Anisotropic Structural Collapse of Mg3Sb2 and Mg3Bi2 at High Pressure

Calderón-Cueva, Mario; Peng, Wanyue; Clarke, Samantha M.; Ding, Jingxuan; Brugman, Benjamin L.; Levental, Gill; Balodhi, Ashiwini; Rylko, Megan; Delaire, Olivier; Walsh, James S.; Dorfman, Susannah M.; Zevalkink, Alexandra

doi:10.1021/acs.chemmater.0c03678

Title: Anisotropic Structural Collapse of Mg₃Sb₂ and Mg₃Bi₂ at High Pressure

Journal Article · Tue Jan 12 00:00:00 EST 2021 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.0c03678· OSTI ID:1765294

^[1]; Peng, Wanyue ^[1];

^[2]; Ding, Jingxuan ^[3]; Brugman, Benjamin L. ^[1]; Levental, Gill ^[1];

^[1]; Rylko, Megan ^[1]; Delaire, Olivier ^[3];

^[4]; Dorfman, Susannah M. ^[1];

^[1]

Michigan State Univ., East Lansing, MI (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Duke Univ., Durham, NC (United States)
Univ. of Massachusetts, Amherst, MA (United States)

Alloys between Mg₃Sb₂ and Mg₃Bi₂ have recently been shown to be exceptional thermoelectric materials due in part to their anomalously low thermal conductivity. In the present study, in situ high-pressure synchrotron X-ray diffraction was used to investigate the structure and bonding in Mg₃Sb₂ and Mg₃Bi₂ at pressures up to 50 GPa. Our results confirm prior predictions of isotropic in-plane and out-of-plane compressibility but reveal large disparities between the bond strength of the two distinct Mg sites. Using single-crystal diffraction, we show that the octahedral Mg–Sb bonds are significantly more compressible than the tetrahedral Mg–Sb bonds in Mg₃Sb₂, which lends support to prior arguments that the weaker octahedral Mg bonds are responsible for the anomalous thermal properties of Mg₃Sb₂ and Mg₃Bi₂. Further, we report the discovery of a displacive and reversible phase transition in both Mg₃Sb₂ and Mg₃Bi₂ above 7.8 and 4.0 GPa, respectively. Furthermore, the transition to the high-pressure structure involves a highly anisotropic volume collapse, in which the out-of-plane axis compresses significantly more than the in-plane axes. Single-crystal diffraction at high pressure was used to solve the monoclinic high-pressure structure (C2/m), which is a distorted variant of the ambient-pressure structure containing four unique Mg coordination environments.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Univ. of Illinois, Chicago, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-07NA27344; NA0003975; SC0019252; SC0019299; FG02-94ER14466; AC02-06CH11357; EAR-1634415

OSTI ID:: 1765294

Alternate ID(s):: OSTI ID: 1774968

Report Number(s):: LLNL-JRNL-814732; 1023098

Journal Information:: Chemistry of Materials, Vol. 33, Issue 2; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (41)

Pressure-Induced Large Volume Collapse, Plane-to-Chain, Insulator to Metal Transition in CaMn ₂ Bi ₂ Gui, Xin; Finkelstein, Gregory J.; Chen, Keyu Inorganic Chemistry, Vol. 58, Issue 14 https://doi.org/10.1021/acs.inorgchem.9b01362	journal	July 2019
The laser micro-machining system for diamond anvil cell experiments and general precision machining applications at the High Pressure Collaborative Access Team Hrubiak, Rostislav; Sinogeikin, Stanislav; Rod, Eric Review of Scientific Instruments, Vol. 86, Issue 7 https://doi.org/10.1063/1.4926889	journal	July 2015
High thermoelectric cooling performance of n-type Mg ₃ Bi ₂ -based materials Mao, Jun; Zhu, Hangtian; Ding, Zhiwei Science, Vol. 365, Issue 6452 https://doi.org/10.1126/science.aax7792	journal	July 2019
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
Making and Breaking Bonds in Superconducting SrAl _{4– x} Si _x (0 ≤ x ≤ 2) Zevalkink, Alex; Bobnar, Matej; Schwarz, Ulrich Chemistry of Materials, Vol. 29, Issue 3 https://doi.org/10.1021/acs.chemmater.6b04615	journal	January 2017
High-Pressure Synthesis and Superconductivity of the Laves Phase Compound Ca(Al,Si) ₂ Composed of Truncated Tetrahedral Cages Ca@(Al,Si) ₁₂ Tanaka, Masashi; Zhang, Shuai; Inumaru, Kei Inorganic Chemistry, Vol. 52, Issue 10 https://doi.org/10.1021/ic400395n	journal	April 2013
Improvement of Low‐Temperature zT in a Mg ₃ Sb ₂ –Mg ₃ Bi ₂ Solid Solution via Mg‐Vapor Annealing Wood, Maxwell; Kuo, Jimmy Jiahong; Imasato, Kazuki Advanced Materials, Vol. 31, Issue 35 https://doi.org/10.1002/adma.201902337	journal	July 2019
Chemical bonding origin of the unexpected isotropic physical properties in thermoelectric Mg3Sb2 and related materials Zhang, Jiawei; Song, Lirong; Sist, Mattia Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06980-x	journal	November 2018
An Unlikely Route to Low Lattice Thermal Conductivity: Small Atoms in a Simple Layered Structure Peng, Wanyue; Petretto, Guido; Rignanese, Gian-Marco Joule, Vol. 2, Issue 9 https://doi.org/10.1016/j.joule.2018.06.014	journal	September 2018
Chemical Flexibility of Mg in Pnictide Materials: Structure and Properties Diversity Wang, Jian; Mark, Justin; Woo, Katherine E. Chemistry of Materials, Vol. 31, Issue 20 https://doi.org/10.1021/acs.chemmater.9b03740	journal	September 2019
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
A tetragonal polymorph of SrMn ₂ P ₂ made under high pressure – theory and experiment in harmony Xie, Weiwei; Winiarski, Michał J.; Klimczuk, Tomasz Dalton Transactions, Vol. 46, Issue 21 https://doi.org/10.1039/C7DT00781G	journal	January 2017
OLEX : new software for visualization and analysis of extended crystal structures Dolomanov, Oleg V.; Blake, Alexander J.; Champness, Neil R. Journal of Applied Crystallography, Vol. 36, Issue 5 https://doi.org/10.1107/S0021889803015267	journal	September 2003
Discovery of high-performance low-cost n-type Mg3Sb2-based thermoelectric materials with multi-valley conduction bands Zhang, Jiawei; Song, Lirong; Pedersen, Steffen Hindborg Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms13901	journal	January 2017
Charting the complete elastic properties of inorganic crystalline compounds de Jong, Maarten; Chen, Wei; Angsten, Thomas Scientific Data, Vol. 2, Issue 1 https://doi.org/10.1038/sdata.2015.9	journal	March 2015
High-Pressure Synthesis, Characterization, and Tuning of Solid State Materials Badding, J. V. Annual Review of Materials Science, Vol. 28, Issue 1 https://doi.org/10.1146/annurev.matsci.28.1.631	journal	August 1998
Pressure dependence of room-temperature structural properties of CaAl ₂ Si ₂ Strikos, S.; Joseph, B.; Alabarse, F. G. Journal of Physics: Condensed Matter, Vol. 32, Issue 36 https://doi.org/10.1088/1361-648X/ab9268	journal	June 2020
EosFit7c and a Fortran module (library) for equation of state calculations Angel, Ross J.; Alvaro, Matteo; Gonzalez-Platas, Javier Zeitschrift für Kristallographie - Crystalline Materials, Vol. 229, Issue 5 https://doi.org/10.1515/zkri-2013-1711	journal	January 2014
VESTA : a three-dimensional visualization system for electronic and structural analysis Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 41, Issue 3 https://doi.org/10.1107/S0021889808012016	journal	May 2008
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
Isotropic Conduction Network and Defect Chemistry in Mg ₃₊ _δ Sb ₂ -Based Layered Zintl Compounds with High Thermoelectric Performance Tamaki, Hiromasa; Sato, Hiroki K.; Kanno, Tsutomu Advanced Materials, Vol. 28, Issue 46 https://doi.org/10.1002/adma.201603955	journal	September 2016
Neue intermetallische Verbindungen im anti-Ce2O2S-Strukturtyp. / New Intermetallic Compounds in the anti-Ce2O2S-Structure Type Cordier, Gerhard; Schäfer, Herbert Zeitschrift für Naturforschung B, Vol. 31, Issue 11 https://doi.org/10.1515/znb-1976-1105	journal	November 1976
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136406	journal	April 2008
High-pressure phases of III-V zinc-blende semiconductors Zhang, S. B.; Cohen, Marvin L. Physical Review B, Vol. 35, Issue 14 https://doi.org/10.1103/PhysRevB.35.7604	journal	May 1987
Crystal structure analysis using integrated X-ray powder diffraction software suite PDXL Schuck, Götz; Iwata, Akihiko; Sasaki, Akito Acta Crystallographica Section A Foundations of Crystallography, Vol. 66, Issue a1 https://doi.org/10.1107/S0108767310092871	journal	August 2010
Fragment formalism in main-group solids: applications to aluminum boride (AlB2), calcium aluminum silicide (CaAl2Si2), barium-aluminum (BaAl4), and related materials Burdett, Jeremy K.; Miller, Gordon J. Chemistry of Materials, Vol. 2, Issue 1 https://doi.org/10.1021/cm00007a004	journal	January 1990
DIOPTAS : a program for reduction of two-dimensional X-ray diffraction data and data exploration Prescher, Clemens; Prakapenka, Vitali B. High Pressure Research, Vol. 35, Issue 3 https://doi.org/10.1080/08957959.2015.1059835	journal	May 2015
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Defect Engineering for Realizing High Thermoelectric Performance in n-Type Mg ₃ Sb ₂ -Based Materials Mao, Jun; Wu, Yixuan; Song, Shaowei ACS Energy Letters, Vol. 2, Issue 10 https://doi.org/10.1021/acsenergylett.7b00742	journal	September 2017
Charting the complete elastic properties of inorganic crystalline compounds de Jong, Maarten; Chen, Wei; Angsten, Thomas Materials Data Facility https://doi.org/10.18126/9fg1-528u	dataset	January 2022
Synthesis and high thermoelectric efficiency of Zintl phase YbCd2−xZnxSb2 Wang, Xiao-Jun; Tang, Mei-Bo; Chen, Hao-Hong Applied Physics Letters, Vol. 94, Issue 9 https://doi.org/10.1063/1.3040321	journal	March 2009
Anisotropic compressibility and expansivity in layered GeSe2 Stølen, S.; Grzechnik, A.; Grande, T. Solid State Communications, Vol. 115, Issue 5 https://doi.org/10.1016/S0038-1098(00)00173-3	journal	June 2000
Insights into the design of thermoelectric Mg3Sb2 and its analogs by combining theory and experiment Zhang, Jiawei; Song, Lirong; Iversen, Bo Brummerstedt npj Computational Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41524-019-0215-y	journal	July 2019
Tuning the carrier scattering mechanism to effectively improve the thermoelectric properties Shuai, Jing; Mao, Jun; Song, Shaowei Energy & Environmental Science, Vol. 10, Issue 3 https://doi.org/10.1039/C7EE00098G	journal	January 2017
High Pressure Single Crystal Diffraction at PX^2 Zhang, Dongzhou; Dera, Przemyslaw K.; Eng, Peter J. Journal of Visualized Experiments, Issue 119 https://doi.org/10.3791/54660	journal	January 2017
Bindungsart und Gitterbau binärer Magnesiumverbindungen Zintl, E.; Husemann, E. Zeitschrift für Physikalische Chemie, Vol. 21B, Issue 1 https://doi.org/10.1515/zpch-1933-2112	journal	January 1933
Toward an international practical pressure scale: A proposal for an IPPS ruby gauge (IPPS-Ruby2020) Shen, Guoyin; Wang, Yanbin; Dewaele, Agnes High Pressure Research, Vol. 40, Issue 3 https://doi.org/10.1080/08957959.2020.1791107	journal	July 2020
Site preferences and bond length differences in CaAl2Si2-type Zintl compounds Zheng, Chong.; Hoffmann, Roald.; Nesper, Reinhard. Journal of the American Chemical Society, Vol. 108, Issue 8 https://doi.org/10.1021/ja00268a027	journal	April 1986
X-ray diffraction data for graphite to 20 GPa Zhao, You Xiang; Spain, Ian L. Physical Review B, Vol. 40, Issue 2 https://doi.org/10.1103/PhysRevB.40.993	journal	July 1989
Anisotropic Thermal Expansion and Compressibility of Black Phosphorus Riedner, R. J.; Srinivasa, S. R.; Cartz, L. THERMAL EXPANSION OF SOLIDS — 1973: International Symposium https://doi.org/10.1063/1.2945940	conference	January 1974

Similar Records

Soft anharmonic phonons and ultralow thermal conductivity in Mg ₃ (Sb, Bi) ₂ thermoelectrics

Journal Article · Fri May 21 00:00:00 EDT 2021 · Science Advances · OSTI ID:1765294

Ding, Jingxuan; Lanigan-Atkins, Tyson; Calderón-Cueva, Mario; +5 more

High-Pressure Study of Perovskites and Postperovskites in the (Mg,Fe)GeO₃ System

Journal Article · Mon Jun 26 00:00:00 EDT 2017 · Inorganic Chemistry · OSTI ID:1765294

Stan, Camelia V.; Dutta, Rajkrishna; Cava, Robert J.; +2 more

Pressure-induced ferroelectric to paraelectric transition in LiTaO₃ and (Li,Mg)TaO₃

Journal Article · Tue Feb 16 00:00:00 EST 2016 · Journal of Applied Physics · OSTI ID:1765294

Yamanaka, Takamitsu; Nakamoto, Yuki; Takei, Fumihiko; +3 more

Related Subjects

36 MATERIALS SCIENCE
Chemical structure
physical and chemical processes
granular materials
phase transitions
crystal structure

Title: Anisotropic Structural Collapse of Mg3Sb2 and Mg3Bi2 at High Pressure

Citation Formats

References (41)

Similar Records

Related Subjects

Title: Anisotropic Structural Collapse of Mg₃Sb₂ and Mg₃Bi₂ at High Pressure