Chen, H;
He, J;
Malliakas, CD;
Stoumpos, CC;
Rettie, AJE;
Bao, J-K;
Chung, DY;
... Kanatzidis, MG; + view all
(2019)
A Natural 2D Heterostructure [Pb3.1Sb0.9S4][AuxTe2-x] with Large Transverse Nonsaturating Negative Magnetoresistance and High Electron Mobility.
Journal of the American Chemical Society
, 141
(18)
pp. 7544-7553.
10.1021/jacs.9b02599.
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Abstract
We report the two-dimensional (2D) natural heterostructure [Pb3.1Sb0.9S4][AuxTe2–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 [Pb3.1Sb0.9S4] rocksalt layers and atomically thin [AuxTe2–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 cm2 V–1 s–1 is obtained (x = 0.36). The confined electrons within the [AuxTe2–x] layers are also exposed to interlayer coupling with the insulating [Pb3.1Sb0.9S4] 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 [AuxTe2–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 [AuxTe2–x] sheets are responsible for the unusual electrical transport properties in this 2D system.
| Type: | Article |
|---|---|
| Title: | A Natural 2D Heterostructure [Pb3.1Sb0.9S4][AuxTe2-x] with Large Transverse Nonsaturating Negative Magnetoresistance and High Electron Mobility |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/jacs.9b02599 |
| Publisher version: | https://doi.org/10.1021/jacs.9b02599 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Crystal structure, Gold, Layers, Magnetic properties, Mobility |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10072506 |
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