Title: Reversible manipulation of the magnetic state in SrRuO₃ through electric-field controlled proton evolution

Abstract

Ionic substitution forms an essential pathway to manipulate the structural phase, carrier density and crystalline symmetry of materials via ion-electron-lattice coupling, leading to a rich spectrum of electronic states in strongly correlated systems. Using the ferromagnetic metal SrRuO3 as a model system, we demonstrate an efficient and reversible control of both structural and electronic phase transformations through the electric-field controlled proton evolution with ionic liquid gating. The insertion of protons results in a large structural expansion and increased carrier density, leading to an exotic ferromagnetic to paramagnetic phase transition. Importantly, we reveal a novel protonated compound of HSrRuO3 with paramagnetic metallic as ground state. We observe a topological Hall effect at the boundary of the phase transition due to the proton concentration gradient across the film-depth. We envision that electric-field controlled protonation opens up a pathway to explore novel electronic states and material functionalities in protonated material systems.

Authors:

Li, Zhuolu ^[1]; Shen, Shengchun ^[1]; Tian, Zijun ^[2]; Hwangbo, Kyle ^[3]; Wang, Meng  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-0297-1180"
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Wang, Yujia ^[1]; Bartram, F. Michael ^[3]; He, Liqun  ^[3];

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• Search DOE PAGES for ORCID "0000-0002-7417-448X"
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Lyu, Yingjie ^[1]; Dong, Yongqi ^[4]; Wan, Gang ^[5]; Li, Haobo ^[1]; Lu, Nianpeng ^[6]; Zang, Jiadong ^[7]; Zhou, Hua ^[5]; Arenholz, Elke ^[8]; He, Qing ^[9]; Yang, Luyi  ^[10];

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• Search DOE PAGES for ORCID "0000-0001-6260-1395"
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Luo, Weidong  ^[11];

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• Search DOE PAGES for ORCID "0000-0003-3829-1547"
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Yu, Pu ^[12]

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+ Show Author Affiliations

1. Tsinghua Univ., Beijing (China)
2. Shanghai Jiao Tong Univ. (China)
3. Univ. of Toronto, ON (Canada)
4. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Science and Technology of China, Hefei (China)
5. Argonne National Lab. (ANL), Argonne, IL (United States)
6. Tsinghua Univ., Beijing (China); Chinese Academy of Sciences (CAS), Beijing (China)
7. Univ. of New Hampshire, Durham, NH (United States)
8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
9. Durham Univ. (United Kingdom)
10. Tsinghua Univ., Beijing (China); Univ. of Toronto, ON (Canada); Frontier Science Center for Quantum Information, Beijing (China)
11. Shanghai Jiao Tong Univ. (China); Collaborative Innovation Center of Advanced Microstructures, Nanjing (China)
12. Tsinghua Univ., Beijing (China); Frontier Science Center for Quantum Information, Beijing (China); Inst. of Physical and Chemical Research (RIKEN), Wako (Japan)

Publication Date:

2020-01-10

Research Org.:

Univ. of New Hampshire, Durham, NH (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NNSFC); National Basic Research Program of China

OSTI Identifier:

1596536

Alternate Identifier(s):

OSTI ID: 1659705

Grant/Contract Number:  

SC0020221; AC02-06CH11357; AC02-05CH11231

Resource Type:

Accepted Manuscript

Journal Name:

Nature Communications

Additional Journal Information:

Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE