Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands
Abstract
Tailoring electron transfer dynamics across solid–liquid interfaces is fundamental to the interconversion of electrical and chemical energy. Stacking atomically thin layers with a small azimuthal misorientation to produce moiré superlattices enables the controlled engineering of electronic band structures and the formation of extremely flat electronic bands. Here, we report a strong twist-angle dependence of heterogeneous charge transfer kinetics at twisted bilayer graphene electrodes with the greatest enhancement observed near the ‘magic angle’ (~1.1°). Furthermore, this effect is driven by the angle-dependent tuning of moiré-derived flat bands that modulate electron transfer processes with the solution-phase redox couple. Combined experimental and computational analysis reveals that the variation in electrochemical activity with moiré angle is controlled by a structural relaxation of the moiré superlattice at twist angles of <2°, and ‘topological defect’ AA stacking regions, where flat bands are localized, produce a large anomalous local electrochemical enhancement that cannot be accounted for by the elevated local density of states alone.
- Authors:
-
- Univ. of California, Berkeley, CA (United States)
- Carnegie Mellon Univ., Pittsburgh, PA (United States)
- Brown Univ., Providence, RI (United States)
- National Institute for Materials Science (NIMS), Tsukuba (Japan). International Center for Materials Nanoarchitectonics
- National Institute for Materials Science (NIMS), Tsukuba (Japan). Research Center for Functional Materials
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Office of Naval Research (ONR); JSPS KAKENHI; National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR)
- OSTI Identifier:
- 1924027
- Alternate Identifier(s):
- OSTI ID: 1877557
- Grant/Contract Number:
- AC02-05CH11231; SC0021049; N00014-18-S-F009; OIA-1921199; N00014-20-1-2599; 19H05790; 20H00354; 21H05233
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Chemistry
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 3; Journal ID: ISSN 1755-4330
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; computational chemistry; electrochemistry; electron transfer; graphene; two-dimensional materials; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; moiré superlattices
Citation Formats
Yu, Yun, Zhang, Kaidi, Parks, Holden, Babar, Mohammad, Carr, Stephen, Craig, Isaac M., Van Winkle, Madeline, Lyssenko, Artur, Taniguchi, Takashi, Watanabe, Kenji, Viswanathan, Venkatasubramanian, and Bediako, D. Kwabena. Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands. United States: N. p., 2022.
Web. doi:10.1038/s41557-021-00865-1.
Yu, Yun, Zhang, Kaidi, Parks, Holden, Babar, Mohammad, Carr, Stephen, Craig, Isaac M., Van Winkle, Madeline, Lyssenko, Artur, Taniguchi, Takashi, Watanabe, Kenji, Viswanathan, Venkatasubramanian, & Bediako, D. Kwabena. Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands. United States. https://doi.org/10.1038/s41557-021-00865-1
Yu, Yun, Zhang, Kaidi, Parks, Holden, Babar, Mohammad, Carr, Stephen, Craig, Isaac M., Van Winkle, Madeline, Lyssenko, Artur, Taniguchi, Takashi, Watanabe, Kenji, Viswanathan, Venkatasubramanian, and Bediako, D. Kwabena. Thu .
"Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands". United States. https://doi.org/10.1038/s41557-021-00865-1. https://www.osti.gov/servlets/purl/1924027.
@article{osti_1924027,
title = {Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands},
author = {Yu, Yun and Zhang, Kaidi and Parks, Holden and Babar, Mohammad and Carr, Stephen and Craig, Isaac M. and Van Winkle, Madeline and Lyssenko, Artur and Taniguchi, Takashi and Watanabe, Kenji and Viswanathan, Venkatasubramanian and Bediako, D. Kwabena},
abstractNote = {Tailoring electron transfer dynamics across solid–liquid interfaces is fundamental to the interconversion of electrical and chemical energy. Stacking atomically thin layers with a small azimuthal misorientation to produce moiré superlattices enables the controlled engineering of electronic band structures and the formation of extremely flat electronic bands. Here, we report a strong twist-angle dependence of heterogeneous charge transfer kinetics at twisted bilayer graphene electrodes with the greatest enhancement observed near the ‘magic angle’ (~1.1°). Furthermore, this effect is driven by the angle-dependent tuning of moiré-derived flat bands that modulate electron transfer processes with the solution-phase redox couple. Combined experimental and computational analysis reveals that the variation in electrochemical activity with moiré angle is controlled by a structural relaxation of the moiré superlattice at twist angles of <2°, and ‘topological defect’ AA stacking regions, where flat bands are localized, produce a large anomalous local electrochemical enhancement that cannot be accounted for by the elevated local density of states alone.},
doi = {10.1038/s41557-021-00865-1},
journal = {Nature Chemistry},
number = 3,
volume = 14,
place = {United States},
year = {Thu Feb 17 00:00:00 EST 2022},
month = {Thu Feb 17 00:00:00 EST 2022}
}
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