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.

doi:10.1021/jacs.9b02599

Title: 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

Journal Article · Thu Apr 11 00:00:00 EDT 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b02599· OSTI ID:1524424

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Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry, and Dept. of Materials Science and Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

We report the two-dimensional (2D) natural hetero-structure [Pb_3.1Sb_0.9S₄][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 [Pb3.1Sb0.9S4] 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 similar to ~1352 cm² V^-1 s^-1 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_3.1Sb_0.9S₄] 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 [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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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1524424

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 18; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 7 works

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References (62)

Van der Waals heterostructures Geim, A. K.; Grigorieva, I. V. Nature, Vol. 499, Issue 7459, p. 419-425 https://doi.org/10.1038/nature12385	journal	July 2013
Liquid Exfoliation of Layered Materials Nicolosi, V.; Chhowalla, M.; Kanatzidis, M. G. Science, Vol. 340, Issue 6139, p. 1226419 https://doi.org/10.1126/science.1226419	journal	June 2013
Electric Field Effect in Atomically Thin Carbon Films Novoselov, K. S. Science, Vol. 306, Issue 5696, p. 666-669 https://doi.org/10.1126/science.1102896	journal	October 2004
Mobility engineering and a metal–insulator transition in monolayer MoS2 Radisavljevic, Branimir; Kis, Andras Nature Materials, Vol. 12, Issue 9 https://doi.org/10.1038/nmat3687	journal	June 2013
Ultrasensitive photodetectors based on monolayer MoS2 Lopez-Sanchez, Oriol; Lembke, Dominik; Kayci, Metin Nature Nanotechnology, Vol. 8, Issue 7 https://doi.org/10.1038/nnano.2013.100	journal	June 2013
Large, non-saturating magnetoresistance in WTe2 Ali, Mazhar N.; Xiong, Jun; Flynn, Steven Nature, Vol. 514, Issue 7521 https://doi.org/10.1038/nature13763	journal	September 2014
Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng Nature, Vol. 508, Issue 7496, p. 373-377 https://doi.org/10.1038/nature13184	journal	April 2014
Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe Zhao, L.-D.; Tan, G.; Hao, S. Science, Vol. 351, Issue 6269, p. 141-144 https://doi.org/10.1126/science.aad3749	journal	November 2015
Anisotropic Dirac Fermions in a Bi Square Net of ${SrMnBi}_{2}$ Park, Joonbum; Lee, G.; Wolff-Fabris, F. Physical Review Letters, Vol. 107, Issue 12 https://doi.org/10.1103/PhysRevLett.107.126402	journal	September 2011
A magnetic topological semimetal Sr1−yMn1−zSb2 (y, z < 0.1) Liu, J. Y.; Hu, J.; Zhang, Q. Nature Materials, Vol. 16, Issue 9 https://doi.org/10.1038/nmat4953	journal	July 2017
Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals Gong, Cheng; Li, Lin; Li, Zhenglu Nature, Vol. 546, Issue 7657 https://doi.org/10.1038/nature22060	journal	April 2017
Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit Huang, Bevin; Clark, Genevieve; Navarro-Moratalla, Efrén Nature, Vol. 546, Issue 7657 https://doi.org/10.1038/nature22391	journal	June 2017
Giant tunneling magnetoresistance in spin-filter van der Waals heterostructures Song, Tiancheng; Cai, Xinghan; Tu, Matisse Wei-Yuan Science, Vol. 360, Issue 6394 https://doi.org/10.1126/science.aar4851	journal	May 2018
Electric-field switching of two-dimensional van der Waals magnets Jiang, Shengwei; Shan, Jie; Mak, Kin Fai Nature Materials, Vol. 17, Issue 5 https://doi.org/10.1038/s41563-018-0040-6	journal	March 2018
2D Intrinsic Ferromagnets from van der Waals Antiferromagnets Miao, Naihua; Xu, Bin; Zhu, Linggang Journal of the American Chemical Society, Vol. 140, Issue 7 https://doi.org/10.1021/jacs.7b12976	journal	February 2018
Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds Mounet, Nicolas; Gibertini, Marco; Schwaller, Philippe Nature Nanotechnology, Vol. 13, Issue 3 https://doi.org/10.1038/s41565-017-0035-5	journal	February 2018
Ligand-field helical luminescence in a 2D ferromagnetic insulator Seyler, Kyle L.; Zhong, Ding; Klein, Dahlia R. Nature Physics, Vol. 14, Issue 3 https://doi.org/10.1038/s41567-017-0006-7	journal	December 2017
Magnetism in two-dimensional van der Waals materials Burch, Kenneth S.; Mandrus, David; Park, Je-Geun Nature, Vol. 563, Issue 7729 https://doi.org/10.1038/s41586-018-0631-z	journal	October 2018
Dirac cone protected by non-symmorphic symmetry and three-dimensional Dirac line node in ZrSiS Schoop, Leslie M.; Ali, Mazhar N.; Straßer, Carola Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11696	journal	May 2016
Observation of topological nodal fermion semimetal phase in ZrSiS Neupane, Madhab; Belopolski, Ilya; Hosen, M. Mofazzel Physical Review B, Vol. 93, Issue 20 https://doi.org/10.1103/PhysRevB.93.201104	journal	May 2016
Large nonsaturating magnetoresistance and signature of nondegenerate Dirac nodes in ZrSiS Singha, Ratnadwip; Pariari, Arnab Kumar; Satpati, Biswarup Proceedings of the National Academy of Sciences, Vol. 114, Issue 10 https://doi.org/10.1073/pnas.1618004114	journal	February 2017
The crystal structure of synthetic buckhornite, [Pb ₂ BiS ₃ ][AuTe ₂ ] Effenberger, H.; Culetto, F. J.; Topa, D. Zeitschrift für Kristallographie - Crystalline Materials, Vol. 215, Issue 1 https://doi.org/10.1524/zkri.2000.215.1.10	journal	January 2000
Two-Dimensional Mineral [Pb ₂ BiS ₃ ][AuTe ₂ ]: High-Mobility Charge Carriers in Single-Atom-Thick Layers Fang, Lei; Im, Jino; Stoumpos, Constantinos C. Journal of the American Chemical Society, Vol. 137, Issue 6 https://doi.org/10.1021/ja5111688	journal	February 2015
Large spin-orbit coupling and helical spin textures in 2D heterostructure [Pb2BiS3][AuTe2] Fang, L.; Im, J.; DeGottardi, W. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep35313	journal	October 2016
Synthesis and physical properties of cylindrite micro tubes and lamellae: Synthesis and physical properties of cylindrite micro tubes and lamellae Kaden, Ronny; Wagner, Gerald; Sturm, Chris physica status solidi (b), Vol. 247, Issue 6 https://doi.org/10.1002/pssb.200945594	journal	May 2010
Abramovite, Pb2SnInBiS7, a new mineral species from fumaroles of the Kudryavy volcano, Kurile Islands, Russia Yudovskaya, M. A.; Trubkin, N. V.; Koporulina, E. V. Geology of Ore Deposits, Vol. 50, Issue 7 https://doi.org/10.1134/S1075701508070052	journal	December 2008
Merelaniite, Mo4Pb4VSbS15, a New Molybdenum-Essential Member of the Cylindrite Group, from the Merelani Tanzanite Deposit, Lelatema Mountains, Manyara Region, Tanzania Jaszczak, John; Rumsey, Michael; Bindi, Luca Minerals, Vol. 6, Issue 4 https://doi.org/10.3390/min6040115	journal	October 2016
La lévyclaudite, Pb8Sn7Cu3(Bi,Sb)3S28, une nouvelle espèce à structure incommensurable, de la série de la cylindrite [La lévyclaudite, Pb8Sn7Cu3(Bi,Sb)3S28, une nouvelle espèce à structure incommensurable, de la série de la cylindrite] Moëlo, Yves; Makovicky, Emil; Karup-Moller, Sven European Journal of Mineralogy, Vol. 2, Issue 5 https://doi.org/10.1127/ejm/2/5/0711	journal	October 1990
Jaszczakite, [(Bi, Pb)3 S3][AuS2], a new mineral species from Nagybörzsöny, Hungary [Jaszczakite, [(Bi, Pb)3 S3][AuS2], a new mineral species from Nagybörzsöny, Hungary] Bindi, Luca; Paar, Werner H. European Journal of Mineralogy, Vol. 29, Issue 4 https://doi.org/10.1127/ejm/2017/0029-2620	journal	October 2017
Franckeite as a naturally occurring van der Waals heterostructure Molina-Mendoza, Aday J.; Giovanelli, Emerson; Paz, Wendel S. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14409	journal	February 2017
First (3 + 2)-dimensional superspace approach to the structure of levyclaudite-(Sb), a member of the cylindrite-type minerals Evain, Michel; Petricek, Vaclav; Moëlo, Yves Acta Crystallographica Section B Structural Science, Vol. 62, Issue 5 https://doi.org/10.1107/S010876810602547X	journal	September 2006
Crystal structure of a synthetic tin-selenium representative of the cylindrite structure type Makovicky, E.; Petricek, V.; Dusek, M. American Mineralogist, Vol. 93, Issue 11-12 https://doi.org/10.2138/am.2008.2910	journal	November 2008
Nb–Nb Interactions Define the Charge Density Wave Structure of 2H-NbSe ₂ Malliakas, Christos D.; Kanatzidis, Mercouri G. Journal of the American Chemical Society, Vol. 135, Issue 5 https://doi.org/10.1021/ja3120554	journal	January 2013
Charge Density Wave and Narrow Energy Gap at Room Temperature in 2D Pb _{3– x} Sb _{1+ x} S ₄ Te _2−δ with Square Te Sheets Chen, Haijie; Malliakas, Christos D.; Narayan, Awadhesh Journal of the American Chemical Society, Vol. 139, Issue 32 https://doi.org/10.1021/jacs.7b06446	journal	August 2017
Tellurides from Sunrise Dam gold deposit, Yilgarn Craton, Western Australia: a new occurrence of nagyágite Sung, Y. -H.; Ciobanu, C. L.; Pring, A. Mineralogy and Petrology, Vol. 91, Issue 3-4 https://doi.org/10.1007/s00710-007-0199-z	journal	August 2007
Toward the crystal structure of nagyagite, [Pb(Pb,Sb)S ₂ ][(Au,Te)] Effenberger, Herta; Paar, Werner H.; Topa, Dan American Mineralogist, Vol. 84, Issue 4 https://doi.org/10.2138/am-1999-0420	journal	April 1999
Crystallographic Computing System JANA2006: General features Petříček, Václav; Dušek, Michal; Palatinus, Lukáš Zeitschrift für Kristallographie - Crystalline Materials, Vol. 229, Issue 5 https://doi.org/10.1515/zkri-2014-1737	journal	January 2014
Giant magnetoresistance of manganese oxides with a layered perovskite structure Moritomo, Y.; Asamitsu, A.; Kuwahara, H. Nature, Vol. 380, Issue 6570 https://doi.org/10.1038/380141a0	journal	March 1996
Giant Magnetoresistance of (001)Fe/(001)Cr Magnetic Superlattices Baibich, M. N.; Broto, J. M.; Fert, A. Physical Review Letters, Vol. 61, Issue 21 https://doi.org/10.1103/PhysRevLett.61.2472	journal	November 1988
Copper Vacancies and Heavy Holes in the Two-Dimensional Semiconductor KCu _{3– x} Se ₂ Rettie, Alexander J. E.; Sturza, Mihai; Malliakas, Christos D. Chemistry of Materials, Vol. 29, Issue 14 https://doi.org/10.1021/acs.chemmater.7b02117	journal	July 2017
High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu ₄ Se ₄ Synthesized by a Unique Pathway Chen, Haijie; Rodrigues, João N. B.; Rettie, Alexander J. E. Journal of the American Chemical Society, Vol. 141, Issue 1 https://doi.org/10.1021/jacs.8b11911	journal	November 2018
Ab initio molecular dynamics for open-shell transition metals Kresse, G.; Hafner, J. Physical Review B, Vol. 48, Issue 17 https://doi.org/10.1103/PhysRevB.48.13115	journal	November 1993
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Graphene: Status and Prospects Geim, A. K. Science, Vol. 324, Issue 5934, p. 1530-1534 https://doi.org/10.1126/science.1158877	journal	June 2009
Physics of Semiconductor Devices Sze, S. M.; Ng, Kwok K. https://doi.org/10.1002/0470068329	book	January 2007
Conduction in glasses containing transition metal ions Mott, N. F. Journal of Non-Crystalline Solids, Vol. 1, Issue 1 https://doi.org/10.1016/0022-3093(68)90002-1	journal	December 1968
The New Phase [Tl ₄ Sb ₆ Se ₁₀ ][Sn ₅ Sb ₂ Se ₁₄ ]: A Naturally Formed Semiconducting Heterostructure with Two-Dimensional Conductance Fang, Lei; Iyer, Ratnasabapathy G.; Tan, Gangjian Journal of the American Chemical Society, Vol. 136, Issue 31 https://doi.org/10.1021/ja505301y	journal	July 2014
Variable Range Hopping Conduction in Semiconductor Nanocrystal Solids Yu, Dong; Wang, Congjun; Wehrenberg, Brian L. Physical Review Letters, Vol. 92, Issue 21 https://doi.org/10.1103/PhysRevLett.92.216802	journal	May 2004
Formation of the layered conductive magnet CrCl2(pyrazine)2 through redox-active coordination chemistry Pedersen, Kasper S.; Perlepe, Panagiota; Aubrey, Michael L. Nature Chemistry, Vol. 10, Issue 10 https://doi.org/10.1038/s41557-018-0107-7	journal	September 2018
Weak antilocalization and localization in disordered and interacting Weyl semimetals Lu, Hai-Zhou; Shen, Shun-Qing Physical Review B, Vol. 92, Issue 3 https://doi.org/10.1103/PhysRevB.92.035203	journal	July 2015
Gate-tunable negative longitudinal magnetoresistance in the predicted type-II Weyl semimetal WTe2 Wang, Yaojia; Liu, Erfu; Liu, Huimei Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13142	journal	October 2016
Chiral magnetic effect in ZrTe5 Li, Qiang; Kharzeev, Dmitri E.; Zhang, Cheng Nature Physics, Vol. 12, Issue 6 https://doi.org/10.1038/nphys3648	journal	February 2016
Colossal negative magnetoresistance in a two-dimensional electron gas Shi, Q.; Martin, P. D.; Ebner, Q. A. Physical Review B, Vol. 89, Issue 20 https://doi.org/10.1103/PhysRevB.89.201301	journal	May 2014
Gigantic negative magnetoresistance in the bulk of a disordered topological insulator Breunig, Oliver; Wang, Zhiwei; Taskin, A. A. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15545	journal	May 2017
Colossal magnetoresistance Ramirez, A. P. Journal of Physics: Condensed Matter, Vol. 9, Issue 39 https://doi.org/10.1088/0953-8984/9/39/005	journal	September 1997
Colossal magnetoresistance in Cr-based chalcogenide spinels Ramirez, A. P.; Cava, R. J.; Krajewski, J. Nature, Vol. 386, Issue 6621 https://doi.org/10.1038/386156a0	journal	March 1997
Chiral anomaly and classical negative magnetoresistance of Weyl metals Son, D. T.; Spivak, B. Z. Physical Review B, Vol. 88, Issue 10 https://doi.org/10.1103/PhysRevB.88.104412	journal	September 2013
Chiral Anomaly and Diffusive Magnetotransport in Weyl Metals Burkov, A. A. Physical Review Letters, Vol. 113, Issue 24 https://doi.org/10.1103/PhysRevLett.113.247203	journal	December 2014
Observation of the Chiral-Anomaly-Induced Negative Magnetoresistance in 3D Weyl Semimetal TaAs Huang, Xiaochun; Zhao, Lingxiao; Long, Yujia Physical Review X, Vol. 5, Issue 3 https://doi.org/10.1103/PhysRevX.5.031023	journal	August 2015

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Title: 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

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Title: 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