Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films
Abstract
We report the combination of small coercive fields and weak magnetic anisotropy makes soft ferromagnetic films extremely useful for nanoscale devices that need to easily switch spin directions. However, soft ferromagnets are relatively rare, particularly in ultrathin films with thicknesses of a few nanometers or less. We have synthesized large-area, high-quality, ultrathin freestanding LaMnO3 films on Si and found unexpected soft ferromagnetism along both the in-plane and out-of-plane directions when the film thickness was reduced to 4 nm. We argue that the vanishing magnetic anisotropy between the two directions is a consequence of two coexisting magnetic easy axes in different atomic layers of the LaMnO3 film. Spectroscopy measurements reveal a change in Mn valence from 3+ in the film interior to approximately 2+ at the surfaces where considerable hydrogen infiltration occurs due to the water dissolving process. First-principles calculations show that protonation of LaMnO3 decreases valence and Our the Mn switches the magnetic easy axis from in-plane to out-of-plane as the Mn valence approaches 2+ from its 3+ bulk value. Our work demonstrates that ultrathin freestanding films can exhibit functional properties that are absent in homogeneous materials, concomitant with their convenient compatibility with Si-based devices.
- Authors:
-
[1];
[5];
[7];
[8];
[5];
[10]
- University of Science and Technology of China, Hefei (China); ShanghaiTech University (China)
- East China Normal University, Shanghai (China); NYU Shanghai, Shanghai (China)
- ShanghaiTech University (China)
- Argonne National Laboratory (ANL), Lemont, IL (United States)
- National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)
- University of Science and Technology of China, Hefei (China)
- University of Illinois at Urbana-Champaign, IL (United States)
- Argonne National Laboratory (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
- NYU Shanghai, Shanghai (China); New York Univ. (NYU), NY (United States)
- School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation of China; Science and Technology Commission of Shanghai Municipality; NYU University Research Challenge Fund; National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1902641
- Grant/Contract Number:
- AC02-06CH11357; 52072244; 12104305; 21JC1405000; 11774236
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 16; Journal Issue: 5; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; freestanding oxides; hydrogen doping; interface and surface; magnetic anisotropy; soft ferromagnetism
Citation Formats
Lu, Qinwen, Liu, Zhiwei, Yang, Qun, Cao, Hui, Balakrishnan, Purnima, Wang, Qing, Cheng, Long, Lu, Yalin, Zuo, Jian-Min, Zhou, Hua, Quarterman, Patrick, Muramoto, Shin, Grutter, Alexander J., Chen, Hanghui, and Zhai, Xiaofang. Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films. United States: N. p., 2022.
Web. doi:10.1021/acsnano.1c11065.
Lu, Qinwen, Liu, Zhiwei, Yang, Qun, Cao, Hui, Balakrishnan, Purnima, Wang, Qing, Cheng, Long, Lu, Yalin, Zuo, Jian-Min, Zhou, Hua, Quarterman, Patrick, Muramoto, Shin, Grutter, Alexander J., Chen, Hanghui, & Zhai, Xiaofang. Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films. United States. https://doi.org/10.1021/acsnano.1c11065
Lu, Qinwen, Liu, Zhiwei, Yang, Qun, Cao, Hui, Balakrishnan, Purnima, Wang, Qing, Cheng, Long, Lu, Yalin, Zuo, Jian-Min, Zhou, Hua, Quarterman, Patrick, Muramoto, Shin, Grutter, Alexander J., Chen, Hanghui, and Zhai, Xiaofang. Thu .
"Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films". United States. https://doi.org/10.1021/acsnano.1c11065. https://www.osti.gov/servlets/purl/1902641.
@article{osti_1902641,
title = {Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films},
author = {Lu, Qinwen and Liu, Zhiwei and Yang, Qun and Cao, Hui and Balakrishnan, Purnima and Wang, Qing and Cheng, Long and Lu, Yalin and Zuo, Jian-Min and Zhou, Hua and Quarterman, Patrick and Muramoto, Shin and Grutter, Alexander J. and Chen, Hanghui and Zhai, Xiaofang},
abstractNote = {We report the combination of small coercive fields and weak magnetic anisotropy makes soft ferromagnetic films extremely useful for nanoscale devices that need to easily switch spin directions. However, soft ferromagnets are relatively rare, particularly in ultrathin films with thicknesses of a few nanometers or less. We have synthesized large-area, high-quality, ultrathin freestanding LaMnO3 films on Si and found unexpected soft ferromagnetism along both the in-plane and out-of-plane directions when the film thickness was reduced to 4 nm. We argue that the vanishing magnetic anisotropy between the two directions is a consequence of two coexisting magnetic easy axes in different atomic layers of the LaMnO3 film. Spectroscopy measurements reveal a change in Mn valence from 3+ in the film interior to approximately 2+ at the surfaces where considerable hydrogen infiltration occurs due to the water dissolving process. First-principles calculations show that protonation of LaMnO3 decreases valence and Our the Mn switches the magnetic easy axis from in-plane to out-of-plane as the Mn valence approaches 2+ from its 3+ bulk value. Our work demonstrates that ultrathin freestanding films can exhibit functional properties that are absent in homogeneous materials, concomitant with their convenient compatibility with Si-based devices.},
doi = {10.1021/acsnano.1c11065},
journal = {ACS Nano},
number = 5,
volume = 16,
place = {United States},
year = {Thu Apr 21 00:00:00 EDT 2022},
month = {Thu Apr 21 00:00:00 EDT 2022}
}
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