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.
|Original language||English (US)|
|Number of pages||10|
|Journal||Journal of the American Chemical Society|
|State||Published - Apr 11 2019|
ASJC Scopus subject areas
- Colloid and Surface Chemistry
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CSD 1912405: Experimental Crystal Structure Determination
Chen, H. (Contributor), He, J. (Contributor), Malliakas, C. D. (Contributor), Stoumpos, C. C. (Contributor), Rettie, A. J. E. (Contributor), Bao, J. (Contributor), Chung, D. Y. (Contributor), Kwok, W. (Contributor), Wolverton, C. M. (Contributor) & Kanatzidis, M. (Contributor), FIZ Karlsruhe - Leibniz Institute for Information Infrastructure, 2019
DOI: 10.25505/fiz.icsd.cc2260ht, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc2260ht&sid=DataCite
CSD 1912404: Experimental Crystal Structure Determination
Chen, H. (Creator), He, J. (Creator), Malliakas, C. D. (Creator), Stoumpos, C. C. (Creator), Rettie, A. J. E. (Creator), Bao, J. (Creator), Chung, D. Y. (Creator), Kwok, W. (Creator), Wolverton, C. M. (Creator) & Kanatzidis, M. (Creator), FIZ Karlsruhe – Leibniz Institute for Information Infrastructure, 2019
DOI: 10.25505/fiz.icsd.cc2260gs, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc2260gs&sid=DataCite