology, software, validation, visualization, writing—original draft, writing—review and editing. D.J.F. contributions were conceptualization, formal analysis, funding acquisition, methodology, project administration, resources, supervision, visualization, writing—original draft, writing—review and editing. Competing interests. The author(s) declare that they have no competing interests. Funding. This material is based on work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award No. DE-SC0018204. This material is based upon work supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1348264. Part of this work was carried out in the College of Science and Engineering Characterization Facility, University of Minnesota, which has received capital equipment funding from the NSF through the UMN MRSEC program under Award Number DMR-2011401.
- Ultrafast electron microscopy
- coherent acoustic phonons
- gallium arsenide
- in situ electron microscopy
How much support was provided by MRSEC?
Reporting period for MRSEC
- Period 7
- Period 1
PubMed: MeSH publication types
- Journal Article
9/1/20 → 8/31/26
Project: Research project
11/1/14 → …
Project: Research project
High-Resolution Analog of Time-Domain Phonon Spectroscopy in the TEM Experimental Data and Analysis 2019-2020
Vandenbussche, E. & Flannigan, D. J., Data Repository for the University of Minnesota, May 12 2020