High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu 4 Se 4 Synthesized by a Unique Pathway

Haijie Chen, Joao N.B. Rodrigues, Alexander J.E. Rettie, Tze Bin Song, Daniel G. Chica, Xianli Su, Jin Ke Bao, Duck Young Chung, Wai Kwong Kwok, Lucas Kyle Wagner, Mercouri G. Kanatzidis

Research output: Contribution to journalArticle

Abstract

The new compound NaCu 4 Se 4 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 P6 3 /mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu 4 Se 4 ] - slabs separated by Na + cations. X-ray photoelectron spectroscopy suggests that NaCu 4 Se 4 is mixed-valent with the formula (Na + )(Cu + ) 4 (Se 2- )(Se - )(Se 2 ) 2- . NaCu 4 Se 4 is a p-type metal with a carrier density of â10 21 cm -3 and a high hole mobility of â808 cm 2 V -1 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 â1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.

Original languageEnglish (US)
Pages (from-to)635-642
Number of pages8
JournalJournal of the American Chemical Society
Volume141
Issue number1
DOIs
StatePublished - Jan 9 2019

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Giant magnetoresistance
Hole mobility
Metals
Photoelectron Spectroscopy
metal
Magnetoresistance
Fermi level
Oxides
X-ray spectroscopy
Carrier concentration
Cations
Molten materials
slab
X ray photoelectron spectroscopy
cation
Positive ions
Sodium
sodium
Fluxes
calculation

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu 4 Se 4 Synthesized by a Unique Pathway . / 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 Kyle; Kanatzidis, Mercouri G.

In: Journal of the American Chemical Society, Vol. 141, No. 1, 09.01.2019, p. 635-642.

Research output: Contribution to journalArticle

Chen, H, Rodrigues, JNB, Rettie, AJE, Song, TB, Chica, DG, Su, X, Bao, JK, Chung, DY, Kwok, WK, Wagner, LK & Kanatzidis, MG 2019, ' High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu 4 Se 4 Synthesized by a Unique Pathway ', Journal of the American Chemical Society, vol. 141, no. 1, pp. 635-642. 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 Kyle ; Kanatzidis, Mercouri G. / High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu 4 Se 4 Synthesized by a Unique Pathway In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 1. pp. 635-642.
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abstract = "The new compound NaCu 4 Se 4 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 P6 3 /mmc with cell parameters a = 3.9931(6) {\AA} and c = 25.167(5) {\AA}), consisting of infinite two-dimensional [Cu 4 Se 4 ] - slabs separated by Na + cations. X-ray photoelectron spectroscopy suggests that NaCu 4 Se 4 is mixed-valent with the formula (Na + )(Cu + ) 4 (Se 2- )(Se - )(Se 2 ) 2- . NaCu 4 Se 4 is a p-type metal with a carrier density of {\^a}10 21 cm -3 and a high hole mobility of {\^a}808 cm 2 V -1 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 {\^a}1400{\%} was observed, with a nonsaturating, linear dependence on field up to 9 T. Our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.",
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AB - The new compound NaCu 4 Se 4 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 P6 3 /mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu 4 Se 4 ] - slabs separated by Na + cations. X-ray photoelectron spectroscopy suggests that NaCu 4 Se 4 is mixed-valent with the formula (Na + )(Cu + ) 4 (Se 2- )(Se - )(Se 2 ) 2- . NaCu 4 Se 4 is a p-type metal with a carrier density of â10 21 cm -3 and a high hole mobility of â808 cm 2 V -1 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 â1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.

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