Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO3 Films

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

doi:10.1021/acsnano.1c11065

Engineering Magnetic Anisotropy and Emergent Multidirectional Soft Ferromagnetism in Ultrathin Freestanding LaMnO₃ Films

Journal Article · Thu Apr 21 00:00:00 EDT 2022 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.1c11065· OSTI ID:1902641

^[1]; Liu, Zhiwei ^[2]; Yang, Qun ^[3]; Cao, Hui ^[4]; ^[5]; Wang, Qing ^[3]; Cheng, Long ^[3]; Lu, Yalin ^[6]; ^[7]; ^[8]; Quarterman, Patrick ^[5]; Muramoto, Shin ^[5]; ^[5]; Chen, Hanghui ^[9]; ^[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

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Lemont, IL (United States)

Sponsoring Organization:: NYU University Research Challenge Fund; National Natural Science Foundation of China; National Science Foundation of China; Science and Technology Commission of Shanghai Municipality; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1902641

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 5 Vol. 16; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
freestanding oxides
hydrogen doping
interface and surface
magnetic anisotropy
soft ferromagnetism