A Natural 2D Heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] with Large Transverse Nonsaturating Negative Magnetoresistance and High Electron Mobility

Haijie Chen, Jiangang He, Christos D. Malliakas, Constantinos C. Stoumpos, Alexander J.E. Rettie, Jin Ke Bao, Duck Young Chung, Wai Kwong Kwok, Christopher Wolverton, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

Abstract

We report the two-dimensional (2D) natural heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] (x = 0.52-0.36) which shows anomalous, transverse nonsaturating negative magnetoresistance (MR). For x = 0.52, the material has a commensurately modulated structure with alternating [Pb 3.1 Sb 0.9 S 4 ] rocksalt layers and atomically thin [Au x Te 2-x ] sheets, as determined by single-crystal X-ray diffraction using a (3 + 1)-dimensional space group; for other x compositions, the modulated structure is absent and the Au and Te atoms are disordered. The transport properties in this system at low temperature (<100 K) are dominated by an unusual 2D hopping mechanism, while at room temperature a high carrier mobility of 1352 cm 2 V -1 s -1 is obtained (x = 0.36). The confined electrons within the [Au x Te 2-x ] layers are also exposed to interlayer coupling with the insulating [Pb 3.1 Sb 0.9 S 4 ] layers, and as a result, the properties of the heterostructures emerge not only from the constituent layers but also the interactions between them. Furthermore, the various Au and Te coordination patterns found in the [Au x Te 2-x ] sheets as a function of x further contribute to a unique electronic structure that leads to the anomalous nonsaturating negative MR with different field dependent behaviors. First-principles calculations indicate that the [Au x Te 2-x ] sheets are responsible for the unusual electrical transport properties in this 2D system.

Original languageEnglish
Pages (from-to)7544-7553
Number of pages10
JournalJournal of the American Chemical Society
Volume141
Issue number18
DOIs
Publication statusPublished - Apr 11 2019

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Electron mobility
Magnetoresistance
Transport properties
Heterojunctions
Electrons
Temperature
Carrier mobility
X-Ray Diffraction
Electronic structure
Single crystals
X ray diffraction
Atoms
Chemical analysis

ASJC Scopus subject areas

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

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A Natural 2D Heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] with Large Transverse Nonsaturating Negative Magnetoresistance and High Electron Mobility . / Chen, Haijie; He, Jiangang; Malliakas, Christos D.; Stoumpos, Constantinos C.; Rettie, Alexander J.E.; Bao, Jin Ke; Chung, Duck Young; Kwok, Wai Kwong; Wolverton, Christopher; Kanatzidis, Mercouri G.

In: Journal of the American Chemical Society, Vol. 141, No. 18, 11.04.2019, p. 7544-7553.

Research output: Contribution to journalArticle

Chen, Haijie ; He, Jiangang ; Malliakas, Christos D. ; Stoumpos, Constantinos C. ; Rettie, Alexander J.E. ; Bao, Jin Ke ; Chung, Duck Young ; Kwok, Wai Kwong ; Wolverton, Christopher ; Kanatzidis, Mercouri G. / A Natural 2D Heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] with Large Transverse Nonsaturating Negative Magnetoresistance and High Electron Mobility In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 18. pp. 7544-7553.
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abstract = "We report the two-dimensional (2D) natural heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] (x = 0.52-0.36) which shows anomalous, transverse nonsaturating negative magnetoresistance (MR). For x = 0.52, the material has a commensurately modulated structure with alternating [Pb 3.1 Sb 0.9 S 4 ] rocksalt layers and atomically thin [Au x Te 2-x ] sheets, as determined by single-crystal X-ray diffraction using a (3 + 1)-dimensional space group; for other x compositions, the modulated structure is absent and the Au and Te atoms are disordered. The transport properties in this system at low temperature (<100 K) are dominated by an unusual 2D hopping mechanism, while at room temperature a high carrier mobility of 1352 cm 2 V -1 s -1 is obtained (x = 0.36). The confined electrons within the [Au x Te 2-x ] layers are also exposed to interlayer coupling with the insulating [Pb 3.1 Sb 0.9 S 4 ] layers, and as a result, the properties of the heterostructures emerge not only from the constituent layers but also the interactions between them. Furthermore, the various Au and Te coordination patterns found in the [Au x Te 2-x ] sheets as a function of x further contribute to a unique electronic structure that leads to the anomalous nonsaturating negative MR with different field dependent behaviors. First-principles calculations indicate that the [Au x Te 2-x ] sheets are responsible for the unusual electrical transport properties in this 2D system.",
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T1 - A Natural 2D Heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] with Large Transverse Nonsaturating Negative Magnetoresistance and High Electron Mobility

AU - Chen, Haijie

AU - He, Jiangang

AU - Malliakas, Christos D.

AU - Stoumpos, Constantinos C.

AU - Rettie, Alexander J.E.

AU - Bao, Jin Ke

AU - Chung, Duck Young

AU - Kwok, Wai Kwong

AU - Wolverton, Christopher

AU - Kanatzidis, Mercouri G

PY - 2019/4/11

Y1 - 2019/4/11

N2 - We report the two-dimensional (2D) natural heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] (x = 0.52-0.36) which shows anomalous, transverse nonsaturating negative magnetoresistance (MR). For x = 0.52, the material has a commensurately modulated structure with alternating [Pb 3.1 Sb 0.9 S 4 ] rocksalt layers and atomically thin [Au x Te 2-x ] sheets, as determined by single-crystal X-ray diffraction using a (3 + 1)-dimensional space group; for other x compositions, the modulated structure is absent and the Au and Te atoms are disordered. The transport properties in this system at low temperature (<100 K) are dominated by an unusual 2D hopping mechanism, while at room temperature a high carrier mobility of 1352 cm 2 V -1 s -1 is obtained (x = 0.36). The confined electrons within the [Au x Te 2-x ] layers are also exposed to interlayer coupling with the insulating [Pb 3.1 Sb 0.9 S 4 ] layers, and as a result, the properties of the heterostructures emerge not only from the constituent layers but also the interactions between them. Furthermore, the various Au and Te coordination patterns found in the [Au x Te 2-x ] sheets as a function of x further contribute to a unique electronic structure that leads to the anomalous nonsaturating negative MR with different field dependent behaviors. First-principles calculations indicate that the [Au x Te 2-x ] sheets are responsible for the unusual electrical transport properties in this 2D system.

AB - We report the two-dimensional (2D) natural heterostructure [Pb 3.1 Sb 0.9 S 4 ][Au x Te 2-x ] (x = 0.52-0.36) which shows anomalous, transverse nonsaturating negative magnetoresistance (MR). For x = 0.52, the material has a commensurately modulated structure with alternating [Pb 3.1 Sb 0.9 S 4 ] rocksalt layers and atomically thin [Au x Te 2-x ] sheets, as determined by single-crystal X-ray diffraction using a (3 + 1)-dimensional space group; for other x compositions, the modulated structure is absent and the Au and Te atoms are disordered. The transport properties in this system at low temperature (<100 K) are dominated by an unusual 2D hopping mechanism, while at room temperature a high carrier mobility of 1352 cm 2 V -1 s -1 is obtained (x = 0.36). The confined electrons within the [Au x Te 2-x ] layers are also exposed to interlayer coupling with the insulating [Pb 3.1 Sb 0.9 S 4 ] layers, and as a result, the properties of the heterostructures emerge not only from the constituent layers but also the interactions between them. Furthermore, the various Au and Te coordination patterns found in the [Au x Te 2-x ] sheets as a function of x further contribute to a unique electronic structure that leads to the anomalous nonsaturating negative MR with different field dependent behaviors. First-principles calculations indicate that the [Au x Te 2-x ] sheets are responsible for the unusual electrical transport properties in this 2D system.

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