Real-time studies of the mechanisms of nanocrystal structural phase changes

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Abstract/Contents

Abstract
Nanocrystals provide ideal systems with which to study structural phase changes. By making use of the ultra-short pulsed nature of synchrotrons and free-electron lasers, one may visualize with atomic-resolution and in real time how nanosized systems rearrange and potentially resolve the transition state itself. Such information could lead to new material design opportunities in which the phase-change behavior is optimal for a given application. Here are presented ultrafast studies of both temperature and pressure-driven phase changes in nanocrystalline materials, utilizing x-ray diffraction and x-ray spectroscopy to monitor the atomic rearrangement on femtosecond time-scales. For a thermally-driven phase change, the onset of superionicity is considered, a unique superposition of liquid-like cationic conductivity within a solid-phase anionic lattice. Using near-edge spectroscopy, the superionic structural transformation is observed to occur faster than twenty picoseconds in laser-excited copper (I) sulfide nanocrystals, and it is shown that it is the ionic hopping time which determines this time-scale. For pressure-induced studies, the dynamics of the well-known change of cadmium selenide nanocrystals from a wurtzite to rock-salt unit cell under increasing pressure are investigated. Laser-induced shock compression is used to initiate the phase transformation and hard x-ray scattering acts as as the probe. Finally, the efforts to introduce time-resolved capabilities at SSRL are presented. In particular, measurements of the x-ray pulse duration under different synchrotron operating conditions show the ability to perform experiments with single-picosecond resolution at SSRL. These single-photon sensitive measurements allowed the optimization of the pulse compression for future x-ray experiments at SSRL.

Description

Type of resource text
Form electronic; electronic resource; remote
Extent 1 online resource.
Publication date 2012
Issuance monographic
Language English

Creators/Contributors

Associated with Miller, Timothy Alan
Associated with Stanford University, Department of Materials Science and Engineering
Primary advisor Lindenberg, Aaron Michael
Thesis advisor Lindenberg, Aaron Michael
Thesis advisor Reis, David A, 1970-
Thesis advisor Toney, Michael Folsom
Advisor Reis, David A, 1970-
Advisor Toney, Michael Folsom

Subjects

Genre Theses

Bibliographic information

Statement of responsibility Timothy Alan Miller.
Note Submitted to the Department of Materials Science and Engineering.
Thesis Thesis (Ph.D.)--Stanford University, 2012.
Location electronic resource

Access conditions

Copyright
© 2012 by Timothy Alan Miller
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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