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Title: Sorting Stable versus Unstable Hypothetical Compounds: The Case of Multi-Functional ABX Half-Heusler Filled Tetrahedral Structures

Abstract

Electronic structure theory has recently been used to propose hypothetical compounds in presumed crystal structures, seeking new useful functional materials. In some cases, such hypothetical materials are metastable, albeit with technologically useful long lifetimes. Yet, in other cases, suggested hypothetical compounds may be significantly higher in energy than their lowest-energy crystal structures or competing phases, making their synthesis and eventual device-stability questionable. By way of example, the focus here is on the family of 1:1:1 compounds ABX called 'filled tetrahedral structure' (sometimes called Half-Heusler) in the four groups with octet electron count: I-I-VI (e.g., CuAgSe), I-II-V (e.g., AgMgAs), I-III-IV (e.g., LiAlSi), and II-II-IV (e.g., CaZnSn). First-principles thermodynamics is used to sort the lowest-energy structure and the thermodynamic stability of the 488 unreported hypothetical ABX compounds, many of which were previously proposed to be useful technologically. It is found that as many as 235 of the 488 are unstable with respect to decomposition (hence, are unlikely to be viable technologically), whereas other 235 of the unreported compounds are predicted to be thermodynamically stable (hence, potentially interesting new materials). 18 additional materials are too close to determine. The electronic structures of these predicted stable compounds are evaluated, seeking potential new material functionalities.

Authors:
; ; ;
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science, Basic Energy Sciences, Energy Frontier Research Centers and National Energy Research Scientific Computing Center; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1043741
Report Number(s):
NREL/JA-5900-54159
Journal ID: ISSN 1616-301X; TRN: US201213%%428
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 22; Journal Issue: 7; Journal ID: ISSN 1616-301X
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; CRYSTAL STRUCTURE; ELECTRONIC STRUCTURE; ELECTRONS; FORECASTING; FUNCTIONALS; SORTING; STABILITY; SYNTHESIS; THERMODYNAMICS; hypothetical compounds; filled tetrahedral structure; Half-Heusler

Citation Formats

Zhang, Xiuwen, Yu, Liping, Zakutayev, Andriy, and Zunger, Alex. Sorting Stable versus Unstable Hypothetical Compounds: The Case of Multi-Functional ABX Half-Heusler Filled Tetrahedral Structures. United States: N. p., 2012. Web. doi:10.1002/adfm.201102546.
Zhang, Xiuwen, Yu, Liping, Zakutayev, Andriy, & Zunger, Alex. Sorting Stable versus Unstable Hypothetical Compounds: The Case of Multi-Functional ABX Half-Heusler Filled Tetrahedral Structures. United States. https://doi.org/10.1002/adfm.201102546
Zhang, Xiuwen, Yu, Liping, Zakutayev, Andriy, and Zunger, Alex. Tue . "Sorting Stable versus Unstable Hypothetical Compounds: The Case of Multi-Functional ABX Half-Heusler Filled Tetrahedral Structures". United States. https://doi.org/10.1002/adfm.201102546.
@article{osti_1043741,
title = {Sorting Stable versus Unstable Hypothetical Compounds: The Case of Multi-Functional ABX Half-Heusler Filled Tetrahedral Structures},
author = {Zhang, Xiuwen and Yu, Liping and Zakutayev, Andriy and Zunger, Alex},
abstractNote = {Electronic structure theory has recently been used to propose hypothetical compounds in presumed crystal structures, seeking new useful functional materials. In some cases, such hypothetical materials are metastable, albeit with technologically useful long lifetimes. Yet, in other cases, suggested hypothetical compounds may be significantly higher in energy than their lowest-energy crystal structures or competing phases, making their synthesis and eventual device-stability questionable. By way of example, the focus here is on the family of 1:1:1 compounds ABX called 'filled tetrahedral structure' (sometimes called Half-Heusler) in the four groups with octet electron count: I-I-VI (e.g., CuAgSe), I-II-V (e.g., AgMgAs), I-III-IV (e.g., LiAlSi), and II-II-IV (e.g., CaZnSn). First-principles thermodynamics is used to sort the lowest-energy structure and the thermodynamic stability of the 488 unreported hypothetical ABX compounds, many of which were previously proposed to be useful technologically. It is found that as many as 235 of the 488 are unstable with respect to decomposition (hence, are unlikely to be viable technologically), whereas other 235 of the unreported compounds are predicted to be thermodynamically stable (hence, potentially interesting new materials). 18 additional materials are too close to determine. The electronic structures of these predicted stable compounds are evaluated, seeking potential new material functionalities.},
doi = {10.1002/adfm.201102546},
url = {https://www.osti.gov/biblio/1043741}, journal = {Advanced Functional Materials},
issn = {1616-301X},
number = 7,
volume = 22,
place = {United States},
year = {2012},
month = {4}
}

Works referenced in this record:

Prediction of New Low Compressibility Solids
journal, August 1989


Low-Compressibility Carbon Nitrides
journal, January 1996


Elastic and structural instability of cubic Sn 3 N 4 and C 3 N 4 under pressure
journal, October 2010


Structural and electronic properties of Co / Al 2 O 3 / Co magnetic tunnel junction from first principles
journal, August 2000


Room-Temperature Ferromagnetism in Carbon-Doped ZnO
journal, September 2007


Li3SbO4: A new high rate anode material for lithium-ion batteries
journal, April 2011


Topological Insulators in Ternary Compounds with a Honeycomb Lattice
journal, April 2011


New optical transitions in strained Si-Ge superlattices
journal, September 1987


I-II-V half-Heusler compounds for optoelectronics: Ab initio calculations
journal, February 2010


Ordering in semiconductor alloys
journal, February 1990


Stability of coherently strained semiconductor superlattices
journal, January 1990


Synthesis and Structure of Na3N
journal, May 2002


Cluster-Doping Approach for Wide-Gap Semiconductors: The Case of p -Type ZnO
journal, June 2003


Half-Metallic Ferromagnetism and Structural Stability of Zincblende Phases of the Transition-Metal Chalcogenides
journal, July 2003


Synthesis and characterization of a binary noble metal nitride
journal, April 2004


Instability of the high-pressure CsCl structure in most III-V semiconductors
journal, September 1999


New developments in the Inorganic Crystal Structure Database (ICSD): accessibility in support of materials research and design
journal, May 2002


Finding Nature’s Missing Ternary Oxide Compounds Using Machine Learning and Density Functional Theory
journal, June 2010


Electronic excitations: density-functional versus many-body Green’s-function approaches
journal, June 2002


Farm Adjustments to Meet War Impacts1
journal, January 1941


Die Kristallstrukturen LiMgN, LiZnN, Li3AlN2 und Li3GaN2 1
journal, January 1946


Die ternären Nitride LiMgN und LiZnN. 16. Mitteilung über Metallamide und Metallnitride
journal, August 1948


Die Verbindungen LiMgP, LiZnP und LiZnAs
journal, January 1950


Electronic structure of filled tetrahedral semiconductors
journal, February 1985


Evaluation of Half-Heusler Compounds as Thermoelectric Materials Based on the Calculated Electrical Transport Properties
journal, October 2008


Evidence for temperature dependent moments ordering in ferromagnetic NiMnSb(100)
journal, July 2001


Effect of Ti substitution on the thermoelectric properties of (Zr,Hf)NiSn half-Heusler compounds
journal, February 2005


Structure and properties of CoMnSb in the context of half-metallic ferromagnetism
journal, October 2006


Preparation and characterization of some A I B II C V type semiconductors
journal, April 1988


Growth and band gap of the filled tetrahedral semiconductor LiMgN
journal, April 2002


Electrical transport properties and crystal structure of LiZnAs
journal, September 1987


Optical band gap of the filled tetrahedral semiconductor LiZnP
journal, April 1988


Optical band gap of the filled tetrahedral semiconductor LiZnAs
journal, April 1994


Raman scattering from the filled tetrahedral semiconductor LiZnAs
journal, December 2005


Tunable multifunctional topological insulators in ternary Heusler compounds
journal, May 2010


Global space-group optimization problem: Finding the stablest crystal structure without constraints
journal, March 2007


Predicting stable stoichiometries of compounds via evolutionary global space-group optimization
journal, September 2009


Possible pitfalls in theoretical determination of ground-state crystal structures: The case of platinum nitride
journal, March 2009


Long-range order instead of phase separation in large lattice-mismatch isovalent AX BX systems
journal, December 2009


Structure prediction and targeted synthesis: A new NanN2 diazenide crystalline structure
journal, November 2010


Molecular Geometry Optimization with a Genetic Algorithm
journal, July 1995


Crystal structure prediction using ab initio evolutionary techniques: Principles and applications
journal, June 2006


Ionic high-pressure form of elemental boron
journal, January 2009


Transparent dense sodium
journal, March 2009


A self-interaction corrected approach to many-electron systems: Beyond the local spin density approximation
journal, June 1980


Generalized Gradient Approximation Made Simple
journal, October 1996


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998


Crystal structure prediction from first principles
journal, December 2008


Semiconductor thermochemistry in density functional calculations
journal, December 2008


Preparation and properties of radio-frequency-sputtered half-Heusler films for use in solar cells
journal, January 2011


KAuTe, Synthese und struktur des ersten alkalimetallgoldtellurids
journal, April 1990


Magnetic susceptibility and 119Sn Mössbauer spectroscopy studies of RAuSn compounds (R=La, Ce, Pr)
journal, January 2001


Valence band studies of the RTX (R=Pr,Nd; T=Cu,Ag,Au; X=Ge,Sn) compounds
journal, December 2000


Phasenbeziehungen im System LiGa?Sn und die Kristallstrukturen der intermedi�ren Phasen LiGaSn und Li2Ga2Sn
journal, July 1993


Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961