*Supported by NSF Grants DMR and DMR and WFU s Center for Energy, Environment, and Sustainability.
|
|
- Byron Reynolds
- 6 years ago
- Views:
Transcription
1 First Principles Modeling of Electrolye Materials in All-Solid-State Batteries* N. A. W. Holzwarth** Department of Physics Wake Forest University, Winston-Salem, NC, USA, *Supported by NSF Grants DMR and DMR and WFU s Center for Energy, Environment, and Sustainability. **With help from: Nicholas Lepley, Ahmad Al-Qawasmeh (graduate students), Cameron Kates (undergraduate student), Yaojun Du (previous physics postdoc) and colleagues from WFU chemistry department Dr. Keerthi Senevirathne, Dr. Cynthia Day, Professor Michael Gross (visiting from Bucknell U.) and Professor Abdessadek Lachgar. 02/25/ th CSP Workshop 1
2 Outline What is meant by first principles? Computational methods & validation Why are we interested in solid electrolytes? How can first principles help? Survey of known solid electrolytes Prediction of new solid electrolytes Study of electrolyte/electrode interfaces Remaining challenges 02/25/ th CSP Workshop 2
3 What is meant by first principles? A series of well-controlled approximations 02/25/ th CSP Workshop 3
4 Summary of first-principles calculation methods Electronic coordinates Exact Schrodinger equation: Atomic coordinates H({ r },{ R a }) ({ r },{ R a }) E ({ r },{ R a }) i i i Born-Oppenheimer approximation Born & Huang, Dynamical Theory of Crystal Lattices, Oxford (1954) Approximate factorization: a Nuclei a Electrons a ({ ri },{ R }) X ({ R }) ({ ri },{ R }) 02/25/ th CSP Workshop 4
5 Summary of first-principles calculation methods -- continued Electronic Schrodinger equation: H ({ r },{ R }) ({ r },{ R }) U ({ R }) ({ r },{ R }) Electrons a Electrons a a Electrons a i i i H Electrons a ({ r },{ R }) i 2 Z e e 2 m r R r r 2 a 2 2 i a i a, i i i j Density functional theory Hohenberg and Kohn, Phys. Rev. 136 B864 (1964) Kohn and Sham, Phys. Rev. 140 A1133 (1965) Electron For electronic ground state: 0 density a a Mean field approximation: U 0 ({ R }) U 0 ( ( r),{ R }) Electrons a HK S ( r, ( r),{ R }) ( r) ( r) ( r) ( r) n n n n n i j 2 02/25/ th CSP Workshop 5
6 Summary of first-principles calculation methods -- continued Nuclear Hamiltonian (usually treated classically) H Nuclei a2 a { R } P ( ( r),{ R }) a a 2M Electron density a U0 02/25/ th CSP Workshop 6
7 H More computational details: 2 2 a 2 a Z e ( r ') ( r, ( r),{ R }) e d r ' Vxc ( ) a 2 m r r R r r ' Electrons 2 3 KS a Exchange-correlation functionals: LDA: J. Perdew and Y. Wang, Phys. Rev. B 45, (1992) GGA: J. Perdew, K. Burke, and M. Ernzerhof, PRL 77, 3865 (1996) HSE06: J. Heyd, G. E. Scuseria, and M. Ernzerhof, JCP 118, 8207 (2003) Numerical methods: Muffin-tin construction: Augmented Plane Wave developed by Slater linearized version by Andersen: J. C. Slater, Phys. Rev (1937) O. K. Andersen, Phys. Rev. B (1975) (LAPW) Pseudopotential methods: J. C. Phillips and L. Kleinman, Phys. Rev (1959) -- original idea P. Blöchl, Phys. Rev. B (1994) Projector Augmented Wave (PAW) method electron-nucleus electron-electron exchangecorrelation 02/25/ th CSP Workshop 7
8 Ground state energy: U 0 { R } 0 a ( ( r),{ R }) Determine formation energies a min U ( ( r),{ R }) Determine structural parameters a 2 Stable and meta-stable structures Normal modes of vibration ( r) ( r) Self-consistent electron density n n n Outputs of calculations: One-electron energies; densities of states 02/25/ th CSP Workshop 8
9 Estimate of ionic conductivity assuming activated hopping : 02/25/ th CSP Workshop 9
10 Public domain codes available for electronic structure calculations Method Codes Comments LAPW PAW elk.sourceforge.net Works well for smaller unit cells; variable unit cell optimization not implemented. Need to choose nonoverlapping muffin tin radii and avoid ghost solutions. Works well for large unit cells (<200 atoms or so); includes variable unit cell optimization. ATOMPAW pwpaw.wfu.edu Generates PAW datasets for abinit and quantum-espresso (and other codes) Other efforts: Gerbrand Ceder s group at MIT Materials Project; A Materials Genome Approach -- Stefano Curtarolo s group at Duke Energy Materials Laboratory /25/ th CSP Workshop 10
11 ATOMPAW Code for generating atomic datasets for PAW calculations Holzwarth, Tackett, and Matthews, CPC (2001) 02/25/ th CSP Workshop 11
12 02/25/ th CSP Workshop 12
13 Example validation of computation methods 02/25/ th CSP Workshop 13
14 Li 3 PO 4 crystals (Pmn2 1 ) (Pnma) 02/25/ th CSP Workshop 14
15 Validation of calculations A: B. N. Mavrin et al, J. Exp. Theor. Phys. 96,53 (2003); B: F. Harbach and F. Fischer, Phys. Status Solidi B 66, 237 (1974) room temp. C: Ref. B at liquid nitrogen temp.; D: L. Popović et al, J. Raman Spectrosc. 34,77 (2003). 02/25/ th CSP Workshop 15
16 What is meant by first principles? A series of well-controlled approximations Born-Oppenheimer Approximation Density Functional Approximation Local density Approximation (LDA) Numerical method: Projector Augmented Wave Validation Lattice vibration modes Heats of formation Activation energies for lattice migration 02/25/ th CSP Workshop 16
17 What is the interest in solid electrolytes? 02/25/ th CSP Workshop 17
18 Materials components of a Li ion battery
19 Example: Thin-film battery developed by Nancy Dudney and collaborators at Oak Ridge National Laboratory LiPON (lithium phosphorus oxinitride) From: N. J. Dudney, Interface 77(3) 44 (2008) 02/25/ th CSP Workshop 19
20 Solid vs liquid electrolytes in Li ion batteries Advantages 1. Excellent chemical and physical stability. 2. Perform well as thin film ( 1m) 3. Li + conduction only (excludes electrons). Advantages 1. Excellent contact area with high capacity electrodes. 2. Can accommodate size changes of electrodes during charge and discharge cycles. 3. Relatively high ionic conductivity. Solid electrolytes Disadvantages 1. Reduced contact area for high capacity electrodes. 2. Interface stress due to electrode charging and discharging. 3. Relatively low ionic conductivity. Liquid electrolytes Disadvantages 1. Relatively poor physical and chemical stability. 2. Relies on the formation of solid electrolyte interface (SEI) layer. 3. May have both Li + and electron conduction. 02/25/ th CSP Workshop 20
21 Motivation: Paper by N. Kayama, et. al in Nature Materials 10, (2011) 02/25/ th CSP Workshop 21
22 Motivation: Paper by N. Kamaya, et. al in Nature Materials 10, (2011) R T LiPON 02/25/ th CSP Workshop 22
23 Motivation: Paper by N. Kamaya, et. al in Nature Materials 10, (2011) Li 7 P 3 S 11 R T 02/25/ th CSP Workshop 23
24 Motivation: Paper by N. Kamaya, et. al in Nature Materials 10, (2011) Li 10 GeP 2 S 12 R T 02/25/ th CSP Workshop 24
25 How can computer simulations contribute to the development of materials? Examine known materials and predict new materials Structural forms Relative stabilities Analyze vibrational modes and other experimentally accessible properties Model ion migration mechanisms Vacancy migration Interstitial migration Vacancy-interstitial formation energies 02/25/ th CSP Workshop 25
26 The Li 2 PO 2 N story 02/25/ th CSP Workshop 26
27 Systematic study of LiPON materials Li x PO y N z (Yaojun A. Du and N. A. W. Holzwarth, Phys. Rev. B 81, (2010) ) 02/25/ th CSP Workshop 27
28 02/25/ th CSP Workshop 28
29 02/25/ th CSP Workshop 29
30 Li ion PO 2 N 2 ion (Pbcm) (Aem2) 02/25/ th CSP Workshop 30
31 Synthesis of Li 2 PO 2 N by Keerthi Senevirathne, Cynthia Day, Michael Gross, and Abdessadek Lachgar Method: High temperature solid state synthesis based on reaction 1 1 Li O P O P3 N5 Li2PO2N Structure from X-ray refinement: Cmc2 1 Li P O N Li ion PO 2 N 2 ion 02/25/ th CSP Workshop 31
32 Comparison of synthesized and predicted structures of Li 2 PO 2 N: Synthesized Predicted Li P O N SD-Li 2 PO 2 N (Cmc2 1 ) s 2 -Li 2 PO 2 N (Aem2) Calculations have now verified that the SD structure is more stable than the s 2 structure by 0.1 ev/fu. 02/25/ th CSP Workshop 32
33 Comparison of synthesized Li 2 PO 2 N with Li 2 SiO 3 SD-Li 2 PO 2 N (Cmc2 1 ) Li 2 SiO 3 (Cmc2 1 ) a=9.07 Å, b=5.40 Å, c=4.60 Å Li P O N a=9.39 Å, b=5.40 Å, c=4.66 Å K.-F. Hesse, Acta Cryst. B33, 901 (1977) Si 02/25/ th CSP Workshop 33
34 Electronic band structure of SD-Li 2 PO 2 N 02/25/ th CSP Workshop 34
35 More details of SD-Li 2 PO 2 N structure Ball and stick model Li P O N b c Isosurfaces (maroon) of charge density of states at top of valence band, primarily p states on N. 02/25/ th CSP Workshop 35
36 Vibrational spectrum of SD-Li 2 PO 2 N 02/25/ th CSP Workshop 36
37 Ionic conductivity of SD-Li 2 PO 2 N NEB analysis of E m (vacancy mechanism) 02/25/ th CSP Workshop 37
38 Summary of the Li 2 PO 2 N story Predicted on the basis of first principles theory Subsequently, experimentally realized by Keerthi Seneviranthe and colleagues; generally good agreement between experiment and theory Ion conductivity properties not (yet) competitive Simulations of other solid electrolytes and electrolyte/electrode interfaces 02/25/ th CSP Workshop 38
39 From ORNL: Experiment on electrolyte Li 3 PS 4 02/25/ th CSP Workshop 39
40 Crystal structure of bulk Li 3 PS 4 g-form Pmn2 1 (#31) Note: Li 3 PS 4 is also found in the b-form with Pnma (#62) structure 02/25/ th CSP Workshop 40
41 g-li 3 PS 4 [0 1 0] surface 02/25/ th CSP Workshop 41
42 Simulations of ideal g-li 3 PS 4 [0 1 0] surface in the presence of Li Initial configuration: Computed optimized structure: 02/25/ th CSP Workshop 42
43 More simulations of ideal g-li 3 PS 4 [0 1 0] surface in the presence of Li supercells containing 12 Li atoms and 2 or 4 electrolyte layers 02/25/ th CSP Workshop 43
44 g-li 3 PS 4 [0 1 0] surface in the presence of Li supercells containing 12 Li atoms and 2 or 4 electrolyte layers (greater detail) 2 electrolyte layers 4 electrolyte layers 02/25/ th CSP Workshop 44
45 Mystery: Models of ideal Li 3 PS 4 surfaces are computational found to be structurally (and chemically) altered by the presence of Li metal. (Also found for b-li 3 PS 4 and for various initial configurations of Li metal.) Experimentally, the ORNL group has found that solid Li 3 PS 4 electrolyte samples can be prepared in Li/ Li 3 PS 4 /Li cells and cycled many times 02/25/ th CSP Workshop 45
46 Computational counter example stable interface: Li/b-Li 3 PO 4 02/25/ th CSP Workshop 46
47 Computational counter example stable interface: Li/SD-Li 2 PO 2 N 02/25/ th CSP Workshop 47
48 Back to mystery: Models of ideal Li 3 PS 4 surfaces are computational found to be structurally (and chemically) altered by the presence of Li metal. (Also found for b-li 3 PS 4 and for various initial configurations of Li metal.) Experimentally, the ORNL group has found that solid Li 3 PS 4 electrolyte samples can be prepared in Li/ Li 3 PS 4 /Li cells and cycled many times. Possible solution: Thin protective buffer layer at Li 3 PS 4 surface can stabilize electrolyte for example Li 2 S/Li 3 PS 4 /Li 2 S 02/25/ th CSP Workshop 48
49 Idealized Li 2 S/Li 3 PS 4 /Li 2 S system Details: Thin film of cubic Li 2 S oriented in its non-polar [1 1 0] direction, optimized on [0 1 0] surface of g-li 3 PS 4. While the Li 2 S film was slightly strained, the binding energy of the composite was found to be stable with a binding energy of -0.9 ev. 02/25/ th CSP Workshop 49
50 Idealized Li 2 S/Li 3 PS 4 /Li 2 S system optimized in presence of Li 02/25/ th CSP Workshop 50
51 Summary of the interface simulations: Models of ideal Li 3 PO 4 and Li 2 PO 2 N surfaces are computational found to structurally stable in the presence of Li metal. Models of ideal Li 3 PS 4 surfaces are computational found to be structurally (and chemically) altered by the presence of Li metal. (Also found for b-li 3 PS 4 and for various initial configurations of Li metal.) Thin protective buffer layer of Li 2 S at Li 3 PS 4 surface can stabilize electrolyte; Li 2 S/Li 3 PS 4 /Li 2 S is found to be stable in the presence of Li metal. Experimentally, the ORNL samples of solid Li 3 PS 4 electrolyte, prepared in Li/ Li 3 PS 4 /Li cells and cycled many times, may form thin buffer layer in first few cycles. 02/25/ th CSP Workshop 51
52 Additional thoughts Limitations of first principles modeling Small simulation cells Zero temperature Possible extensions Develop approximation schemes for treatment of larger supercells Use molecular dynamics and/or Monte Carlo techniques 02/25/ th CSP Workshop 52
Serendipitous. *Supported by NSF Grants DMR and DMR and WFU s Center for Energy, Environment, and Sustainability.
Serendipitous ^ Design and synthesis of a crystalline LiPON electrolyte* N. A. W. Holzwarth** Department of Physics Wake Forest University, Winston-Salem, NC, USA, 27109 *Supported by NSF Grants DMR-0705239
More information*Supported by NSF Grant DMR and WFU s Center for Energy, Environment, and Sustainability.
Simulations of Idealized Solid Electrolytes for Solid State Battery Designs* N. A. W. Holzwarth** Department of Physics Wake Forest University, Winston-Salem, NC, USA, 27109 *Supported by NSF Grant DMR-1105485
More informationSimulations of Li ion diffusion in the electrolyte material Li 3 PO 4
Simulations of Li ion diffusion in the electrolyte material Li 3 PO 4 a, b N. A. W. Holzwarth Wake Forest University, Winston-Salem, NC, USA Motivation Calculational methods Diffusion in crystalline material
More informationFirst principles computer simulations of Li 10 GeP 2 S 12 and related lithium superionic conductors*
First principles computer simulations of Li 10 GeP 2 S 12 and related lithium superionic conductors* N. A. W. Holzwarth Wake Forest University, Winston-Salem, NC, USA, 27109 Motivation and background information
More informationLi = 1.6, rc Sn = 2.3, and rc S = 1.7 in bohr units. The
: Simulations of Its Structure and Electrolyte Properties N. A. W. Holzwarth Department of Physics, Wake Forest University, Winston-Salem, NC 2719, USA First principles simulations show that the ground
More informationLi 4 SnS 4 : Simulations of Its Structure and Electrolyte Properties
: Simulations of Its Structure and Electrolyte Properties N. A. W. Holzwarth Department of Physics, Wake Forest University, Winston-Salem, NC, USA Introduction Recently, there has been significant progress
More informationSimulations of Li-ion migration in LiPON electrolytes
Simulations of Li-ion migration in LiPON electrolytes Yaojun Du and N. A. W. Holzwarth: Department of Physics, Wake Forest University, Winston-Salem, NC, USA Introduction The thin film solid electrolyte
More informationFirst principles computer simulations of Li 10 GeP 2 S 12 and related lithium superionic conductors
First principles computer simulations of Li 10 GeP 2 S 12 and related lithium superionic conductors N. A. W. Holzwarth Department of Physics, Wake Forest University, Winston-Salem, NC, 27109, USA Introduction
More informationLi ion migration in Li 3 PO 4 electrolytes: Effects of O vacancies and N substitutions. Winston-Salem, North Carolina 27106, USA
75 Downloaded 22 Dec 28 to 52.7.52.46. Redistribution subject to ECS license or copyright; see http://www.ecsdl.org/terms_use.jsp ECS Transactions, 3 (26) 75-82 (28).49/.35379 The Electrochemical Society
More informationTwo implementations of the Projector Augmented Wave (PAW) formalism
Introduction The tools available for detailed first-principles studies of materials have benefited enormously from the development of several international collaborations engaged in developing open source
More informationBiographical Sketch: N. A. W. Holzwarth (updated 1/8/2017)
Biographical Sketch: N. A. W. Holzwarth (updated 1/8/2017) Address Mail: Wake Forest University, Department of Physics, Winston-Salem, NC 27109-7507 Email: natalie@wfu.edu Phone: (336)-758-5510 (Office)
More informationComputational Study of ( ) and ( ) *
Computational Study of ( ) and ( ) * Jason Howard, advisor Natalie Holzwarth Department of Physics, Wake Forest University, Winston-Salem, NC USA Li Sn O S Li2SnO3 Li2SnS3 *Supported by NSF grants DMR-1105485
More informationModeling Crystalline Electrolytes: Li 7 P 3 S 11 and Analogous Phosphates
Modeling Crystalline Electrolytes: Li 7 P S and Analogous Phosphates Wake Forest University February 27, 22 Why Study Thiophosphate Solid Electrolytes Many solid electrolytes have safety advantages over
More informationThe electronic structure of materials 2 - DFT
Quantum mechanics 2 - Lecture 9 December 19, 2012 1 Density functional theory (DFT) 2 Literature Contents 1 Density functional theory (DFT) 2 Literature Historical background The beginnings: L. de Broglie
More information(This is a sample cover image for this issue. The actual cover is not yet available at this time.)
(This is a sample cover image for this issue. The actual cover is not yet available at this time.) This article appeared in a journal published by Elsevier. The attached copy is furnished to the author
More informationSurface structure and stability in Li 3 PS 4 and Li 3 PO 4 electrolytes from first principles
: Bulk Surface structure and stability in Li 3 PS 4 and Li 3 PO 4 electrolytes from first principles Wake Forest University APS March Meeting 2013 : Bulk Outline 1 Solid Electrolytes Li 3 PS 4 and Li 3
More information6. Computational Design of Energy-related Materials
6. Computational Design of Energy-related Materials Contents 6.1 Atomistic Simulation Methods for Energy Materials 6.2 ab initio design of photovoltaic materials 6.3 Solid Ion Conductors for Fuel Cells
More informationFULL POTENTIAL LINEARIZED AUGMENTED PLANE WAVE (FP-LAPW) IN THE FRAMEWORK OF DENSITY FUNCTIONAL THEORY
FULL POTENTIAL LINEARIZED AUGMENTED PLANE WAVE (FP-LAPW) IN THE FRAMEWORK OF DENSITY FUNCTIONAL THEORY C.A. Madu and B.N Onwuagba Department of Physics, Federal University of Technology Owerri, Nigeria
More informationPS 4. Cl 2. Superionic Conductors Predicted from Silver. Thiophosphates using Efficiently Tiered Ab Initio. Molecular Dynamics Simulations
Li 3 Y(PS 4 ) 2 and Li 5 PS 4 Cl 2 : New Lithium Superionic Conductors Predicted from Silver Thiophosphates using Efficiently Tiered Ab Initio Molecular Dynamics Simulations Supporting Information Zhuoying
More informationIntegrated Computational Materials Engineering Education
Integrated Computational Materials Engineering Education Lecture on Density Functional Theory An Introduction Mark Asta Dept. of Materials Science and Engineering, University of California, Berkeley &
More informationSupporting Information Tuning Local Electronic Structure of Single Layer MoS2 through Defect Engineering
Supporting Information Tuning Local Electronic Structure of Single Layer MoS2 through Defect Engineering Yan Chen, 1,2,,$, * Shengxi Huang, 3,6, Xiang Ji, 2 Kiran Adepalli, 2 Kedi Yin, 8 Xi Ling, 3,9 Xinwei
More informationPseudopotentials: design, testing, typical errors
Pseudopotentials: design, testing, typical errors Kevin F. Garrity Part 1 National Institute of Standards and Technology (NIST) Uncertainty Quantification in Materials Modeling 2015 Parameter free calculations.
More informationAndré Schleife Department of Materials Science and Engineering
André Schleife Department of Materials Science and Engineering Yesterday you (should have) learned this: http://upload.wikimedia.org/wikipedia/commons/e/ea/ Simple_Harmonic_Motion_Orbit.gif 1. deterministic
More informationFundamentals and applications of Density Functional Theory Astrid Marthinsen PhD candidate, Department of Materials Science and Engineering
Fundamentals and applications of Density Functional Theory Astrid Marthinsen PhD candidate, Department of Materials Science and Engineering Outline PART 1: Fundamentals of Density functional theory (DFT)
More informationIntroduction to First-Principles Method
Joint ICTP/CAS/IAEA School & Workshop on Plasma-Materials Interaction in Fusion Devices, July 18-22, 2016, Hefei Introduction to First-Principles Method by Guang-Hong LU ( 吕广宏 ) Beihang University Computer
More informationTeoría del Funcional de la Densidad (Density Functional Theory)
Teoría del Funcional de la Densidad (Density Functional Theory) Motivation: limitations of the standard approach based on the wave function. The electronic density n(r) as the key variable: Functionals
More informationMulti-Scale Modeling from First Principles
m mm Multi-Scale Modeling from First Principles μm nm m mm μm nm space space Predictive modeling and simulations must address all time and Continuum Equations, densityfunctional space scales Rate Equations
More informationDensity Functional Theory. Martin Lüders Daresbury Laboratory
Density Functional Theory Martin Lüders Daresbury Laboratory Ab initio Calculations Hamiltonian: (without external fields, non-relativistic) impossible to solve exactly!! Electrons Nuclei Electron-Nuclei
More informationBasics of density-functional theory and fast guide to actual calculations Matthias Scheffler
Basics of density-functional theory and fast guide to actual calculations Matthias Scheffler http://www.fhi-berlin.mpg.de/th/th.html I. From the many-particle problem to the Kohn-Sham functional II. From
More informationSupporting information. The Unusual and the Expected in the Si/C Phase Diagram. Guoying Gao, N. W. Ashcroft and Roald Hoffmann.
Supporting information The Unusual and the Expected in the Si/C Phase Diagram Guoying Gao, N. W. Ashcroft and Roald Hoffmann Table of Contents Computational Methods...S1 Hypothetical Structures for Si
More informationExplaining the apparent arbitrariness of the LDA-1/2 self-energy. correction method applied to purely covalent systems
Explaining the apparent arbitrariness of the LDA-1/2 self-energy correction method applied to purely covalent systems Kan-Hao Xue, 1,2 Leonardo R. C. Fonseca, 3 and Xiang-Shui Miao 1,2 1 School of Optical
More informationSupporting Information
Supporting Information The Origin of Active Oxygen in a Ternary CuO x /Co 3 O 4 -CeO Catalyst for CO Oxidation Zhigang Liu, *, Zili Wu, *, Xihong Peng, ++ Andrew Binder, Songhai Chai, Sheng Dai *,, School
More informationIntroduction to Density Functional Theory with Applications to Graphene Branislav K. Nikolić
Introduction to Density Functional Theory with Applications to Graphene Branislav K. Nikolić Department of Physics and Astronomy, University of Delaware, Newark, DE 19716, U.S.A. http://wiki.physics.udel.edu/phys824
More informationCHAPTER 3 WIEN2k. Chapter 3 : WIEN2k 50
CHAPTER 3 WIEN2k WIEN2k is one of the fastest and reliable simulation codes among computational methods. All the computational work presented on lanthanide intermetallic compounds has been performed by
More informationInstitut Néel Institut Laue Langevin. Introduction to electronic structure calculations
Institut Néel Institut Laue Langevin Introduction to electronic structure calculations 1 Institut Néel - 25 rue des Martyrs - Grenoble - France 2 Institut Laue Langevin - 71 avenue des Martyrs - Grenoble
More informationNorm-conserving pseudopotentials and basis sets in electronic structure calculations. Javier Junquera. Universidad de Cantabria
Norm-conserving pseudopotentials and basis sets in electronic structure calculations Javier Junquera Universidad de Cantabria Outline Pseudopotentials Why pseudopotential approach is useful Orthogonalized
More informationSupporting information. Realizing Two-Dimensional Magnetic Semiconductors with. Enhanced Curie Temperature by Antiaromatic Ring Based
Supporting information Realizing Two-Dimensional Magnetic Semiconductors with Enhanced Curie Temperature by Antiaromatic Ring Based Organometallic Frameworks Xingxing Li and Jinlong Yang* Department of
More informationFirst-principles studies of cation-doped spinel LiMn 2 O 4 for lithium ion batteries
First-principles studies of cation-doped spinel LiMn 2 O 4 for lithium ion batteries Siqi Shi, 1 Ding-sheng Wang, 2 Sheng Meng, 2 Liquan Chen, 1 and Xuejie Huang 1, * 1 Nanoscale Physics and Devices Laboratory,
More informationA COMPUTATIONAL INVESTIGATION OF MIGRATION ENTHALPIES AND ELECTRONIC STRUCTURE IN SrFeO 3-δ
A COMPUTATIONAL INVESTIGATION OF MIGRATION ENTHALPIES AND ELECTRONIC STRUCTURE IN SrFeO 3-δ A. Predith and G. Ceder Massachusetts Institute of Technology Department of Materials Science and Engineering
More informationPractical Guide to Density Functional Theory (DFT)
Practical Guide to Density Functional Theory (DFT) Brad Malone, Sadas Shankar Quick recap of where we left off last time BD Malone, S Shankar Therefore there is a direct one-to-one correspondence between
More informationSupporting information. Origins of High Electrolyte-Electrode Interfacial Resistances in Lithium Cells. Containing Garnet Type LLZO Solid Electrolytes
Electronic Supplementary Material (ESI) for Physical Chemistry Chemical Physics. This journal is the Owner Societies 2014 Supporting information Origins of High Electrolyte-Electrode Interfacial Resistances
More informationIntroduction to DFT and its Application to Defects in Semiconductors
Introduction to DFT and its Application to Defects in Semiconductors Noa Marom Physics and Engineering Physics Tulane University New Orleans The Future: Computer-Aided Materials Design Can access the space
More informationPseudopotentials for hybrid density functionals and SCAN
Pseudopotentials for hybrid density functionals and SCAN Jing Yang, Liang Z. Tan, Julian Gebhardt, and Andrew M. Rappe Department of Chemistry University of Pennsylvania Why do we need pseudopotentials?
More informationELECTRONIC AND MAGNETIC PROPERTIES OF BERKELIUM MONONITRIDE BKN: A FIRST- PRINCIPLES STUDY
ELECTRONIC AND MAGNETIC PROPERTIES OF BERKELIUM MONONITRIDE BKN: A FIRST- PRINCIPLES STUDY Gitanjali Pagare Department of Physics, Sarojini Naidu Govt. Girls P. G. Auto. College, Bhopal ( India) ABSTRACT
More informationAnion-redox nanolithia cathodes for Li-ion batteries
ARTICLE NUMBER: 16111 Anion-redox nanolithia cathodes for Li-ion batteries Zhi Zhu 1,2, Akihiro Kushima 1,2, Zongyou Yin 1,2, Lu Qi 3 *, Khalil Amine 4, Jun Lu 4 * and Ju Li 1,2 * 1 Department of Nuclear
More informationMagnetism in transition metal oxides by post-dft methods
Magnetism in transition metal oxides by post-dft methods Cesare Franchini Faculty of Physics & Center for Computational Materials Science University of Vienna, Austria Workshop on Magnetism in Complex
More informationarxiv: v1 [cond-mat.mes-hall] 15 Aug 2014
The potential applications of phosphorene as anode arxiv:1408.3488v1 [cond-mat.mes-hall] 15 Aug 2014 materials in Li-ion batteries Shijun Zhao,, and Wei Kang, HEDPS, Center for Applied Physics and Technology,
More informationDensity Functional Theory (DFT)
Density Functional Theory (DFT) An Introduction by A.I. Al-Sharif Irbid, Aug, 2 nd, 2009 Density Functional Theory Revolutionized our approach to the electronic structure of atoms, molecules and solid
More informationChris G. Van de Walle Materials Department, UCSB
First-principles simulations of defects in oxides and nitrides Chris G. Van de Walle Materials Department, UCSB Acknowledgments: A. Janotti, J. Lyons, J. Varley, J. Weber (UCSB) P. Rinke (FHI), M. Scheffler
More informationDensity Functional Theory for Electrons in Materials
Density Functional Theory for Electrons in Materials Richard M. Martin Department of Physics and Materials Research Laboratory University of Illinois at Urbana-Champaign 1 Density Functional Theory for
More informationHuman ages are named after materials - stone, bronze, iron, nuclear, silicon
MATERIALS ARE KEY TO SOCIETAL WELL BEING Human ages are named after materials - stone, bronze, iron, nuclear, silicon MATERIALS ARE KEY TO SOCIETAL WELL BEING We need novel materials for: Energy harvesting,
More informationProjector augmented wave Implementation
Projector augmented wave Implementation Peter. E. Blöchl Institute for Theoretical Physics Clausthal University of Technology, Germany http://www.pt.tu-clausthal.de/atp/ 1 = Projector augmented wave +
More informationElectronic Supplementary Information for. Impact of Intermediate Sites on Bulk Diffusion Barriers: Mg. Intercalation in Mg 2 Mo 3 O 8
Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A. This journal is The Royal Society of Chemistry 2016 Electronic Supplementary Information for Impact of Intermediate Sites on
More information1 Density functional theory (DFT)
1 Density functional theory (DFT) 1.1 Introduction Density functional theory is an alternative to ab initio methods for solving the nonrelativistic, time-independent Schrödinger equation H Φ = E Φ. The
More informationDENSITY FUNCTIONAL THEORY FOR NON-THEORISTS JOHN P. PERDEW DEPARTMENTS OF PHYSICS AND CHEMISTRY TEMPLE UNIVERSITY
DENSITY FUNCTIONAL THEORY FOR NON-THEORISTS JOHN P. PERDEW DEPARTMENTS OF PHYSICS AND CHEMISTRY TEMPLE UNIVERSITY A TUTORIAL FOR PHYSICAL SCIENTISTS WHO MAY OR MAY NOT HATE EQUATIONS AND PROOFS REFERENCES
More informationComputational Research on Lithium Ion Battery Materials
Computational Research on Lithium Ion Battery Materials by Ping Tang A Dissertation Submitted to the Graduate Faculty of WAKE FOREST UNIVERSITY in Partial Fulfillment of the Requirements for the Degree
More informationAn Approximate DFT Method: The Density-Functional Tight-Binding (DFTB) Method
Fakultät für Mathematik und Naturwissenschaften - Lehrstuhl für Physikalische Chemie I / Theoretische Chemie An Approximate DFT Method: The Density-Functional Tight-Binding (DFTB) Method Jan-Ole Joswig
More informationRe-evaluating CeO 2 Expansion Upon Reduction: Non-counterpoised Forces, Not Ionic Radius Effects, are the Cause
Re-evaluating CeO 2 Expansion Upon Reduction: Non-counterpoised Forces, Not Ionic Radius Effects, are the Cause Christopher L. Muhich, a* a ETH Zurich, Department of Mechanical and Process Engineering,
More informationSolid State Ionics 284 (2016) Contents lists available at ScienceDirect. Solid State Ionics. journal homepage:
Solid State Ionics 284 (216) 61 7 Contents lists available at ScienceDirect Solid State Ionics journal homepage: www.elsevier.com/locate/ssi Structural and electrolyte properties of Li 4 P 2 S 6 Zachary
More informationMgO-decorated carbon nanotubes for CO 2 adsorption: first principles calculations
MgO-decorated carbon nanotubes for CO 2 adsorption: first principles calculations Zhu Feng( ), Dong Shan( ), and Cheng Gang( ) State Key Laboratory for Superlattices and Microstructures, Institute of Semiconductors,
More informationKey concepts in Density Functional Theory (I) Silvana Botti
From the many body problem to the Kohn-Sham scheme European Theoretical Spectroscopy Facility (ETSF) CNRS - Laboratoire des Solides Irradiés Ecole Polytechnique, Palaiseau - France Temporary Address: Centre
More informationComparison of various abinitio codes used in periodic calculations
Comparison of various abinitio codes used in periodic calculations 1 Prof.P. Ravindran, Department of Physics, Central University of Tamil Nadu, India & Center for Materials Science and Nanotechnology,
More informationDept of Mechanical Engineering MIT Nanoengineering group
1 Dept of Mechanical Engineering MIT Nanoengineering group » To calculate all the properties of a molecule or crystalline system knowing its atomic information: Atomic species Their coordinates The Symmetry
More informationChapter 3. The (L)APW+lo Method. 3.1 Choosing A Basis Set
Chapter 3 The (L)APW+lo Method 3.1 Choosing A Basis Set The Kohn-Sham equations (Eq. (2.17)) provide a formulation of how to practically find a solution to the Hohenberg-Kohn functional (Eq. (2.15)). Nevertheless
More informationDesigned nonlocal pseudopotentials for enhanced transferability
PHYSICAL REVIEW B VOLUME 59, NUMBER 19 15 MAY 1999-I Designed nonlocal pseudopotentials for enhanced transferability Nicholas J. Ramer and Andrew M. Rappe Department of Chemistry and Laboratory for Research
More informationNew applications of Diffusion Quantum Monte Carlo
New applications of Diffusion Quantum Monte Carlo Paul R. C. Kent (ORNL) Graphite: P. Ganesh, J. Kim, C. Park, M. Yoon, F. A. Reboredo (ORNL) Platinum: W. Parker, A. Benali, N. Romero (ANL), J. Greeley
More informationAb initio Electronic Structure
Ab initio Electronic Structure M. Alouani IPCMS, UMR 7504, Université Louis Pasteur, Strasbourg France http://www-ipcms.u-strasbg.fr In coll. with: B. Arnaud, O. Bengone, Y. Dappe, and S. Lebègue 1965
More informationIs the homogeneous electron gas homogeneous?
Is the homogeneous electron gas homogeneous? Electron gas (jellium): simplest way to view a metal homogeneous and normal Hartree-Fock: simplest method for many-electron systems a single Slater determinant
More informationA DFT Study on Electronic Structures and Elastic Properties of AgX (X=C, N) in Rock Salt Structure
Invertis Journal of Jameson Science Maibam, and Technology, Kh. Kabita, Vol. B. Indrajit 7, No. 2, Sharma, 2014. R.K. ; pp. Thapa 114-118 and R.K. Brojen Singh A DFT Study on Electronic Structures and
More informationAb-initio Electronic Structure Calculations β and γ KNO 3 Energetic Materials
ISSN 0974-9373 Vol. 15 No.3 (2011) Journal of International Academy of Physical Sciences pp. 337-344 Ab-initio Electronic Structure Calculations of α, β and γ KNO 3 Energetic Materials Pradeep Jain and
More informationAll-Electron Full-Potential Calculations at O(ASA) Speed A Fata Morgana?
All-Electron Full-Potential Calculations at O(ASA) Speed A Fata Morgana? SFB 484, Teilprojekt D6 October 5, 2007 Outline 1 2 3 Outline 1 2 3 Outline 1 2 3 Outline 1 2 3 Back in the 1930 s... John C. Slater
More informationElectronic Supplementary Information
Electronic Supplementary Information Stable cycling of lithium sulfide cathodes through strong affinity with a bifunctional binder Zhi Wei Seh, Qianfan Zhang, Weiyang Li, Guangyuan Zheng, Hongbin Yao,
More informationExchange-Correlation Functional
Exchange-Correlation Functional Aiichiro Nakano Collaboratory for Advanced Computing & Simulations Depts. of Computer Science, Physics & Astronomy, Chemical Engineering & Materials Science, and Biological
More informationDefects in Semiconductors
Defects in Semiconductors Mater. Res. Soc. Symp. Proc. Vol. 1370 2011 Materials Research Society DOI: 10.1557/opl.2011. 771 Electronic Structure of O-vacancy in High-k Dielectrics and Oxide Semiconductors
More informationThe effect of point defects in zircon
aterials for nuclear waste immobilization: The effect of point defects in zircon iguel Pruneda Department of Earth Sciences University of Centre for Ceramic Immobilisation Radiation damage process α-decay
More informationPHYSICAL REVIEW B, VOLUME 65,
PHYSICAL REVIEW B, VOLUME 65, 245212 Cohesive properties of group-iii nitrides: A comparative study of all-electron and pseudopotential calculations using the generalized gradient approximation M. Fuchs,
More informationSUPPLEMENTARY INFORMATION
Synthesis of an open-framework allotrope of silicon Duck Young Kim, Stevce Stefanoski, Oleksandr O. Kurakevych, Timothy A. Strobel Electronic structure calculations Electronic structure calculations and
More informationSolid State Theory: Band Structure Methods
Solid State Theory: Band Structure Methods Lilia Boeri Wed., 11:00-12:30 HS P3 (PH02112) http://itp.tugraz.at/lv/boeri/ele/ Who am I? Assistant Professor, Institute for Theoretical and Computational Physics,
More informationMODULE 2: QUANTUM MECHANICS. Practice: Quantum ESPRESSO
MODULE 2: QUANTUM MECHANICS Practice: Quantum ESPRESSO I. What is Quantum ESPRESSO? 2 DFT software PW-DFT, PP, US-PP, PAW http://www.quantum-espresso.org FREE PW-DFT, PP, PAW http://www.abinit.org FREE
More informationSpring College on Computational Nanoscience May Variational Principles, the Hellmann-Feynman Theorem, Density Functional Theor
2145-25 Spring College on Computational Nanoscience 17-28 May 2010 Variational Principles, the Hellmann-Feynman Theorem, Density Functional Theor Stefano BARONI SISSA & CNR-IOM DEMOCRITOS Simulation Center
More informationCHAPTER 6. ELECTRONIC AND MAGNETIC STRUCTURE OF ZINC-BLENDE TYPE CaX (X = P, As and Sb) COMPOUNDS
143 CHAPTER 6 ELECTRONIC AND MAGNETIC STRUCTURE OF ZINC-BLENDE TYPE CaX (X = P, As and Sb) COMPOUNDS 6.1 INTRODUCTION Almost the complete search for possible magnetic materials has been performed utilizing
More informationFIRST-PRINCIPLES INVESTIGATION OF ELECTRONIC PROPERTIES IN SODIUM-ION ELECTROLYTES FOR SOLID-STATE BATTERY MATERIALS LARRY E. RUSH JR.
FIRST-PRINCIPLES INVESTIGATION OF ELECTRONIC PROPERTIES IN SODIUM-ION ELECTROLYTES FOR SOLID-STATE BATTERY MATERIALS BY LARRY E. RUSH JR. A Thesis Submitted to the Graduate Faculty of WAKE FOREST UNIVERSITY
More informationKey concepts in Density Functional Theory
From the many body problem to the Kohn-Sham scheme ILM (LPMCN) CNRS, Université Lyon 1 - France European Theoretical Spectroscopy Facility (ETSF) December 12, 2012 Lyon Outline 1 The many-body problem
More informationComputer Modeling of Crystalline Electrolytes Lithium Thiophosphates and Phosphates
Computer Modeling of Crystalline Electrolytes thium Thiophosphates and hosphates N. D. Lepley and N. A. W. Holzwarth Department of hysics, Wake Forest University, Winston-alem, North Carolina 279, UA (Dated:
More information[100] directed Cu-doped h-coo Nanorods: Elucidation of. Growth Mechanism and Application to Lithium-Ion Batteries
Supplementary Information [100] directed Cu-doped h-coo Nanorods: Elucidation of Growth Mechanism and Application to Lithium-Ion Batteries Ki Min Nam, Young Cheol Choi, Sung Chul Jung, Yong-Il Kim, Mi
More informationOrbital Density Dependent Functionals
Orbital Density Dependent Functionals S. Kluepfel1, P. Kluepfel1, Hildur Guðmundsdóttir1 and Hannes Jónsson1,2 1. Univ. of Iceland; 2. Aalto University Outline: Problems with GGA approximation (PBE, RPBE,...)
More informationALMA: All-scale predictive design of heat management material structures
ALMA: All-scale predictive design of heat management material structures Version Date: 2015.11.13. Last updated 2015.12.02 Purpose of this document: Definition of a data organisation that is applicable
More informationThe Nature of the Interlayer Interaction in Bulk. and Few-Layer Phosphorus
Supporting Information for: The Nature of the Interlayer Interaction in Bulk and Few-Layer Phosphorus L. Shulenburger, A.D. Baczewski, Z. Zhu, J. Guan, and D. Tománek, Sandia National Laboratories, Albuquerque,
More informationSTRUCTURAL AND MECHANICAL PROPERTIES OF AMORPHOUS SILICON: AB-INITIO AND CLASSICAL MOLECULAR DYNAMICS STUDY
STRUCTURAL AND MECHANICAL PROPERTIES OF AMORPHOUS SILICON: AB-INITIO AND CLASSICAL MOLECULAR DYNAMICS STUDY S. Hara, T. Kumagai, S. Izumi and S. Sakai Department of mechanical engineering, University of
More informationOutline. Introduction: graphene. Adsorption on graphene: - Chemisorption - Physisorption. Summary
Outline Introduction: graphene Adsorption on graphene: - Chemisorption - Physisorption Summary 1 Electronic band structure: Electronic properties K Γ M v F = 10 6 ms -1 = c/300 massless Dirac particles!
More informationAb initio calculations of fundamental properties of SrTe 1 x O x alloys
Bull. Mater. Sci., Vol. 39, No. 3, June 2016, pp. 827 835. DOI 10.1007/s12034-016-1189-8 c Indian Academy of Sciences. Ab initio calculations of fundamental properties of SrTe 1 x O x alloys J ZEROUAL
More informationfor Magnesium-Ion Batteries
[Supporting Information] Cointercalation of Mg 2+ Ions into Graphite for Magnesium-Ion Batteries Dong Min Kim, Sung Chul Jung, Seongmin Ha, Youngjin Kim, Yuwon Park, Ji Heon Ryu ǂ, Young Kyu Han*,, Kyu
More informationIndependent electrons in an effective potential
ABC of DFT Adiabatic approximation Independent electrons in an effective potential Hartree Fock Density Functional Theory MBPT - GW Density Functional Theory in a nutshell Every observable quantity of
More informationSupplementary Information: Construction of Hypothetical MOFs using a Graph Theoretical Approach. Peter G. Boyd and Tom K. Woo*
Electronic Supplementary Material ESI) for CrystEngComm. This journal is The Royal Society of Chemistry 2016 Supplementary Information: Construction of Hypothetical MOFs using a Graph Theoretical Approach
More informationMaterials for Li-Ion Batteries
Modeling of Electrode Materials for Li-Ion Batteries M. Atanasov, J. -L. Barras, L. Benco, C. Daul, E. Deiss + University of Fribourg, Switzerland + Paul Scherrer Institute, Villigen, Switzerland Battery
More informationSupporting Information
Electronic Supplementary Material (ESI) for Nanoscale. This journal is The Royal Society of Chemistry 2015 Supporting Information Single Layer Lead Iodide: Computational Exploration of Structural, Electronic
More informationKey concepts in Density Functional Theory (II)
Kohn-Sham scheme and band structures European Theoretical Spectroscopy Facility (ETSF) CNRS - Laboratoire des Solides Irradiés Ecole Polytechnique, Palaiseau - France Present Address: LPMCN Université
More informationELECTRONIC AND STRUCTURAL PROPERTIES OF TIN DIOXIDE IN CUBIC PHASE *
Iranian Journal of Science & Technology, Transaction A, Vol. 34, No. A Printed in the Islamic Republic of Iran, 1 Shiraz University ELECTRONIC AND STRUCTURAL PROPERTIES OF TIN DIOXIDE IN CUBIC PHASE *
More informationSupporting Information for: Atomic Substitution Enabled Synthesis of Vacancy-Rich Two- Rechargeable Magnesium Batteries
Supporting Information for: Atomic Substitution Enabled Synthesis of Vacancy-Rich Two- Dimensional Black TiO 2-x Nanoflakes for High-Performance Rechargeable Magnesium Batteries Authors: Yanrong Wang,
More informationAb initio study of the electronic band structure and phonon dispersion spectra of Silicon disulphide (SiP 2 ) and Silicon diarsenide (SiAs 2 )
American Journal of Engineering Research (AJER) e-issn: 2320-0847 p-issn : 2320-0936 Volume-6, Issue-12, pp-439-447 www.ajer.org Research Paper Open Access Ab initio study of the electronic band structure
More information