Machine Learning-Guided Discovery of Ternary Compounds Containing La, P, and Group 14 Elements

Sun, Huaijun; Zhang, Chao; Xia, Weiyi; Tang, Ling; Wang, Renhai; Akopov, Georgiy; Hewage, Nethmi W.; Ho, Kai-Ming; Kovnir, Kirill; Wang, Cai-Zhuang

doi:10.1021/acs.inorgchem.2c02431

Machine Learning-Guided Discovery of Ternary Compounds Containing La, P, and Group 14 Elements

Journal Article · Tue Oct 11 00:00:00 EDT 2022 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.2c02431· OSTI ID:1923474

Sun, Huaijun ^[1]; ^[2]; Xia, Weiyi ^[3]; Tang, Ling ^[4]; Wang, Renhai ^[5]; ^[3]; ^[3]; Ho, Kai-Ming ^[3]; Kovnir, Kirill ^[3]; ^[3]

Jiyang College of Zhejiang Agriculture and Forestry University, Zhuji (China); Ames Lab., Ames, IA (United States)
Yantai University (China)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Zhejiang Univ. of Technology, Hangzhou (China); Ames Lab., Ames, IA (United States)
Guangdong University of Technology, Guangzhou (China)

In this work, we integrate a deep machine learning (ML) method with first-principles calculations to efficiently search for the energetically favorable ternary compounds. Using La–Si–P as a prototype system, we demonstrate that ML-guided first-principles calculations can efficiently explore crystal structures and their relative energetic stabilities, thus greatly accelerate the pace of material discovery. A number of new La–Si–P ternary compounds with formation energies less than 30 meV/atom above the known ternary convex hull are discovered. Among them, the formation energies of La₅SiP₃ and La₂SiP phases are only 2 and 10 meV/atom, respectively, above the convex hull. These two compounds are dynamically stable with no imaginary phonon modes. Moreover, by replacing Si with heavier-group 14 elements in the eight lowest-energy La–Si–P structures from our ML-guided predictions, a number of low-energy La–X–P phases (X = Ge, Sn, Pb) are predicted.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Laboratory Directed Research and Development (LDRD) Program; National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1923474

Report Number(s):: IS-J-10,915

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 42 Vol. 61; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (36)

Noncentrosymmetric Tetrel Pnictides RuSi ₄ P ₄ and IrSi ₃ P ₃ : Nonlinear Optical Materials with Outstanding Laser Damage Threshold Lee, Shannon; Carnahan, Scott L.; Akopov, Georgiy Advanced Functional Materials, Vol. 31, Issue 16 https://doi.org/10.1002/adfm.202010293	journal	February 2021
Few-Layer GeAs Field-Effect Transistors and Infrared Photodetectors Guo, Jian; Liu, Yuan; Ma, Yue Advanced Materials, Vol. 30, Issue 21 https://doi.org/10.1002/adma.201705934	journal	April 2018
LaSiP ₃ and LaSi ₂ P ₆ : Two Excellent Rare‐Earth Pnictides with Strong SHG Responses as Mid‐ and Far‐Infrared Nonlinear Optical Crystals Sun, Yingshuang; Chen, Jindong; Yang, Shunda Advanced Optical Materials, Vol. 9, Issue 10 https://doi.org/10.1002/adom.202002176	journal	March 2021
Add a Pinch of Tetrel: The Transformation of a Centrosymmetric Metal into a Nonsymmorphic and Chiral Semiconductor Lee, Shannon J.; Viswanathan, Gayatri; Carnahan, Scott L. Chemistry – A European Journal, Vol. 28, Issue 9 https://doi.org/10.1002/chem.202104319	journal	January 2022
Synthesis, Crystal and Electronic Structure of La ₂ SiP ₄ Akopov, Georgiy; Viswanathan, Gayatri; Kovnir, Kirill Zeitschrift für anorganische und allgemeine Chemie, Vol. 647, Issue 2-3 https://doi.org/10.1002/zaac.202000378	journal	January 2021
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
The Rare Earth Silicon PhosphidesLnSi2P6(Ln= La, Ce, Pr, and Nd) Kaiser, Peter; Jeitschko, Wolfgang Journal of Solid State Chemistry, Vol. 124, Issue 2 https://doi.org/10.1006/jssc.1996.0248	journal	July 1996
Non-Centrosymmetric Superconductors: Introduction and Overview Bauer, Ernst; Sigrist, Manfred Lecture Notes in Physics https://doi.org/10.1007/978-3-642-24624-1	book	January 2012
CALYPSO: A method for crystal structure prediction Wang, Yanchao; Lv, Jian; Zhu, Li Computer Physics Communications, Vol. 183, Issue 10 https://doi.org/10.1016/j.cpc.2012.05.008	journal	October 2012
New developments in evolutionary structure prediction algorithm USPEX Lyakhov, Andriy O.; Oganov, Artem R.; Stokes, Harold T. Computer Physics Communications, Vol. 184, Issue 4 https://doi.org/10.1016/j.cpc.2012.12.009	journal	April 2013
GeP and (Ge1−Sn )(P1−Ge ) (x≈0.12, y≈0.05): Synthesis, structure, and properties of two-dimensional layered tetrel phosphides Lee, Kathleen; Synnestvedt, Sarah; Bellard, Maverick Journal of Solid State Chemistry, Vol. 224 https://doi.org/10.1016/j.jssc.2014.04.021	journal	April 2015
Aliovalent substitutions of the 2D layered semiconductor GeAs Lee, Shannon; Owens-Baird, Bryan; Kovnir, Kirill Journal of Solid State Chemistry, Vol. 276 https://doi.org/10.1016/j.jssc.2019.05.016	journal	August 2019
Superconductivity in non-centrosymmetric materials Kneidinger, F.; Bauer, E.; Zeiringer, I. Physica C: Superconductivity and its Applications, Vol. 514 https://doi.org/10.1016/j.physc.2015.02.016	journal	July 2015
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
Predictive Synthesis Kovnir, Kirill Chemistry of Materials, Vol. 33, Issue 13 https://doi.org/10.1021/acs.chemmater.1c01484	journal	July 2021
GeAs: Highly Anisotropic van der Waals Thermoelectric Material Lee, Kathleen; Kamali, Saeed; Ericsson, Tore Chemistry of Materials, Vol. 28, Issue 8 https://doi.org/10.1021/acs.chemmater.6b00567	journal	April 2016
Synthesis, Crystal Growth, and Transport Properties of van der Waals Tetrel Pnictide GeAs ₂ Mark, Justin; McBride, Brennan C.; Lee, Shannon ACS Applied Energy Materials, Vol. 3, Issue 5 https://doi.org/10.1021/acsaem.0c00565	journal	April 2020
Interface Structure Prediction from First-Principles Zhao, Xin; Shu, Qiang; Nguyen, Manh Cuong The Journal of Physical Chemistry C, Vol. 118, Issue 18 https://doi.org/10.1021/jp5010852	journal	April 2014
Third time's the charm: intricate non-centrosymmetric polymorphism in Ln SiP ₃ ( Ln = La and Ce) induced by distortions of phosphorus square layers Akopov, Georgiy; Mark, Justin; Viswanathan, Gayatri Dalton Transactions, Vol. 50, Issue 19 https://doi.org/10.1039/D1DT00845E	journal	January 2021
Synthesis and characterization of a new family of layered Pb _x Sn _4−x As ₃ alloys Koster, Karl G.; Wang, Yaxian; Scudder, Michael R. Journal of Materials Chemistry C, Vol. 9, Issue 20 https://doi.org/10.1039/D1TC00842K	journal	January 2021
Semiconducting silicon–phosphorus frameworks for caging exotic polycations Yox, Philip; Porter, Andrew P.; Dorn, Rick W. Chemical Communications, Vol. 58, Issue 55 https://doi.org/10.1039/D2CC02304K	journal	January 2022
A unified formulation of the constant temperature molecular dynamics methods Nosé, Shuichi The Journal of Chemical Physics, Vol. 81, Issue 1 https://doi.org/10.1063/1.447334	journal	July 1984
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
Evolutionary crystal structure prediction as a tool in materials design Oganov, Artem R.; Glass, Colin W. Journal of Physics: Condensed Matter, Vol. 20, Issue 6 https://doi.org/10.1088/0953-8984/20/6/064210	journal	January 2008
An adaptive genetic algorithm for crystal structure prediction Wu, S. Q.; Ji, M.; Wang, C. Z. Journal of Physics: Condensed Matter, Vol. 26, Issue 3 https://doi.org/10.1088/0953-8984/26/3/035402	journal	December 2013
Superconductivity and spin–orbit coupling in non-centrosymmetric materials: a review Smidman, M.; Salamon, M. B.; Yuan, H. Q. Reports on Progress in Physics, Vol. 80, Issue 3 https://doi.org/10.1088/1361-6633/80/3/036501	journal	January 2017
Canonical dynamics: Equilibrium phase-space distributions Hoover, William G. Physical Review A, Vol. 31, Issue 3 https://doi.org/10.1103/PhysRevA.31.1695	journal	March 1985
Crystal structure prediction via particle-swarm optimization Wang, Yanchao; Lv, Jian; Zhu, Li Physical Review B, Vol. 82, Issue 9 https://doi.org/10.1103/PhysRevB.82.094116	journal	September 2010
Identification of post-pyrite phase transitions in SiO 2 by a genetic algorithm Wu, Shunqing; Umemoto, Koichiro; Ji, Min Physical Review B, Vol. 83, Issue 18 https://doi.org/10.1103/PhysRevB.83.184102	journal	May 2011
Ultrahigh-pressure phases of H 2 O ice predicted using an adaptive genetic algorithm Ji, Min; Umemoto, Koichiro; Wang, Cai-Zhuang Physical Review B, Vol. 84, Issue 22 https://doi.org/10.1103/PhysRevB.84.220105	journal	December 2011
Exploring the Structural Complexity of Intermetallic Compounds by an Adaptive Genetic Algorithm Zhao, X.; Nguyen, M. C.; Zhang, W. Y. Physical Review Letters, Vol. 112, Issue 4 https://doi.org/10.1103/PhysRevLett.112.045502	journal	January 2014
Crystal Graph Convolutional Neural Networks for an Accurate and Interpretable Prediction of Material Properties Xie, Tian; Grossman, Jeffrey C. Physical Review Letters, Vol. 120, Issue 14 https://doi.org/10.1103/PhysRevLett.120.145301	journal	April 2018
The Cambridge Structural Database Groom, Colin R.; Bruno, Ian J.; Lightfoot, Matthew P. Acta Crystallographica Section B Structural Science, Crystal Engineering and Materials, Vol. 72, Issue 2, p. 171-179 https://doi.org/10.1107/S2052520616003954	journal	April 2016
TaRh ₂ B ₂ and NbRh ₂ B ₂ : Superconductors with a chiral noncentrosymmetric crystal structure Carnicom, Elizabeth M.; Xie, Weiwei; Klimczuk, Tomasz Science Advances, Vol. 4, Issue 5 https://doi.org/10.1126/sciadv.aar7969	journal	May 2018
The Crystal Structures of SiP2, SiAs2, and GeP. Wadsten, Tommy; Vikan, M.; Krohn, C. Acta Chemica Scandinavica, Vol. 21 https://doi.org/10.3891/acta.chem.scand.21-0593	journal	January 1967
Synthesis of a Pyrite-Type Modification of SiP2. Wadsten, Tommy; Jerslev, Bodil; Cyvin, S. J. Acta Chemica Scandinavica, Vol. 21 https://doi.org/10.3891/acta.chem.scand.21-1374	journal	January 1967

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Machine Learning-Guided Discovery of Ternary Compounds Containing La, P, and Group 14 Elements

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