Synthesis of the Candidate Topological Compound Ni3Pb2

Alexandra D. Tamerius; Alison B. Altman; Michael J. Waters; Eric A. Riesel; Christos D. Malliakas; Matthew L. Whitaker; Tony Yu; Gilberto Fabbris; Yue Meng; Daniel Haskel; Yanbin Wang; Steven D. Jacobsen; James M. Rondinelli; Danna E. Freedman

doi:10.1021/jacs.2c03485

Synthesis of the Candidate Topological Compound Ni₃Pb₂

Alexandra D. Tamerius, Alison B. Altman, Michael J. Waters, Eric A. Riesel, Christos D. Malliakas, Matthew L. Whitaker, Tony Yu, Gilberto Fabbris, Yue Meng, Daniel Haskel, Yanbin Wang, Steven D. Jacobsen, James M. Rondinelli^*, Danna E. Freedman^*

^*Corresponding author for this work

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

3 Scopus citations

Abstract

Spin-orbit coupling enables the realization of topologically nontrivial ground states. As spin-orbit coupling increases with increasing atomic number, compounds featuring heavy elements, such as lead, offer a pathway toward creating new topologically nontrivial materials. By employing a high-pressure flux synthesis method, we synthesized single crystals of Ni₃Pb₂, the first structurally characterized bulk binary phase in the Ni-Pb system. Combining experimental and theoretical techniques, we examined structure and bonding in Ni₃Pb₂, revealing the impact of chemical substitutions on electronic structure features of importance for controlling topological behavior. From these results, we determined that Ni₃Pb₂completes a series of structurally related transition-metal-heavy main group intermetallic materials that exhibit diverse electronic structures, opening a platform for synthetically tunable topologically nontrivial materials.

Original language	English (US)
Pages (from-to)	11943-11948
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	144
Issue number	27
DOIs	https://doi.org/10.1021/jacs.2c03485
State	Published - Jul 13 2022

Funding

The authors would like to thank Dr. James P. S. Walsh, Dr. Doug H. Fabini, Dr. Ryan A. Klein, Dr. Lei Sun, Dr. Chung-Jui Yu, Dr. Stephen W. von Kugelgen, and Dr. Michael K. Wojnar for helpful discussions, and Dr. Chung-Jui Yu for assistance with the table of contents graphic. Experimental work was supported by the AFOSR (FA9550-17-1-0247). S.D.J. acknowledges support from the NSF (DMR-1508577) and beamtime provided through the Chicago/DOE Alliance Center. A.B.A. acknowledges support from the IIN Postdoctoral Fellowship and the Northwestern University International Institute of Nanotechnology. The multianvil cell assemblies used were from the COMPRES Cell Assembly Project, which was supported by COMPRES under NSF Cooperative Agreement EAR 1661511. This research used resources at XPD (sector 28) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Use of the MAXPD Endstation was supported by COMPRES, the Consortium for Materials Properties Research in Earth Sciences, under NSF Cooperative Agreement No. EAR 16-61511, and by the Mineral Physics Institute, Department of Geosciences, Stony Brook University. A portion of this work was performed at GeoSoilEnviroCARS (Sector 13), Advanced Photon Source (APS), Argonne National Laboratory (ANL). GeoSoilEnviroCARS is supported by the National Science Foundation-Earth Sciences (EAR 0217473), Department of Energy–Geosciences (DE-FG02-94ER14466) and the State of Illinois. A portion of this work was performed at HPCAT (Sector 16), APS, ANL. HPCAT operations are supported by DOE-NNSA’s Office of Experimental Sciences. The APS is a Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by ANL under Contract No. DE-AC02-06CH11357. M.J.W. and J.M.R. acknowledge support from the National Science Foundation (NSF) under Award Number DMR-2011208. Calculations were performed using the Center for Nanoscale Materials (Carbon) Cluster, an Office of Science user facility supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357 and the National Energy Research Scientific Computing Center (NERSC), a U.S. DOE Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. This work made use of the EPIC facility of the NUANCE Center, and IMSERC, which is supported by Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSFECCS-2025633); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN.

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

Access to Document

10.1021/jacs.2c03485

Cite this

@article{78682c0791b243d7b00cb3215648726d,

title = "Synthesis of the Candidate Topological Compound Ni3Pb2",

abstract = "Spin-orbit coupling enables the realization of topologically nontrivial ground states. As spin-orbit coupling increases with increasing atomic number, compounds featuring heavy elements, such as lead, offer a pathway toward creating new topologically nontrivial materials. By employing a high-pressure flux synthesis method, we synthesized single crystals of Ni3Pb2, the first structurally characterized bulk binary phase in the Ni-Pb system. Combining experimental and theoretical techniques, we examined structure and bonding in Ni3Pb2, revealing the impact of chemical substitutions on electronic structure features of importance for controlling topological behavior. From these results, we determined that Ni3Pb2completes a series of structurally related transition-metal-heavy main group intermetallic materials that exhibit diverse electronic structures, opening a platform for synthetically tunable topologically nontrivial materials.",

author = "Tamerius, {Alexandra D.} and Altman, {Alison B.} and Waters, {Michael J.} and Riesel, {Eric A.} and Malliakas, {Christos D.} and Whitaker, {Matthew L.} and Tony Yu and Gilberto Fabbris and Yue Meng and Daniel Haskel and Yanbin Wang and Jacobsen, {Steven D.} and Rondinelli, {James M.} and Freedman, {Danna E.}",

note = "Funding Information: The authors would like to thank Dr. James P. S. Walsh, Dr. Doug H. Fabini, Dr. Ryan A. Klein, Dr. Lei Sun, Dr. Chung-Jui Yu, Dr. Stephen W. von Kugelgen, and Dr. Michael K. Wojnar for helpful discussions, and Dr. Chung-Jui Yu for assistance with the table of contents graphic. Experimental work was supported by the AFOSR (FA9550-17-1-0247). S.D.J. acknowledges support from the NSF (DMR-1508577) and beamtime provided through the Chicago/DOE Alliance Center. A.B.A. acknowledges support from the IIN Postdoctoral Fellowship and the Northwestern University International Institute of Nanotechnology. The multianvil cell assemblies used were from the COMPRES Cell Assembly Project, which was supported by COMPRES under NSF Cooperative Agreement EAR 1661511. This research used resources at XPD (sector 28) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Use of the MAXPD Endstation was supported by COMPRES, the Consortium for Materials Properties Research in Earth Sciences, under NSF Cooperative Agreement No. EAR 16-61511, and by the Mineral Physics Institute, Department of Geosciences, Stony Brook University. A portion of this work was performed at GeoSoilEnviroCARS (Sector 13), Advanced Photon Source (APS), Argonne National Laboratory (ANL). GeoSoilEnviroCARS is supported by the National Science Foundation-Earth Sciences (EAR 0217473), Department of Energy–Geosciences (DE-FG02-94ER14466) and the State of Illinois. A portion of this work was performed at HPCAT (Sector 16), APS, ANL. HPCAT operations are supported by DOE-NNSA{\textquoteright}s Office of Experimental Sciences. The APS is a Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by ANL under Contract No. DE-AC02-06CH11357. M.J.W. and J.M.R. acknowledge support from the National Science Foundation (NSF) under Award Number DMR-2011208. Calculations were performed using the Center for Nanoscale Materials (Carbon) Cluster, an Office of Science user facility supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357 and the National Energy Research Scientific Computing Center (NERSC), a U.S. DOE Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. This work made use of the EPIC facility of the NUANCE Center, and IMSERC, which is supported by Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSFECCS-2025633); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = jul,

day = "13",

doi = "10.1021/jacs.2c03485",

language = "English (US)",

volume = "144",

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journal = "Journal of the American Chemical Society",

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T1 - Synthesis of the Candidate Topological Compound Ni3Pb2

AU - Tamerius, Alexandra D.

AU - Altman, Alison B.

AU - Waters, Michael J.

AU - Riesel, Eric A.

AU - Malliakas, Christos D.

AU - Whitaker, Matthew L.

AU - Yu, Tony

AU - Fabbris, Gilberto

AU - Meng, Yue

AU - Haskel, Daniel

AU - Wang, Yanbin

AU - Jacobsen, Steven D.

AU - Rondinelli, James M.

AU - Freedman, Danna E.

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PY - 2022/7/13

Y1 - 2022/7/13

N2 - Spin-orbit coupling enables the realization of topologically nontrivial ground states. As spin-orbit coupling increases with increasing atomic number, compounds featuring heavy elements, such as lead, offer a pathway toward creating new topologically nontrivial materials. By employing a high-pressure flux synthesis method, we synthesized single crystals of Ni3Pb2, the first structurally characterized bulk binary phase in the Ni-Pb system. Combining experimental and theoretical techniques, we examined structure and bonding in Ni3Pb2, revealing the impact of chemical substitutions on electronic structure features of importance for controlling topological behavior. From these results, we determined that Ni3Pb2completes a series of structurally related transition-metal-heavy main group intermetallic materials that exhibit diverse electronic structures, opening a platform for synthetically tunable topologically nontrivial materials.

AB - Spin-orbit coupling enables the realization of topologically nontrivial ground states. As spin-orbit coupling increases with increasing atomic number, compounds featuring heavy elements, such as lead, offer a pathway toward creating new topologically nontrivial materials. By employing a high-pressure flux synthesis method, we synthesized single crystals of Ni3Pb2, the first structurally characterized bulk binary phase in the Ni-Pb system. Combining experimental and theoretical techniques, we examined structure and bonding in Ni3Pb2, revealing the impact of chemical substitutions on electronic structure features of importance for controlling topological behavior. From these results, we determined that Ni3Pb2completes a series of structurally related transition-metal-heavy main group intermetallic materials that exhibit diverse electronic structures, opening a platform for synthetically tunable topologically nontrivial materials.

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Synthesis of the Candidate Topological Compound Ni₃Pb₂

Abstract

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CSD 2163166: Experimental Crystal Structure Determination

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Synthesis of the Candidate Topological Compound Ni3Pb2

Abstract

Funding

ASJC Scopus subject areas

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Datasets

CSD 2163166: Experimental Crystal Structure Determination

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Synthesis of the Candidate Topological Compound Ni₃Pb₂