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Title: Electric Field–Controlled Multistep Proton Evolution in H x SrCoO 2.5 with Formation of H–H Dimer

Journal Article · · Advanced Science
 [1];  [2];  [3];  [4];  [5];  [6];  [3];  [7];  [7];  [7];  [7];  [7];  [8];  [9];  [7];  [10];  [11];  [12];  [13];  [14] more »;  [13];  [15]; ORCiD logo [16] « less
  1. Tsinghua Univ., Beijing (China). State Key Lab. of Low Dimensional Quantum Physics. Dept. of Physics; DOE/OSTI
  2. Fudan Univ., Shanghai (China). Key Lab. of Computational Physical Sciences (Ministry of Education). State Key Lab. of Surface Physics. Dept. of Physics
  3. Tsinghua Univ., Beijing (China). State Key Lab. of Low Dimensional Quantum Physics. Dept. of Physics
  4. National Center for Electron Microscopy in Beijing,(China). Key Lab. of Advanced Materials (MOE); Tsinghua Univ., Beijing (China). State Key Lab. of New Ceramics and Fine Processing. School of Materials Science and Engineering
  5. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China)
  6. Collaborative Innovation Center of Quantum Matter, Beijing (China); Peking Univ., Beijing (China). International Center for Quantum Materials. School of Physics
  7. Tsinghua Univ., Beijing (China). State Key Lab. of Low Dimensional Quantum Physics. Dept. of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China)
  8. Tsinghua Univ., Beijing (China). State Key Lab. of Low Dimensional Quantum Physics. Dept. of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China); Tsinghua Univ., Beijing (China). Dept. of Mechanical Engineering
  9. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  10. Peking Univ., Beijing (China). International Center for Quantum Materials. School of Physics
  11. Durham Univ. (United Kingdom). Dept. of Physics
  12. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics; Chinese Academy of Sciences (CAS), Beijing (China). School of Physical Sciences; Collaborative Innovation Center of Quantum Matter, Beijing (China)
  13. National Center for Electron Microscopy in Beijing (China). Key Laboratory of Advanced Materials (MOE); Tsinghua Univ., Beijing (China). State Key Lab. of New Ceramics and Fine Processing. School of Materials Science and Engineering
  14. Tsinghua Univ., Beijing (China). State Key Lab. of New Ceramics and Fine Processing. School of Materials Science and Engineering
  15. Fudan Univ., Shanghai (China). Key Lab. of Computational Physical Sciences (Ministry of Education). State Key Lab. of Surface Physics. Dept. of Physics; Collaborative Innovation Center of Advanced Microstructures, Nanjing (China)
  16. Tsinghua Univ., Beijing (China). State Key Lab. of Low Dimensional Quantum Physics. Dept. of Physics; Collaborative Innovation Center of Quantum Matter Beijing (China); RIKEN Center for Emergent Matter Science (CEMS), Saitama (Japan)
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Ionic evolution–induced phase transformation can lead to wide ranges of novel material functionalities with promising applications. Here, using the gating voltage during ionic liquid gating as a tuning knob, the brownmillerite SrCoO2.5 is transformed into a series of protonated HxSrCoO2.5 phases with distinct hydrogen contents. The unexpected electron to charge-neutral doping crossover along with the increase of proton concentration from x = 1 to 2 suggests the formation of exotic charge neutral H–H dimers for higher proton concentration, which is directly visualized at the vacant tetrahedron by scanning transmission electron microscopy and then further supported by first principles calculations. Although the H–H dimers cause no change of the valency of Co2+ ions, they result in clear enhancement of electronic bandgap and suppression of magnetization through lattice expansion. These results not only reveal a hydrogen chemical state beyond anion and cation within the complex oxides, but also suggest an effective pathway to design functional materials through tunable ionic evolution.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1623477
Journal Information:
Advanced Science, Journal Name: Advanced Science Journal Issue: 20 Vol. 6; ISSN 2198-3844
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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