Charge Density Wave and Narrow Energy Gap at Room Temperature in 2D Pb3-xSb1+xS4Te2-δ with Square Te Sheets

Haijie Chen; Christos D. Malliakas; Awadhesh Narayan; Lei Fang; Duck Young Chung; Lucas K. Wagner; Wai Kwong Kwok; Mercouri G. Kanatzidis

doi:10.1021/jacs.7b06446

Charge Density Wave and Narrow Energy Gap at Room Temperature in 2D Pb_3-xSb_1+xS₄Te_2-δ with Square Te Sheets

Haijie Chen, Christos D. Malliakas, Awadhesh Narayan, Lei Fang, Duck Young Chung, Lucas K. Wagner, Wai Kwong Kwok, Mercouri G. Kanatzidis

Northwestern University

Research output: Contribution to journal › Article › peer-review

6 Citations (Scopus)

Abstract

We report a new two-dimensional compound, Pb_3-xSb_1+xS₄Te_2-δ, that has a charge density wave (CDW) at room temperature. The CDW is incommensurate with q-vector of 0.248(6)a∗ + 0.246(8)b∗ + 0.387(9)c∗ for x = 0.29(2) and δ = 0.37(3) due to positional and occupational long-range ordering of Te atoms in the sheets. The modulated structure was refined from the single-crystal X-ray diffraction data with a superspace group P1(αβγ)0 using (3 + 1)-dimensional crystallography. The resistivity increases with decreasing temperature, suggesting semiconducting behavior. The transition temperature (T_CDW) of the CDW is ∼345 K, above which the Te square sheets become disordered with no q-vector. First-principles density functional theory calculations on the undistorted structure and an approximate commensurate supercell reveal that the gap is due to the structure modulation.

Original language	English
Pages (from-to)	11271-11276
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	139
Issue number	32
DOIs	https://doi.org/10.1021/jacs.7b06446
Publication status	Published - Aug 16 2017

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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Charge Density Wave and Narrow Energy Gap at Room Temperature in 2D Pb_3-xSb_1+xS₄Te_2-δ with Square Te Sheets. / Chen, Haijie; Malliakas, Christos D.; Narayan, Awadhesh; Fang, Lei; Chung, Duck Young; Wagner, Lucas K.; Kwok, Wai Kwong; Kanatzidis, Mercouri G.

In: Journal of the American Chemical Society, Vol. 139, No. 32, 16.08.2017, p. 11271-11276.

Research output: Contribution to journal › Article › peer-review

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title = "Charge Density Wave and Narrow Energy Gap at Room Temperature in 2D Pb3-xSb1+xS4Te2-δ with Square Te Sheets",

abstract = "We report a new two-dimensional compound, Pb3-xSb1+xS4Te2-δ, that has a charge density wave (CDW) at room temperature. The CDW is incommensurate with q-vector of 0.248(6)a∗ + 0.246(8)b∗ + 0.387(9)c∗ for x = 0.29(2) and δ = 0.37(3) due to positional and occupational long-range ordering of Te atoms in the sheets. The modulated structure was refined from the single-crystal X-ray diffraction data with a superspace group P1(αβγ)0 using (3 + 1)-dimensional crystallography. The resistivity increases with decreasing temperature, suggesting semiconducting behavior. The transition temperature (TCDW) of the CDW is ∼345 K, above which the Te square sheets become disordered with no q-vector. First-principles density functional theory calculations on the undistorted structure and an approximate commensurate supercell reveal that the gap is due to the structure modulation.",

author = "Haijie Chen and Malliakas, {Christos D.} and Awadhesh Narayan and Lei Fang and Chung, {Duck Young} and Wagner, {Lucas K.} and Kwok, {Wai Kwong} and Kanatzidis, {Mercouri G.}",

note = "Funding Information: This work was supported by the Center for Emergent Superconductivity an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DEAC0298CH1088. Computational resources were provided by the University of Illinois Campus Cluster. This work made use of the Integrated Molecular Structure Education and Research Center (IMSERC) at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the State of Illinois and International Institute for Nanotechnology (IIN).",

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AU - Wagner, Lucas K.

AU - Kwok, Wai Kwong

AU - Kanatzidis, Mercouri G.

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N2 - We report a new two-dimensional compound, Pb3-xSb1+xS4Te2-δ, that has a charge density wave (CDW) at room temperature. The CDW is incommensurate with q-vector of 0.248(6)a∗ + 0.246(8)b∗ + 0.387(9)c∗ for x = 0.29(2) and δ = 0.37(3) due to positional and occupational long-range ordering of Te atoms in the sheets. The modulated structure was refined from the single-crystal X-ray diffraction data with a superspace group P1(αβγ)0 using (3 + 1)-dimensional crystallography. The resistivity increases with decreasing temperature, suggesting semiconducting behavior. The transition temperature (TCDW) of the CDW is ∼345 K, above which the Te square sheets become disordered with no q-vector. First-principles density functional theory calculations on the undistorted structure and an approximate commensurate supercell reveal that the gap is due to the structure modulation.

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