This book compiles selected publications authored or co-authored by the editor to present a comprehensive understanding of following topics: (1) density functional theory and CALPHAD modeling; (2) computational tools; and (3) applications of computational thermodynamics. It is noted that while entropy at one scale is well represented by standard statistical mechanics in terms of probability of individual configurations at that scale, the theory capable of counting total entropy of a system from different scales is lacking. The zentropy theory provides a nested form for configurational entropy enabling multiscale modeling to account for disorder and fluctuations from the electronic scale based on quantum mechanics to the experimental scale based on statistical mechanics using free energies of individual configurations rather than their total energies in standard statistical mechanics. The predictions from the zentropy theory demonstrate remarkable agreements with experimental observations for magnetic transitions and associated emergent behaviors of strongly correlated metals and oxides, including singularity and instability at critical points and positive and negative thermal expansions, without the need of additional truncated models and fitting model parameters beyond density function theory. This paves the way to provide the predicted phase equilibrium data for high throughput predictive CALPHAD modeling of complex material systems, and those individual configurations may thus be considered as the genomic building blocks of individual phases in the spirit of Materials Genome®.
Part I Density Functional Theory and CALPHAD Modeling
1. First-Principles Calculations and CALPHAD Modeling of Thermodynamics
Zi-Kui Liu
2. Thermodynamics of the Cr-Ta-W System by Combining the Ab Initio and CALPHAD Methods
Larry Kaufman, P. E. A. Turchi, Weiming Huang, and Zi-Kui Liu
3. Ab initio Lattice Stability in Comparison with CALPHAD Lattice Stability
Y. Wang, S. Curtarolo, C. Jiang, R. Arroyave, T. Wang, G. Ceder, L.-Q. Chen, and Zi-Kui Liu
4. Thermodynamic Properties of Al, Ni, NiAl, and Ni3Al from First-Principles Calculations
Y. Wang, Zi-Kui Liu, and L.-Q. Chen
5. First-Principles Study of Binary bcc Alloys Using Special Quasirandom Structures
Chao Jiang, C. Wolverton, Jorge Sofo, Long-Qing Chen, and Zi-Kui Liu
6. An Integrated Framework for Multiscale Materials Simulation and Design
Zi-Kui Liu, L.-Q. Chen, P. Raghavan, Q. Du, J. O. Sofo, S. A. Langer, and C. Wolverton
7. First-Principles Calculation of Self-Diffusion Coefficients
M. Mantina, Y. Wang, R. Arroyave, L. Q. Chen, Zi-Kui Liu, and C. Wolverton
8. Ocean of Data: Integrating First-Principles Calculations and CALPHAD Modeling with Machine Learning
Zi-Kui Liu
9. First-Principles Thermodynamic Theory of Seebeck Coefficients
Yi Wang, Yong-Jie Hu, Brandon Bocklund, Shun-Li Shang, Bi-Cheng Zhou, Zi-Kui Liu, and Long-Qing Chen
10. An Alternative Approach to Predict Seebeck Coefficients: Application to La3–xTe4
Yi Wang, Xiaoyu Chong, Yong-Jie Hu, Shun-Li Shang, Fivos R. Drymiotis, Samad A. Firdosy, Kurt E. Star, Jean-Pierre Fleurial, Vilupanur A. Ravi, Long-Qing Chen, and Zi-Kui Liu
11. Quantifying the Degree of Disorder and Associated Phenomena in Materials through Zentropy: Illustrated with Invar Fe3Pt
Shun-Li Shang, Yi Wang, and Zi-Kui Liu
12. Parameter-Free Prediction of Phase Transition in PbTiO3 through Combination of Quantum Mechanics and Statistical Mechanics
Zi-Kui Liu, Shun-Li Shang, Jinglian Du, and Yi Wang
13. Genomic Materials Design: CALculation of PHAse Dynamics
G. B. Olson and Zi-Kui Liu
Part II Computational Tools
14. Efficient Stochastic Generation of Special Quasirandom Structures
A. van de Walle, P. Tiwary, M. de Jong, D.L. Olmsted, M. Asta, A. Dick, D. Shin, Y. Wang, L.-Q. Chen, and Zi-Kui Liu
15. YPHON: A Package for Calculating Phonons of Polar Materials
Yi Wang, Long-Qing Chen, and Zi-Kui Liu
16. pycalphad: CALPHAD-Based Computational Thermodynamics in Python
Richard Otis and Zi-Kui Liu
17. ESPEI for Efficient Thermodynamic Database Development, Modification, and Uncertainty Quantification: Application to Cu–Mg
Brandon Bocklund, Richard Otis, Aleksei Egorov, Abdulmonem Obaied, Irina Roslyakova, and Zi-Kui Liu
18. Quantified Uncertainty in Thermodynamic Modeling for Materials Design
Noah H. Paulson, Brandon J. Bocklund, Richard A. Otis, Zi-Kui Liu, and Marius Stan
19. DFTTK: Density Functional Theory ToolKit for High-throughput Lattice Dynamics Calculations
Yi Wang, Mingqing Liao, Brandon J. Bocklund, Peng Gao, Shun-Li Shang, Hojong Kim, Allison M. Beese, Long-Qing Chen, and Zi-Kui Liu
20. Extensible Structure-Informed Prediction of Formation Energy with Improved Accuracy and Usability Employing Neural Networks
Adam M. Krajewski, Jonathan W. Siegel, Jinchao Xu, and Zi-Kui Liu
21. Predictive Crystal Plasticity Modeling of Single Crystal Nickel Based on First-Principles Calculations
John D. Shimanek, Shipin Qin, Shun-Li Shang, Zi-Kui Liu, and Allison M. Beese
22. Density Functional Theory-Informed Dislocation Density Hardening within Crystal Plasticity: Application to Modeling Deformation of Ni Polycrystals
Adnan Eghtesad, John D. Shimanek, Shun-Li Shang, Ricardo Lebensohn, Marko Knezevic, Zi-Kui Liu, and Allison M. Beese
Part III Applications of Computational Thermodynamics
23. Application of the Le Chatelier Principle on Gas Reactions
Zi-Kui Liu, John Ågren, and Mats Hillert
24. Morphology of Cementite Decomposition in an Fe-Cr-C Alloy
Zi-Kui Liu and John Ågren
25. The Development of Phase-Based Property Data Using the CALPHAD Method and Infrastructure Needs
Carelyn E. Campbell, Ursula R. Kattner, and Zi-Kui Liu
26. Developing Gradient Metal Alloys through Radial Deposition Additive Manufacturing
Douglas C. Hofmann, Scott Roberts, Richard Otis, Joanna Kolodziejska, R. Peter Dillon, Jong-ook Suh, Andrew A. Shapiro, Zi-Kui Liu, and John-Paul Borgonia
27. The Penn State-Georgia Tech CCMD: Ushering in the ICME Era
Zi-Kui Liu and David L. McDowell
28. Synthesis Science of SrRuO3 and CaRuO3 Epitaxial Films with High Residual Resistivity Ratios
Hari P. Nair, Yang Liu, Jacob P. Ruf, Nathaniel J. Schreiber, Shun-Li Shang, David J. Baek, Berit H. Goodge, Lena F. Kourkoutis, Zi-Kui Liu, Kyle M. Shen, and Darrell G. Schlom
29. Suitability of Binary Oxides for Molecular-Beam Epitaxy Source Materials: A Comprehensive Thermodynamic Analysis
Kate M. Adkison, Shun-Li Shang, Brandon J. Bocklund, Detlef Klimm, Darrell G. Schlom, and Zi-Kui Liu
30. Adsorption-Controlled Growth of Ga2O3 by Suboxide Molecular-Beam Epitaxy
Patrick Vogt, Felix V. E. Hensling, Kathy Azizie, Celesta S. Chang, David Turner, Jisung Park, Jonathan P. McCandless, Hanjong Paik, Brandon J. Bocklund, Georg Hoffman, Oliver Bierwagen, Debdeep Jena, Huili G. Xing, Shin Mou, David A. Muller, Shun-Li Shang, Zi-Kui Liu, and Darrell G. Schlom
Biography
Zi-Kui Liu is the Dorothy Pate Enright Professor in the Department of Materials Science and Engineering at the Pennsylvania State University, USA. He obtained his BS from Central South University, China, MS from the University of Science and Technology Beijing, China, and PhD from KTH Royal Institute of Technology, Sweden. He was a research associate at the University of Wisconsin-Madison and a senior research scientist at QuesTek Innovations LLC. He has been at the Pennsylvania State University since 1999, the editor-in-chief of CALPHAD journal since 2001, and the president of CALPHAD Inc. since 2013. Dr Liu coined the term "Materials Genome®" in 2002. He is a fellow of TMS and ASM International and has served as the president of ASM International and a member of the ASM International Board of Trustees and the TMS Board of Directors. He has graduated 32 PhD students and published over 650 papers.
