High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu4Se4 Synthesized by a Unique Pathway.
Abstract
The new compound NaCu4Se4 forms by the reaction of CuO and Cu in a molten sodium polyselenide flux, with the existence of CuO being unexpectedly critical to its synthesis. It adopts a layered hexagonal structure (space group P63/mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu4Se4]-slabs separated by Na+ cations. X-ray photoelectron spectroscopy suggests that NaCu4Se4 is mixed-valent with the formula (Na+)-(Cu+)4(Se2-)(Se-)(Se2)2-. NaCu4Se4 is a p-type metal with a carrier density of similar to ~1021 cm-3 and a high hole mobility of similar to ~808 cm2 s-1 at 2 K based on electronic transport measurements. First-principles calculations suggest the density of states around the Fermi level are composed of Cu-d and Se-p orbitals. At 2 K, a very large transverse magnetoresistance of similar to 1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Furthermore, our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1492394
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 1; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; flux synthesis; magnetoresistance; metal; two-dimensional material
Citation Formats
Chen, Haijie, Rodrigues, Joao N. B., Rettie, Alexander J. E., Song, Tze -Bin, Chica, Daniel G., Su, Xianli, Bao, Jin -Ke, Chung, Duck Young, Kwok, Wai -Kwong, Wagner, Lucas K., and Kanatzidis, Mercouri G. High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu4Se4 Synthesized by a Unique Pathway.. United States: N. p., 2018.
Web. doi:10.1021/jacs.8b11911.
Chen, Haijie, Rodrigues, Joao N. B., Rettie, Alexander J. E., Song, Tze -Bin, Chica, Daniel G., Su, Xianli, Bao, Jin -Ke, Chung, Duck Young, Kwok, Wai -Kwong, Wagner, Lucas K., & Kanatzidis, Mercouri G. High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu4Se4 Synthesized by a Unique Pathway.. United States. https://doi.org/10.1021/jacs.8b11911
Chen, Haijie, Rodrigues, Joao N. B., Rettie, Alexander J. E., Song, Tze -Bin, Chica, Daniel G., Su, Xianli, Bao, Jin -Ke, Chung, Duck Young, Kwok, Wai -Kwong, Wagner, Lucas K., and Kanatzidis, Mercouri G. Tue .
"High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu4Se4 Synthesized by a Unique Pathway.". United States. https://doi.org/10.1021/jacs.8b11911. https://www.osti.gov/servlets/purl/1492394.
@article{osti_1492394,
title = {High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu4Se4 Synthesized by a Unique Pathway.},
author = {Chen, Haijie and Rodrigues, Joao N. B. and Rettie, Alexander J. E. and Song, Tze -Bin and Chica, Daniel G. and Su, Xianli and Bao, Jin -Ke and Chung, Duck Young and Kwok, Wai -Kwong and Wagner, Lucas K. and Kanatzidis, Mercouri G.},
abstractNote = {The new compound NaCu4Se4 forms by the reaction of CuO and Cu in a molten sodium polyselenide flux, with the existence of CuO being unexpectedly critical to its synthesis. It adopts a layered hexagonal structure (space group P63/mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu4Se4]-slabs separated by Na+ cations. X-ray photoelectron spectroscopy suggests that NaCu4Se4 is mixed-valent with the formula (Na+)-(Cu+)4(Se2-)(Se-)(Se2)2-. NaCu4Se4 is a p-type metal with a carrier density of similar to ~1021 cm-3 and a high hole mobility of similar to ~808 cm2 s-1 at 2 K based on electronic transport measurements. First-principles calculations suggest the density of states around the Fermi level are composed of Cu-d and Se-p orbitals. At 2 K, a very large transverse magnetoresistance of similar to 1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Furthermore, our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.},
doi = {10.1021/jacs.8b11911},
journal = {Journal of the American Chemical Society},
number = 1,
volume = 141,
place = {United States},
year = {Tue Dec 11 00:00:00 EST 2018},
month = {Tue Dec 11 00:00:00 EST 2018}
}
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