Challenges and Opportunities in Modeling Oxides for Energy and Information Devices

  • Bilge YildizEmail author
  • Cesare Franchini
  • Jing Yang
Living reference work entry


The growth of computational resources has enabled investigations of large-scale and highly correlated problems by using first principles computational techniques such as density functional theory (DFT). In context of oxide materials, these problems include oxide surface reconstructions (Diebold et al. 2010), diffusion and reaction barriers in heterogeneous systems (Chizallet and Raybaud 2014; Aksyonov et al. 2018), phase diagrams for transition metal oxides (Park et al. 2014; Leonov 2015), and point defects as well as extended defects (Youssef and Yildiz 2012; Sun et al. 2015). These developments have opened up new opportunities for predicting not only the bulk crystal properties of oxides, but also the effect of complex microstructures such as associated point defects (Hu et al. 2013; Liu et al. 2012; Zhang et al. 2014; T-Thienprasert et al. 2012), grain boundaries (Polfus et al. 2012; McKenna and Shluger 2009; Hojo et al. 2010), dislocations (Sun et al. 2015; Hojo et al. 2011; McKenna 2013), and surfaces (Lee and Morgan 2015; Freysoldt and Neugebauer 2018; Bajdich et al. 2015) under thermodynamic drivers. These developments can ultimately allow for ab initio prediction of realistic device performance. Yet, challenges remain on both the theoretical and algorithmic level to accurately predict oxide materials properties on a complex potential energy surface. Here we summarize several growing fields in addressing these challenges and present our perspectives on future directions that these methods will enable.


  1. Abe R et al (2013) Visible-light-induced water splitting based on two-step photoexcitation between dye-sensitized layered niobate and tungsten oxide photocatalysts in the presence of a triiodide/iodide shuttle redox mediator. J Am Chem Soc 135(45):16872–16884Google Scholar
  2. Aksyonov DA et al (2018) Understanding migration barriers for monovalent ion insertion in transition metal oxide and phosphate based cathode materials: a DFT study. Comput Mater Sci 154:449–458Google Scholar
  3. Anisimov VI, Zaanen J, Andersen OK (1991) Band theory and Mott insulators: Hubbard U instead of Stoner I. Phys Rev B 44(3):943–954ADSGoogle Scholar
  4. Bajdich M, Nørskov JK, Vojvodic A (2015) Surface energetics of alkaline-earth metal oxides: trends in stability and adsorption of small molecules. Phys Rev B 91(15):155401ADSGoogle Scholar
  5. Bechstedt F (2018) Correlation beyond the random phase approximation: a consistent many-body perturbation theory approach. Phys Rev B 97(24):241109ADSGoogle Scholar
  6. Becke AD (2014) Perspective: fifty years of density-functional theory in chemical physics. J Chem Phys 140(18):18A301Google Scholar
  7. Cao A, Lu R, Veser G (2010) Stabilizing metal nanoparticles for heterogeneous catalysis. Phys Chem Chem Phys 12(41):13499–13510Google Scholar
  8. Chevrier VL et al (2010) Hybrid density functional calculations of redox potentials and formation energies of transition metal compounds. Phys Rev B 82(7):075122ADSGoogle Scholar
  9. Chibani W et al (2016) Self-consistent Green’s function embedding for advanced electronic structure methods based on a dynamical mean-field concept. Phys Rev B 93(16):165106ADSGoogle Scholar
  10. Chizallet C, Raybaud P (2014) Density functional theory simulations of complex catalytic materials in reactive environments: beyond the ideal surface at low coverage. Catal Sci Technol 4(9):2797–2813Google Scholar
  11. Chizallet C et al (2008) Assignment of photoluminescence spectra of MgO powders: TD-DFT cluster calculations combined to experiments. Part I: structure effects on dehydroxylated surfaces. J Phys Chem C 112(42):16629–16637Google Scholar
  12. Chua ALS et al (2010) A genetic algorithm for predicting the structures of interfaces in multicomponent systems. Nat Mater 9:418ADSGoogle Scholar
  13. Chu et al (2019) Battery electrodes, electrolytes, and their interfaces. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  14. Demkov et al (2019) First-principles modeling of interface effects in oxides. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  15. Diebold U, Li S-C, Schmid M (2010) Oxide surface science. Annu Rev Phys Chem 61(1):129–148Google Scholar
  16. Duff AI et al (2015) Improved method of calculating ab initio high-temperature thermodynamic properties with application to ZrC. Phys Rev B 91(21):214311ADSGoogle Scholar
  17. Ergönenc Z et al (2018) Converged GW quasiparticle energies for transition metal oxide perovskites. Phys Rev Mater 2(2):024601Google Scholar
  18. Fattori A et al (2010) Fast hole surface conduction observed for indoline sensitizer dyes immobilized at fluorine-doped tin oxide–TiO2 surfaces. J Phys Chem C 114(27):11822–11828Google Scholar
  19. Freysoldt C, Neugebauer J (2018) First-principles calculations for charged defects at surfaces, interfaces, and two-dimensional materials in the presence of electric fields. Phys Rev B 97(20):205425ADSGoogle Scholar
  20. Freysoldt C et al (2014) First-principles calculations for point defects in solids. Rev Mod Phys 86(1):253–305ADSGoogle Scholar
  21. Georges A et al (1996) Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions. Rev Mod Phys 68(1):13–125ADSMathSciNetGoogle Scholar
  22. Grabowski B et al (2009) Ab initio up to the melting point: anharmonicity and vacancies in aluminum. Phys Rev B 79(13):134106ADSGoogle Scholar
  23. Han D et al (2016) Phonon-enabled carrier transport of localized states at non-polar semiconductor surfaces: a first-principles-based prediction. J Phys Chem Lett 7(18):3548–3553Google Scholar
  24. Harmer MP (2011) The phase behavior of interfaces. Science 332(6026):182–183ADSGoogle Scholar
  25. Hautier G et al (2012) Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability. Phys Rev B 85(15):155208ADSGoogle Scholar
  26. He J, Franchini C (2017) Assessing the performance of self-consistent hybrid functional for band gap calculation in oxide semiconductors. J Phys Condens Matter 29(45):454004ADSGoogle Scholar
  27. Hedin L (1965) New method for calculating the one-particle Green’s function with application to the electron-gas problem. Phys Rev 139(3A):A796–A823ADSGoogle Scholar
  28. Heinemann M, Eifert B, Heiliger C (2013) Band structure and phase stability of the copper oxides Cu2O, CuO, and Cu4O3. Phys Rev B 87(11):115111Google Scholar
  29. Hess et al (2019) Solid oxide fuel cell materials and interfaces. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  30. Hojo H et al (2010) Atomic structure of a CeO2 grain boundary: the role of oxygen vacancies. Nano Lett 10(11):4668–4672ADSGoogle Scholar
  31. Hojo H et al (2011) Atomic structure and strain field of threading dislocations in CeO2 thin films on yttria-stabilized ZrO2. Appl Phys Lett 98(15):153104ADSGoogle Scholar
  32. Hu W et al (2013) Electron-pinned defect-dipoles for high-performance colossal permittivity materials. Nat Mater 12:821ADSGoogle Scholar
  33. Kirklin S et al (2015) The Open Quantum Materials Database (OQMD): assessing the accuracy of DFT formation energies. Npj Comput Mater 1:15010ADSGoogle Scholar
  34. Kleijn SEF et al (2014) Electrochemistry of nanoparticles. Angew Chem Int Ed 53(14):3558–3586Google Scholar
  35. Klimeš J, Michaelides A (2012) Perspective: advances and challenges in treating Van Der Waals dispersion forces in density functional theory. J Chem Phys 137(12):120901ADSGoogle Scholar
  36. Klimeš J, Kaltak M, Kresse G (2014) Predictive GW calculations using plane waves and pseudopotentials. Phys Rev B 90(7):075125Google Scholar
  37. Kozinsky et al (2019) Transport in frustrated and disordered solid electrolytes. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  38. Kulik HJ (2015) Perspective: treating electron over-delocalization with the DFT+U method. J Chem Phys 142(24):240901Google Scholar
  39. Kuttipillai PS et al (2016) Phosphorescent nanocluster light-emitting diodes. Adv Mater 28(2):320–326Google Scholar
  40. Labat F et al (2012) First-principles modeling of dye-sensitized solar cells: challenges and perspectives. Acc Chem Res 45(8):1268–1277Google Scholar
  41. Laurent AD, Jacquemin D (2013) TD-DFT benchmarks: a review. Int J Quantum Chem 113(17):2019–2039Google Scholar
  42. Leang SS, Zahariev F, Gordon MS (2012) Benchmarking the performance of time-dependent density functional methods. J Chem Phys 136(10):104101ADSGoogle Scholar
  43. Lechermann et al (2019) Oxide heterostructures from a realistic many-body perspective. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  44. Lee Y-L, Morgan D (2015) Ab initio defect energetics of perovskite (001) surfaces for solid oxide fuel cells: a comparative study of LaMnO3 versus SrTiO3 and LaAlO3. Phys Rev B 91(19):195430Google Scholar
  45. Lee JH, Rabe KM (2010) Epitaxial-strain-induced multiferroicity in SrMnO3 from first principles. Phys Rev Lett 104(20):207204Google Scholar
  46. Leonov I (2015) Metal-insulator transition and local-moment collapse in FeO under pressure. Phys Rev B 92(8):085142Google Scholar
  47. Li W et al (2013) Density functional theory and beyond for band-gap screening: performance for transition-metal oxides and dichalcogenides. J Chem Theory Comput 9(7):2950–2958Google Scholar
  48. Libisch F, Huang C, Carter EA (2014) Embedded correlated wavefunction schemes: theory and applications. Acc Chem Res 47(9):2768–2775Google Scholar
  49. Lin H, Truhlar DG (2006) QM/MM: what have we learned, where are we, and where do we go from here? Theor Chem Accounts 117(2):185Google Scholar
  50. Liu L et al (2012) p-Type conductivity in N-doped ZnO: the role of the NZn-VO complex. Phys Rev Lett 108(21):215501Google Scholar
  51. Lu et al (2019) Design of new multiferroic oxides. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  52. Lousada CM et al (2013) Reactivity of metal oxide clusters with hydrogen peroxide and water – a DFT study evaluating the performance of different exchange–correlation functionals. Phys Chem Chem Phys 15(15):5539–5552Google Scholar
  53. Makhal A et al (2010) Role of resonance energy transfer in light harvesting of zinc oxide-based dye-sensitized solar cells. J Phys Chem C 114(23):10390–10395Google Scholar
  54. Mankowsky R et al (2014) Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5. Nature 516:71ADSGoogle Scholar
  55. Mannhart J, Schlom DG (2010) Oxide interfaces – an opportunity for electronics. Science 327(5973):1607–1611ADSGoogle Scholar
  56. Mattsson AE (2002) In pursuit of the “divine” functional. Science 298(5594):759–760Google Scholar
  57. McKenna KP (2013) Electronic and chemical properties of a surface-terminated screw dislocation in MgO. J Am Chem Soc 135(50):18859–18865Google Scholar
  58. McKenna KP, Shluger AL (2009) First-principles calculations of defects near a grain boundary in MgO. Phys Rev B 79(22):224116Google Scholar
  59. Meyer J, Reuter K (2014) Modeling heat dissipation at the nanoscale: an embedding approach for chemical reaction dynamics on metal surfaces. Angew Chem Int Ed 53(18):4721–4724Google Scholar
  60. Nørskov JK et al (2011) Density functional theory in surface chemistry and catalysis. Proc Natl Acad Sci 108(3):937–943. Scholar
  61. Onida G, Reining L, Rubio A (2002) Electronic excitations: density-functional versus many-body Green’s-function approaches. Rev Mod Phys 74(2):601–659ADSGoogle Scholar
  62. Park H, Millis AJ, Marianetti CA (2014) Total energy calculations using DFT+DMFT: computing the pressure phase diagram of the rare earth nickelates. Phys Rev B 89(24):245133Google Scholar
  63. Pastore M, Fantacci S, De Angelis F (2013) Modeling excited states and alignment of energy levels in dye-sensitized solar cells: successes, failures, and challenges. J Phys Chem C 117(8):3685–3700Google Scholar
  64. Perdew JP, Schmidt K (2001) Jacob’s ladder of density functional approximations for the exchange-correlation energy. AIP Conf Proc 577(1):1–20Google Scholar
  65. Perdew JP et al (2005) Prescription for the design and selection of density functional approximations: more constraint satisfaction with fewer fits. J Chem Phys 123(6):062201ADSGoogle Scholar
  66. Petersilka M, Gossmann UJ, Gross EKU (1996) Excitation energies from time-dependent density-functional theory. Phys Rev Lett 76(8):1212–1215ADSGoogle Scholar
  67. Plasser F et al (2012) Electronically excited states and photodynamics: a continuing challenge. Theor Chem Accounts 131(1):1073Google Scholar
  68. Polfus JM et al (2012) Defect chemistry of a BaZrO3 Sigma 3 (111) grain boundary by first principles calculations and space-charge theory. Phys Chem Chem Phys 14(35):12339–12346Google Scholar
  69. Reining L et al (2002) Excitonic effects in solids described by time-dependent density-functional theory. Phys Rev Lett 88(6):066404Google Scholar
  70. Reticcioli M et al (2019) Small polarons in transition metal oxides. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  71. Pentcheva R, Pickett WE (2010) Electronic phenomena at complex oxide interfaces: insights from first principles. J Phys Condens Matter 22(4):043001ADSGoogle Scholar
  72. Runge E, Gross EKU (1984) Density-functional theory for time-dependent systems. Phys Rev Lett 52(12):997–1000ADSGoogle Scholar
  73. Sadasivam S et al (2017) Thermal transport across metal silicide–silicon interfaces: first-principles calculations and Green’s function transport simulations. Phys Rev B 95(8):085310ADSGoogle Scholar
  74. Salpeter EE, Bethe HA (1951) A relativistic equation for bound-state problems. Phys Rev 84(6):1232–1242ADSMathSciNetzbMATHGoogle Scholar
  75. Serrano J et al (2010) Phonon dispersion relations of zinc oxide: inelastic neutron scattering and ab initio calculations. Phys Rev B 81(17):174304Google Scholar
  76. Shluger et al (2019) Defects in oxides in electronic devices. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  77. Stecher T, Reuter K, Oberhofer H (2016) First-principles free-energy barriers for photoelectrochemical surface reactions: proton abstraction at TiO2 (110). Phys Rev Lett 117(27):276001Google Scholar
  78. Stratmann RE, Scuseria GE, Frisch MJ (1998) An efficient implementation of time-dependent density-functional theory for the calculation of excitation energies of large molecules. J Chem Phys 109(19):8218–8224ADSGoogle Scholar
  79. Sun Q, Chan GK-L (2016) Quantum embedding theories. Acc Chem Res 49(12):2705–2712Google Scholar
  80. Sun L, Marrocchelli D, Yildiz B (2015) Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects. Nat Commun 6:6294Google Scholar
  81. Sun J et al (2016) Accurate first-principles structures and energies of diversely bonded systems from an efficient density functional. Nat Chem 8:831ADSGoogle Scholar
  82. Suzuki S, Tsuneda T, Hirao K (2012) A theoretical investigation on photocatalytic oxidation on the TiO2 surface. J Chem Phys 136(2):024706ADSGoogle Scholar
  83. Tadano T, Tsuneyuki S (2015) Self-consistent phonon calculations of lattice dynamical properties in cubic SrTiO3 with first-principles anharmonic force constants. Phys Rev B 92(5):054301Google Scholar
  84. Tao J et al (2003) Climbing the density functional ladder: nonempirical meta – generalized gradient approximation designed for molecules and solids. Phys Rev Lett 91(14):146401ADSGoogle Scholar
  85. Togo A, Tanaka I (2015) First principles phonon calculations in materials science. Scr Mater 108:1–5Google Scholar
  86. Tran F, Stelzl J, Blaha P (2016) Rungs 1 to 4 of DFT Jacob’s ladder: extensive test on the lattice constant, bulk modulus, and cohesive energy of solids. J Chem Phys 144(20):204120ADSGoogle Scholar
  87. T-Thienprasert J et al (2012) Identification of hydrogen defects in SrTiO3 by first-principles local vibration mode calculations. Phys Rev B 85(12):125205Google Scholar
  88. Valentin D, Cristiana SB, Cococcioni M (2014) First principles approaches to spectroscopic properties of complex materials, vol 347. Springer, Berlin/HeidelbergGoogle Scholar
  89. Varley JB et al (2017) High-throughput design of non-oxide p-type transparent conducting materials: data mining, search strategy, and identification of boron phosphide. Chem Mater 29(6):2568–2573Google Scholar
  90. Wang et al (2019) Strain control of domain structures in ferroelectric thin films – applications of phase-field method. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  91. Wang X, Zebarjadi M, Esfarjani K (2016) First principles calculations of solid-state thermionic transport in layered Van Der Waals heterostructures. Nanoscale 8(31):14695–14704ADSGoogle Scholar
  92. Youssef et al (2019) Defect equilibria and kinetics in crystalline insulating oxides – bulk and hetero-interfaces. In: Andreoni W, Yip S (eds) Handbook of materials modeling: applications: current and emerging materials. Springer International Publishing, ChamGoogle Scholar
  93. Youssef M, Yildiz B (2012) Intrinsic point-defect equilibria in tetragonal ZrO2: density functional theory analysis with finite-temperature effects. Phys Rev B 86(14):144109Google Scholar
  94. Youssef M, Yang M, Yildiz B (2016) Doping in the valley of hydrogen solubility: a route to designing hydrogen-resistant zirconium alloys. Phys Rev Appl 5(1):014008Google Scholar
  95. Zhang G, Lu Y, Wang X (2014) Hydrogen interactions with intrinsic point defects in hydrogen permeation barrier of [small alpha]-Al2O3: a first-principles study. Phys Chem Chem Phys 16(33):17523–17530Google Scholar
  96. Zhao Y et al (2015) Understanding the effect of monomeric iridium(III/IV) aquo complexes on the photoelectrochemistry of IrOx·nH2O-catalyzed water-splitting systems. J Am Chem Soc 137(27):8749–8757Google Scholar
  97. Zheng Y et al (2015) Advancing the electrochemistry of the hydrogen-evolution reaction through combining experiment and theory. Angew Chem Int Ed 54(1):52–65Google Scholar
  98. Zhou F et al (2014) Lattice anharmonicity and thermal conductivity from compressive sensing of first-principles calculations. Phys Rev Lett 113(18):185501Google Scholar

Copyright information

© Springer Nature Switzerland AG 2019

Authors and Affiliations

  1. 1.Department of Nuclear Science and EngineeringMassachusetts Institute of TechnologyCambridgeUSA
  2. 2.Department of Materials Science and EngineeringMassachusetts Institute of TechnologyCambridgeUSA
  3. 3.Computational Materials Physics, Faculty of PhysicsUniversity of ViennaViennaAustria

Section editors and affiliations

  • Cesare Franchini
    • 1
  • Bilge Yildiz
    • 2
    • 3
  1. 1.Faculty of Physics and Center for Computational Materials ScienceUniversity of ViennaViennaAustria
  2. 2.Department of Materials Science and EngineeringMassachusetts Institute of TechnologyCambridgeUSA
  3. 3.Department of Nuclear Science and EngineeringMassachusetts Institute of TechnologyCambridgeUSA

Personalised recommendations