Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy
Abstract
The An+1BnO3n+1 Ruddlesden–Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of the intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden–Popper phases. Lastly, we demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La3Ni2O7.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States); Korea Atomic Energy Research Institute, Daejeon (Republic of Korea)
- Univ. of Wisconsin, Madison, WI (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Science and Technology of China, Anhui (China)
- Univ. of Connecticut, Storrs, CT (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Materials Sciences and Engineering Division; University of Wisconsin-Madison, Materials Research Science and Engineering Center (MRSEC)
- OSTI Identifier:
- 1357212
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 9; Journal ID: ISSN 1476-1122
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; design; synthesis and processing; surfaces; interfaces and thin films
Citation Formats
Lee, J. H., Luo, G., Tung, I. C., Chang, S. H., Luo, Z., Malshe, M., Gadre, M., Bhattacharya, A., Nakhmanson, S. M., Eastman, J. A., Hong, H., Jellinek, J., Morgan, D., Fong, D. D., and Freeland, J. W. Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy. United States: N. p., 2014.
Web. doi:10.1038/NMAT4039.
Lee, J. H., Luo, G., Tung, I. C., Chang, S. H., Luo, Z., Malshe, M., Gadre, M., Bhattacharya, A., Nakhmanson, S. M., Eastman, J. A., Hong, H., Jellinek, J., Morgan, D., Fong, D. D., & Freeland, J. W. Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy. United States. https://doi.org/10.1038/NMAT4039
Lee, J. H., Luo, G., Tung, I. C., Chang, S. H., Luo, Z., Malshe, M., Gadre, M., Bhattacharya, A., Nakhmanson, S. M., Eastman, J. A., Hong, H., Jellinek, J., Morgan, D., Fong, D. D., and Freeland, J. W. Sun .
"Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy". United States. https://doi.org/10.1038/NMAT4039. https://www.osti.gov/servlets/purl/1357212.
@article{osti_1357212,
title = {Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy},
author = {Lee, J. H. and Luo, G. and Tung, I. C. and Chang, S. H. and Luo, Z. and Malshe, M. and Gadre, M. and Bhattacharya, A. and Nakhmanson, S. M. and Eastman, J. A. and Hong, H. and Jellinek, J. and Morgan, D. and Fong, D. D. and Freeland, J. W.},
abstractNote = {The An+1BnO3n+1 Ruddlesden–Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of the intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden–Popper phases. Lastly, we demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La3Ni2O7.},
doi = {10.1038/NMAT4039},
journal = {Nature Materials},
number = 9,
volume = 13,
place = {United States},
year = {Sun Aug 03 00:00:00 EDT 2014},
month = {Sun Aug 03 00:00:00 EDT 2014}
}
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