DOCSLIB.ORG

First Principles-Based Interatomic Potentials for Modeling the Body-Centered Cubic Metals V, Nb, Ta, Mo, and W

Total Page：16

File Type：pdf, Size：1020Kb

Download full-text PDF Read full-text

Load more

First Principles-Based Interatomic Potentials for Modeling the Body-Centered Cubic Metals V, Nb, Ta, Mo, and W Dissertation Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University By Michael Richard Fellinger, B.S., M.S. Graduate Program in Physics The Ohio State University 2013 Dissertation Committee: John W. Wilkins, Advisor Jon Pelz Nandini Trivedi Michael Mills c Copyright by Michael Richard Fellinger 2013 Abstract Accurate large-scale materials simulations depend crucially on high-quality clas- sical interatomic potentials. This study constructs embedded-atom method (EAM) and modified embedded-atom method (MEAM) interatomic potentials for the body- centered cubic (bcc) metals V, Nb, Ta, Mo, and W from data generated by first- principles density-functional theory (DFT) calculations. Comparisons of a wide range of computed materials properties to DFT calculations and experimental data test the quality of the potentials. The analysis reveals that EAM and MEAM potentials generated from low-pressure DFT data accurately model many properties of the bcc metals at low to moderate pressure, but MEAM potentials generated from low- and high-pressure data are needed for quantitative high-pressure simulations. These high- pressure potentials capture much of the physics of the bcc metals at ambient con- ditions, produce the correct energies and geometries of multiple crystal phases, and correctly model the pressure dependence of mechanical properties. The potentials provide a reliable method for studying the deformation of bcc metals over a broad range of temperature and strain conditions, and also offer a viable starting point for constructing accurate potentials for technologically important alloys containing the bcc metals. ii Acknowledgments I thank John Wilkins for his guidance and support. This work would not have been possible without him. I thank Hyoungki Park and Jeremy Nicklas for perform- ing calculations and writing code, and for thoughtful discussions about interatomic potentials. All aspects of this project were improved by their efforts. Richard Hennig and Dallas Trinkle guided me during the introductory phases of this study, and dis- cussions with them over the years provided useful insights that improved the quality of this work. Many other people have helped me either professionally or personally and de- serve recognition. I thank my family, Jonathan Pelz, Nandini Trivedi, Michael Mills, Sheikh Akbar, Trisch Longbrake, Alisha Bruderly, Amita Wadhera, James Davis, Cheasequah Blevins, Robert Guidry, Sheldon Bailey, Julia Young, Geoffrey Smith, Leslie Smith, Alex Yuffa, Bruce Hinds, Marissa Hinds, Kevin Driver, William Parker, Lena Osborne, Adam Hauser, Justin Link, Bill Schneider, Russell Peck, Charles Place, Rakesh Tiwari, Mehul Dixit, John Draskovic, Grayson Williams, James Stapleton, Veronica Stapleton, Greg Viera, Catherine Sundt, Patrick Smith, Nicholas Harmon, David Massey, Reni Ayachitula, Mike Hinton, Michael Boss, Greg Sollenberger, Kevin Knobbe, Ty Nelson, Kevin Troudt, Kirk Troudt, Jeff Stevens, Kerry Highbarger, Re- becca Daskalova, Alex Daskalova, and Jake Livesay. iii I was supported for two years at Ohio State as a Fowler fellow, and by the United States Department of Energy the rest of the time. Computing resources were provided by the Ohio Supercomputing Center and the National Energy Research Scientific Computing Center. iv Vita June 20, 1980 ...............................Born–Brighton, Colorado, USA 1998–2002 ..................................Undergraduate Student, Colorado School of Mines, Golden, Colorado 2002–2004 ..................................Master’s Student, Colorado School of Mines, Golden, Colorado 2004–2006 ..................................Fowler Fellow, Department of Physics, The Ohio State University, Columbus, Ohio 2006–present ...............................Graduate Research Associate, Depart- ment of Physics, The Ohio State Uni- versity, Columbus, Ohio Publications Research Publications M. T. Lusk, M. R. Fellinger, and P. D. Beale, Grain-Boundary Free Energy Via Thermodynamic Integration, J. Chem. Phys., 124:064707, 2006. M. R. Fellinger, H. Park, and J. W. Wilkins, Force-Matched Embedded-Atom Method Potential for Niobium, Phys. Rev. B, 81:144119, 2010. H. Park, M. R. Fellinger, T. J. Lenosky, W. W. Tipton, D. R. Trinkle, S. P. Rudin, C. Woodward, J. W. Wilkins, and R. G. Hennig, Ab Initio Based Empirical Potential Used to Study the Mechanical Properties of Molybdenum, Phys. Rev. B, 85:214121, 2012. v Fields of Study Major Field: Physics vi Table of Contents Page Abstract....................................... ii Acknowledgments.................................. iii Vita......................................... v ListofTables.................................... x ListofFigures ................................... xvii 1. Introduction.................................. 1 1.1 Interatomic Potentials for Metals . 1 1.2 Body-Centered Cubic Refractory Metals . 3 1.3 Scope .................................. 4 2. Classical Interatomic Potentials . 6 2.1 Justification for Classical Potentials . 8 2.1.1 Born-Oppenheimer Approximation . 8 2.1.2 Classical Nuclei Approximation . 14 2.2 Classifications of Interatomic Potentials . 16 2.2.1 Pair Potentials . 19 2.2.2 Higher-Order Potentials . 20 2.3 Many-Body Potentials for Real Metals . 21 2.3.1 Embedded-Atom Method Potentials . 22 2.3.2 Modified Embedded-Atom Method Potentials . 25 vii 3. Generating and Testing Classical Potentials . 27 3.1 Cubic Spline-Based Interatomic Potentials . 29 3.2 AccurateFirst-PrinciplesFittingData . 33 3.2.1 Exchange-Correlation Functionals and Pseudopotentials . 36 3.2.2 Convergence Tests . 42 3.3 Tests for Interatomic Potentials . 48 3.3.1 EquationsofState ....................... 49 3.3.2 ElasticConstants........................ 51 3.3.3 Vibrational Frequencies . 61 3.3.4 ThermalExpansion ...................... 65 3.3.5 MeltingTemperature. 66 3.3.6 Point Defects . 67 3.3.7 SurfaceProperties . 71 3.3.8 Dislocations........................... 76 3.3.9 IdealShearStrength . 90 3.3.10 Generalized Stacking Faults . 93 4. Results and Applications of Classical Potentials . 99 4.1 Force-Matched EAM Potential for Nb . 104 4.2 Force-Matched MEAM Potential for Mo . 121 4.3 Application of the Nb EAM Potential to Shock Simulations . 130 4.4 Potentials for High-Pressure Applications . 135 4.4.1 High-Pressure MEAM Potential for Nb . 137 4.4.2 High-Pressure MEAM Potential for Mo . 145 4.4.3 High-Pressure MEAM Potential for W . 153 4.4.4 High-Pressure MEAM Potential for V . 161 4.4.5 High-Pressure MEAM Potential for Ta . 166 5. Conclusion................................... 177 5.1 SummaryofResults .......................... 177 5.2 Limitations and Possible Extensions of This Work . 179 Appendices 181 A. Convergence Parameters for DFT Calculations . 181 A.1 Plane-Wave Cutoff Energy Ecut Convergence . 181 A.2 k-PointConvergence . 184 viii A.3 FermiSurfaceSmearing . 190 B. Optimized Spline Knots for EAM and MEAM Potentials . 196 B.1 NbEAMPotential ........................... 196 B.2 MoMEAMPotential.......................... 197 Bibliography .................................... 200 ix List of Tables Table Page 3.1 Comparison of calculated lattice constant a, bulk modulus B, and elas- tic constants C′ = (C C )/2 and C of Nb to experimental val- 11 − 12 44 ues. The calculations are performed using vasp with different choices of exchange-correlation (XC) functionals and pseudopotentials (PP). LDA is the local density approximation, PW91 and PBE are two dif- ferent versions of generalized gradient approximations (GGAs), US is an ultra-soft pseudopotential, and PAW is a projector-augmented wave pseudopotential. Pseudopotentials labeled pv treat the 4p-semicore states as valence states, and pseudopotentials labeled sv treat the 4p- and 4s-semicore states as valence states. The PBE functional combined with the PAW-sv pseudopotential produces the best overall agreement withexperiment. ............................. 42 3.2 Convergence parameters used for DFT calculations for the bcc refrac- tory metals. The first column specifies the metal, the second column is the plane-wave energy cutoff used to determine the number of plane- wave basis functions, the third column gives the grid of k-points, and the fourth column is the Fermi surface smearing parameter. All the cal- culations use the PBE GGA exchange-correlation functional and PAW pseudopotentials. The pseudopotentials for V and Nb treat the highest s- and p-semicore states as valence states, and the pseudopotentials for Ta, Mo, and W treat the highest p-semicore states as valence states. 48 3.3 Possible values for the indices of Cijkl. The elastic constants obey the relation Cijkl = Cjikl = Cijlk = Cklij. This limits the values of ij to six possible choices. The table list the possible values of kl for each choice of ij. The total number of possibilities is 6 + 5 + 4 + 3 + 2 + 1 = 21. Thus, there are at most 21 independent values of Cijkl. ........ 56 x 3.4 Voigt notation for stress-strain variables. The six possible pairs of values taken by ij or kl are replaced by six single values taken by α or β. In Voigt notation C C , σ σ , ǫ ǫ , and ǫ ǫ /2 for ijkl ≡ αβ ij ≡ α ii ≡ α ij ≡ α i = j..................................... 57 6 4.1 Configurations in the DFT database used to construct the EAM po- tential for Nb [1]. The “Structure” column lists the crystal structure of each configuration. The “primitive” and “conventional”
Recommended publications
  • A Survey of Some Empirical and Semiempirical Interatomic And

    A Survey of Some Empirical and Semiempirical Interatomic And

    ui avaiiuai'ua , iuxicu. DUi;au rcererence door; noTto Library, N.W. Bldg D8 taken fr NBS TECHNICAL 246 A Survey of Some Empirical and Semi-Empirical Interatomic SI and Intermolecular Potentials i§ BENJAMIN M. AXILROD or KtHt /T \ U.S. DEPARTMENT OF COMMERCE >rV z *& National Bureau of Standards o \ ^CAU Of * IS — THE NATIONAL BUREAU OF STANDARDS The National Bureau of Standards 1 provides measurement and technical information services essential to the efficiency and effectiveness of the work of the Nation's scientists and engineers. The Bureau serves also as a focal point in the Federal Government for assuring maximum application of the physical and engineering sciences to the advancement of technology in industry and commerce. To accomplish this mission, the Bureau is organized into three institutes covering broad program areas of research and services: THE INSTITUTE FOR BASIC STANDARDS . provides the central basis within the United States for a complete and consistent system of physical measurements, coordinates that system with the measurement systems of other nations, and furnishes essential services leading to accurate and uniform physical measurements throughout the Nation's scientific community, industry, and commerce. This Institute comprises a series of divisions, each serving a classical subject matter area: —Applied Mathematics—Electricity—Metrology—Mechanics —Heat—Atomic Physics—Physical Chemistry—Radiation Physics—Laboratory Astrophysics 2—Radio Standards Laboratory, 2 which includes Radio Standards Physics and Radio Standards Engineering—Office of Standard Refer- ence Data. THE INSTITUTE FOR MATERIALS RESEARCH . conducts materials research and provides associated materials services including mainly reference materials and data on the properties of ma- terials.
  • Interatomic Potentials

    Interatomic Potentials

    Interatomic Potentials Dorothy Duffy October 2020 1 Introduction Interatomic potentials, also commonly referred to as forcefields, are widely used in the materials modelling community for simulating processes and calculating structural properties. They have been employed for several decades in a range of modelling methods, including molecular dynamics, Monte Carlo and, more recently, in rare event methods, such umbrella sampling and metadynamics, discussed in previous lectures of this course. The primary reasons for the popularity and success of methods employing in- teratomic potentials are their computational efficiency. Simulations of hundreds of millions of atoms are now commonplace and molecular dynamics timescales of tens of nanoseconds, or even microseconds, are achievable on high perfor- mance computing platforms. Extending simulation length and time scales is a universal aim of materials modellers, as they endeavor to close the gap between modelling and experiment. The main disadvantage with employing interatomic potentials is, of course, that the results are sensitive to the model. While this is true to some extent for density functional theory calculations, the sensitivity to the model is much stronger in interatomic potential methods. A second significant limitation is that the methods provide no information about electronic structure, therefore calculations of electronic properties, such as band gaps, are inaccessible. Nev- ertheless, carefully parameterised potentials are an invaluable tool for exploring time and length scale
  • Unifying Interatomic Potential, G (R), Elasticity, Viscosity, and Fragility of Metallic Glasses: Analytical Model, Simulations, and Experiments

    Unifying Interatomic Potential, G (R), Elasticity, Viscosity, and Fragility of Metallic Glasses: Analytical Model, Simulations, and Experiments

    View metadata, citation and similar papers at core.ac.uk brought to you by CORE provided by Apollo Home Search Collections Journals About Contact us My IOPscience Unifying interatomic potential, g (r), elasticity, viscosity, and fragility of metallic glasses: analytical model, simulations, and experiments This content has been downloaded from IOPscience. Please scroll down to see the full text. J. Stat. Mech. (2016) 084001 (http://iopscience.iop.org/1742-5468/2016/8/084001) View the table of contents for this issue, or go to the journal homepage for more Download details: IP Address: 131.111.184.102 This content was downloaded on 02/11/2016 at 17:59 Please note that terms and conditions apply. You may also be interested in: Relaxation and physical aging in network glasses: a review Matthieu Micoulaut Computer simulations of glasses: the potential energy landscape Zamaan Raza, Björn Alling and Igor A Abrikosov Length scales in glass-forming liquids and related systems: a review Smarajit Karmakar, Chandan Dasgupta and Srikanth Sastry Dynamical and structural signatures of the glass transition in emulsions Chi Zhang, Nicoletta Gnan, Thomas G Mason et al. Localization model description of diffusion and structural relaxation in glass-forming Cu–Zr alloys Jack F Douglas, Beatriz A Pazmino Betancourt, Xuhang Tong et al. Models of the glass transition J Jackle Exploring the potential energy landscape of glass-forming systems: from inherent structuresvia metabasins to macroscopic transport Andreas Heuer IOP Journal of Statistical Mechanics: Theory and Experiment J. Stat. Mech. 2016 ournal of Statistical Mechanics: Theory and Experiment 2016 J © 2016 IOP Publishing Ltd and SISSA Medialab srl Special Issue on Structure in Glassy and Jammed Systems JSMTC6 Unifying interatomic potential, g r , 084001 ( ) elasticity, viscosity, and fragility of A E Lagogianni et al metallic glasses: analytical model, Mech.
  • Machine Learning a General-Purpose Interatomic Potential for Silicon

    Machine Learning a General-Purpose Interatomic Potential for Silicon

    PHYSICAL REVIEW X 8, 041048 (2018) Machine Learning a General-Purpose Interatomic Potential for Silicon Albert P. Bartók Scientific Computing Department, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Didcot, OX11 0QX, United Kingdom James Kermode Warwick Centre for Predictive Modelling, School of Engineering, University of Warwick, Coventry, CV4 7AL, United Kingdom Noam Bernstein Center for Materials Physics and Technology, U.S. Naval Research Laboratory, Washington, D.C. 20375, USA Gábor Csányi Engineering Laboratory, University of Cambridge, Trumpington Street, Cambridge, CB2 1PZ, United Kingdom (Received 26 May 2018; revised manuscript received 11 October 2018; published 14 December 2018) The success of first-principles electronic-structure calculation for predictive modeling in chemistry, solid-state physics, and materials science is constrained by the limitations on simulated length scales and timescales due to the computational cost and its scaling. Techniques based on machine-learning ideas for interpolating the Born-Oppenheimer potential energy surface without explicitly describing electrons have recently shown great promise, but accurately and efficiently fitting the physically relevant space of configurations remains a challenging goal. Here, we present a Gaussian approximation potential for silicon that achieves this milestone, accurately reproducing density-functional-theory reference results for a wide range of observable properties, including crystal, liquid, and amorphous bulk phases, as well as point, line, and plane defects. We demonstrate that this new potential enables calculations such as finite-temperature phase-boundary lines, self-diffusivity in the liquid, formation of the amorphous by slow quench, and dynamic brittle fracture, all of which are very expensive with a first-principles method. We show that the uncertainty quantification inherent to the Gaussian process regression framework gives a qualitative estimate of the potential’s accuracy for a given atomic configuration.
  • Simulations of the Structure and Properties of Amorphous Silica

    Simulations of the Structure and Properties of Amorphous Silica

    Chemical Engineering Science 56 (2001) 4205–4216 www.elsevier.com/locate/ces Simulations of the structure andproperties of amorphous silica surfaces Jeanette M. Stallons, Enrique Iglesia ∗ Department of Chemical Engineering, University of California at Berkeley, Berkeley, CA 94720, USA Received10 December 1999; accepted26 December 2000 Abstract The structure andtransport properties of solidsurfaces have been describedusingmodelsof varying complexity andrigor without systematic comparisons among available methods. Here, we describe the surface of amorphous silica using four techniques: (1) an orderedsurfacecreatedby cutting the structure of a known silica polymorph ( -cristobalite); (2) an unrelaxedamorphous surface obtainedby cutting bulk amorphous silica structures createdby molecular dynamicsmethods;(3) a relaxedamorphous surface createdby relaxing the amorphous surface; and(4) a randomsurface createdby Monte Carlo sphere packing methods. Calculations of the adsorption potential surface and simulation of the surface di4usion of weakly bound adsorbates (N2, Ar, CH4) interacting via Lennard–Jones potentials with these surfaces were used to compare surface models and to judge their ÿdelity by comparisons with available experimental values. Similar heats of adsorption were obtained on the relaxed, unrelaxed, and random surfaces (±0:5kJ=mol), but the relaxed surface showed greater heterogeneity with a wider distribution of adsorption energies. Surface di4usion on the relaxed surface was slower than on the other surfaces, with slightly higher activation energies (0:5–1:0kJ=mol). Rigorous comparisons between simulatedandexperimental surface di4usivitiesare not possible, because of scarce surface di4usion data on well-characterized surfaces. The values obtained from simulations on silica were similar to experimental surface di4usivities reported on borosilicate glasses. ? 2001 Publishedby Elsevier Science Ltd. Keywords: Porous media; Simulation; Transport processes; Di4usion; Surface di4usion; Adsorption 1.
  • Disentangling Interatomic Repulsion and Anharmonicity in the Viscosity and Fragility of Glasses

    Disentangling Interatomic Repulsion and Anharmonicity in the Viscosity and Fragility of Glasses

    Disentangling interatomic repulsion and anharmonicity in the viscosity and fragility of glasses J. Krausser,1 A. E. Lagogianni,2 K. Samwer,2 and A. Zaccone1, 3 1Statistical Physics Group, Department of Chemical Engineering and Biotechnology, University of Cambridge, New Museums Site, Pembroke Street, CB2 3RA Cambridge, U.K. 2I. Physikalisches Institut, Universit¨atG¨ottingen, Friedrich-Hund-Platz 1, 37077 G¨ottingen,Germany 3Cavendish Laboratory, University of Cambridge, CB3 0HE Cambridge, U.K. (Dated: February 22, 2017) Within the shoving model of the glass transition, the relaxation time and the viscosity are related to the local cage rigidity. This approach can be extended down to the atomic-level in terms of the interatomic interaction, or potential of mean-force. We applied this approach to both real metallic glass-formers and model Lennard-Jones glasses. The main outcome of this analysis is that in metallic glasses the thermal expansion contribution is mostly independent of composition and is uncorrelated with the interatomic repulsion: as a consequence, the fragility increases upon increasing the interatomic repulsion steepness. In the Lennard-Jones glasses, the scenario is opposite: thermal expansion and interatomic repulsion contributions are strongly correlated, and the fragility decreases upon increasing the repulsion steepness. This framework allows one to tell apart systems where "soft atoms make strong glasses" from those where, instead, "soft atoms make fragile glasses". Hence, it opens up the way for the rational, atomistic tuning of the fragility and viscosity of widely different glass-forming materials all the way from strong to fragile. I. INTRODUCTION fundamental observation in terms of the underlying microstructure, dynamics and interaction picture.
  • Development of Interatomic Potentials in the Tersoff-Albe Formalism For

    Development of Interatomic Potentials in the Tersoff-Albe Formalism For

    View metadata, citation and similar papers at core.ac.uk brought to you by CORE provided by Helsingin yliopiston digitaalinen arkisto M.Sc. thesis Computational physics Development of interatomic potentials in the Tersoff-Albe formalism for metal compounds Jesper Byggmästar 2016 Supervisors: Morten Nagel Krister Henriksson Examiners: Krister Henriksson Kai Nordlund UNIVERSITY OF HELSINKI DEPARTMENT OF PHYSICS PL 64 (Gustaf Hällströmin katu 2) 00014 Helsingin yliopisto HELSINGIN YLIOPISTO | HELSINGFORS UNIVERSITET | UNIVERSITY OF HELSINKI Tiedekunta/Osasto | Fakultet/Sektion | Faculty Laitos | Institution | Department Faculty of Science Department of Physics Tekij¨a | F¨orfattare | Author Jesper Byggm¨astar Ty¨on nimi | Arbetets titel | Title Development of interatomic potentials in the Tersoff-Albe formalism for metal compounds Oppiaine | L¨aro¨amne | Subject Fysik Ty¨on laji | Arbetets art | Level Aika | Datum | Month and year Sivum¨a¨ar¨a | Sidoantal | Number of pages M.Sc. 08/2016 57 Tiivistelm¨a | Referat | Abstract Interatomic potentials are used to describe the motion of the individual atoms in atomistic simula- tions. An accurate treatment of the interatomic forces in a system of atoms requires heavy quantum mechanical calculations, which are not computationally feasible in large-scale simulations. Intera- tomic potentials are computationally more efficient analytical functions used for calculating the potential energy of a system of atoms, allowing simulations of larger systems or longer time scales than in quantum mechanical simulations. The interatomic potential functions must be fitted to known properties of the material the poten- tial describes. Developing a potential for a specific material typically involves fitting a number of parameters included in the functional form, against a database of important material properties, such as cohesive, structural, and elastic properties of the relevant crystal structures.
  • Development of Embedded Atom Method Interatomic Potentials for Ge-Sn-Si Ternary and Constituent Binary Alloys for Modeling Material Crystallization

    Development of Embedded Atom Method Interatomic Potentials for Ge-Sn-Si Ternary and Constituent Binary Alloys for Modeling Material Crystallization

    DEVELOPMENT OF EMBEDDED ATOM METHOD INTERATOMIC POTENTIALS FOR GE-SN-SI TERNARY AND CONSTITUENT BINARY ALLOYS FOR MODELING MATERIAL CRYSTALLIZATION A thesis submitted in partial fulfillment of the requirements for the degree of Master of Science By SUDIP ACHARYA B.S., Tribhuvan University, Nepal, 2017 2020 Wright State University WRIGHT STATE UNIVERSITY GRADUATE SCHOOL July 30, 2020 I HEREBY RECOMMEND THAT THE THESIS PREPARED UNDER MY SUPERVISION BY Sudip Acharya ENTITLED “Development of Embedded Atom Method Interatomic Potentials for Ge-Sn-Si Ternary and Constituent Binary Alloys for Modeling Material Crystallization” BE ACCEPTED IMPARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF Master of Science. _________________________________ Amit Sharma, Ph. D. Thesis Advisor _________________________________ Jason Deibel, Ph.D. Chair, Department of Physics Final Examination Committee _________________________________ Amit Sharma, Ph. D. _________________________________ Brent D. Foy, Ph. D. _________________________________ Sarah F. Tebbens, Ph. D. __________________________________ Barry Milligan, Ph. D. Interim Dean of the Graduate School Abstract Acharya, Sudip. M.S. Department of Physics, Wright State University, 2020. Development of Embedded Atom Method Interatomic Potentials for Ge-Sn-Si Ternary and Constituent Binary Alloys for Modeling Material Crystallization. Group IV elements based nanoelectronics devices (mainly Si and Ge based devices) have been developed and improved over a long period of time and are the most influencing
  • Hybrid Bond-Order Potential for Silicon Suleiman Oloriegbe Clemson University, Solorie@Clemson.Edu

    Hybrid Bond-Order Potential for Silicon Suleiman Oloriegbe Clemson University, [email protected]

    Clemson University TigerPrints All Dissertations Dissertations 12-2008 Hybrid Bond-Order Potential for Silicon Suleiman Oloriegbe Clemson University, [email protected] Follow this and additional works at: https://tigerprints.clemson.edu/all_dissertations Part of the Physical Chemistry Commons Recommended Citation Oloriegbe, Suleiman, "Hybrid Bond-Order Potential for Silicon" (2008). All Dissertations. 328. https://tigerprints.clemson.edu/all_dissertations/328 This Dissertation is brought to you for free and open access by the Dissertations at TigerPrints. It has been accepted for inclusion in All Dissertations by an authorized administrator of TigerPrints. For more information, please contact [email protected]. HYBRID BOND-ORDER POTENTIAL FOR SILICON _____________________________________ A Dissertation Presented to the Graduate School of Clemson University ___________________________________ In Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy Chemistry _____________________________________ by Suleiman Yahaya Oloriegbe December 2008 _____________________________________ Accepted by: Dr. Steven J. Stuart, Committee Chair Dr. Brian Dominy Dr. Jason McNeill Dr. Robert Latour ABSTRACT A new hybrid bond-order potential for silicon is developed. The functional form of the potential is derived from hybrid of expressions from empirical bond-order formalism and first principles approximations. The total energy is expressed as the sum of attractive, repulsive and promotion energies. By introducing a screening function derived from approximations to first principles expressions, the potential is made long-ranged by allowing covalent interactions beyond the first nearest neighbor shell of atoms in agreement with quantum mechanical descriptions of the bonding in silicon. Environment- dependent promotion energy is introduced that accurately accounts for energetic interactions due to changes in hybridization state of atoms during chemical bonding.
  • Bond Order Potentials for Covalent Elements

    Bond Order Potentials for Covalent Elements

    Bond order potentials for covalent elements. This chapter will be dedicated to a short history of the so called \bond order" potentials [1, 2, 3, 4, 5, 6, 7] (BOPs), that represent an interesting class of the rather scattered family of analytic potentials. Analytic interatomic potentials (sometimes referred to as empirical, semi-empirical or clas- sical potentials) are used for a variety of purposes, ranging from the estimation of minimum energy structures for surface reconstruction, grain boundaries or related defects, to the descrip- tion of the liquid structure. All analytic potentials are de¯ned through a functional form of the interatomic interactions, whose parameters are ¯tted to a selected database. According to Brenner [8], an analytic potential needs to be: ² Flexible: the function should be flexible enough to accommodate the inclusion of a relatively wide range of structures in a ¯tting database. ² Accurate: the potential function must be able to accurately reproduce quantities such energies, bond lengths, elastic constant, and related properties entering a ¯tting database. ² Transferable: the functional form of the potential should be able to reproduce related prop- erties that are not included in the ¯tting database. In practise the potential should be able to give a good description of the energy landscape for any possible realistic con¯guration characterized by the set of atomic positions frig. ² Computationally e±cient: the function should be of such a form that it is tractable for a desired calculation, given the available computing resources. We note that one of the paradigms that has led science through its development, i.e. the Occam razor (\Entities should not be multiplied beyond necessity"), is not mentioned here.
  • Atomic-Scale Expressions for Viscosity and Fragile-Strong Behavior in Metal Alloys Based on the Zwanzig-Mountain Formula

    Atomic-Scale Expressions for Viscosity and Fragile-Strong Behavior in Metal Alloys Based on the Zwanzig-Mountain Formula

    PHYSICAL REVIEW RESEARCH 2, 033134 (2020) Atomic-scale expressions for viscosity and fragile-strong behavior in metal alloys based on the Zwanzig-Mountain formula G. Chevallard,1 K. Samwer,2 and A. Zaccone 1,3 1Department of Physics “A. Pontremoli,” University of Milan, via Celoria 16, 20133 Milan, Italy 2I. Physikalisches Institut, Universität Göttingen, D-37077 Göttingen, Germany 3Department of Chemical Engineering and Biotechnology, University of Cambridge, Cambridge CB3 0AS, United Kingdom (Received 12 May 2020; revised 23 June 2020; accepted 30 June 2020; published 24 July 2020) We combine the shoving model of T -dependent viscosity of supercooled liquids with the Zwanzig-Mountain formula for the high-frequency shear modulus using the g(r) of molecular dynamics simulations of metal alloys as the input. This scheme leads to a semianalytical expression for the viscosity as a function of temperature, which provides a three-parameter model fitting of experimental data of viscosity for the same alloy for which g(r) was calculated. The model provides direct access to the influence of atomic-scale physical quantities such as the interatomic potential φ(r) on the viscosity and fragile-strong behavior. In particular, it is established that a steeper interatomic repulsion leads to fragile liquids, or, conversely, that “soft atoms make strong liquids.” DOI: 10.1103/PhysRevResearch.2.033134 I. INTRODUCTION the activation energy is expressed via the product of the high-frequency shear modulus of the liquid and an activation Different views of the glass transition have led to quite volume, which follows from the analysis of the work done by different descriptions of the viscosity of supercooled liquids.
  • Two-Body Interatomic Potentials for He, Ne, Ar, Kr, and Xe from Ab Initio Data

    Two-Body Interatomic Potentials for He, Ne, Ar, Kr, and Xe from Ab Initio Data

    Two-Body Interatomic Potentials for He, Ne, Ar, Kr and Xe from Ab Initio Data U. K. Deiters Institut für Physikalische Chemie, University of Cologne, Luxemburger Str. 116, D-50939 Köln, Germany Richard J. Sadusa Centre for Computational Innovations, Swinburne University of Technology, PO Box 218, Hawthorn, Victoria 3122, Australia Abstract A new method is reported for developing accurate two-body interatomic potentials from existing ab initio data. The method avoids the computational complexity of alternative methods without sacrificing accuracy. Two-body potentials are developed for He, Ne, Ar, Kr and Xe, which accurately reproduce the potential energy at all inter-atomic separations. Monte Carlo simulations of the pressure, radial distribution function and isochoric heat capacity using the simplified potential indicate that the results are in very close, and sometimes almost indistinguishable, agreement with more complicated current state-of-the-art two-body potentials. a Author for correspondence, email: [email protected]. 1 I. INTRODUCTION The macroscopic properties of materials, irrespective of whether in the liquid, gas or solid state, are ultimately determined by the nature of interactions between their constituent atoms or molecules.1 In most instances, the dominant contribution from such interatomic or intermolecular interactions can be attributed to the sum of interactions between all of the different pairs of atoms or molecules, i.e. two-body interactions. Although it is well-documented2-4 that the addition of three– or more-body interactions are required for an accurate representation of the properties of materials, the dominance of two-body interactions means that understanding such interactions is of paramount importance.