traditional vs. ab initio modeling · experimental data analysis predictions simulations...
TRANSCRIPT
![Page 1: Traditional vs. ab initio modeling · Experimental data Analysis Predictions Simulations Microscopic parameters Quantum mechanical calculations Validation Traditional vs. ab initio](https://reader030.vdocuments.us/reader030/viewer/2022013020/5e8d492d76fd7026186e23f3/html5/thumbnails/1.jpg)
Experimental data
Analysis
Predictions
Simulations
Microscopic parameters
Quantum mechanical calculations
Validation
Traditional vs. ab initio modeling
First-principles (or ab initio) calculations based on
Density Functional Theory (DFT).
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Microscopic parametersgoverning materials properties
Example: nucleation and growth of precipitate
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Outline
• Example of ab initio calculations• Why ab initio Thermodynamics?• Methods• Applications
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Self-Assembling Ge/Si(001) Quantum Dots
Goal: quantify thestrain-dependence of
the parameters governingGe adatom diffusion
Related works: Roland and Gilmer (1992), Spjut and Faux (1994), Schroeder and Wolf (1997),Ratsch et al. (1997), Zoethout et al. (2000), Shu et al. (2001), Penev et al. (2001).
Si (001) substrate
Ge wetting layerGe quantum dot
Ge
Strain field(Medeiros-Ribeiro, et al., 1998)
adatom
(top view)
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Unwanted Coarsening
• Thermodynamic effect
• Kinetic effect (?)
Lower surface/volume(capillarity)
µ
DHigher adatom mobility
(Lower barrier foradatom attachement)e.g. Koduvely and Zangwill (1999)
Larger island:
Near Larger island:
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Saddle pointBinding site
Ge Adatom Diffusion on Ge (001)
Ge (001) Surface c(4x2) Reconstruction
Schematic top viewisoelectronic density plot 3D schematic
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0 % strain = Si lattice param. 4 % strain = Ge lattice param.
Strain dependence
Diffusion-driven kinetic coarsening
Binding Site (Eb) Saddle point (Ea+Eb ) Activation barrier (Ea)
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Magnitude of the effect
0.038Si2/Si(001)Zoethout et al. (2000)
0.007-0.028Ag/Ag(111)Ratsch et al. (1997)
-0.023Si/Si(001)Roland et al. (1992)
-0.0220.002Ge/Si(001)PresentGe/Ge(001)/Si
Si/Si(001)
In/GaAs(001)
Systemadatom/subst.
-0.1280.212Present
-0.050Shu et al. (2001)
-0.020-0.050Penev et al. (2001)
dEa/de(eV/%)
dEb/de(eV/%)
Reference
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The “Virtual” Laboratory
Advantages
• Absolute control over “experimental’’ conditions• Unlimited “characterization’’ capabilities• Ability to perform thought experiments • Automation of repetitive tasks• “Materials by design”
• Limited by computational resources• Cannot predict effects not included in simulation
Weaknesses
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Outline
• Example of ab initio calculations• Why ab initio Thermodynamics?• Methods• Applications
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From a virtual to a real material...Useless material
Wonderful compound
We need a way to predict phase stability:
First-principles phase diagram calculations
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Outline
• Example of ab initio calculations• Why ab initio Thermodynamics?• Methods• Applications
![Page 13: Traditional vs. ab initio modeling · Experimental data Analysis Predictions Simulations Microscopic parameters Quantum mechanical calculations Validation Traditional vs. ab initio](https://reader030.vdocuments.us/reader030/viewer/2022013020/5e8d492d76fd7026186e23f3/html5/thumbnails/13.jpg)
Thermodynamic data
Quantum Mechanical Calculations
Lattice model &Monte Carlo Simulations
Electronic excitationsLattice vibrations
•Large number of atoms•Many configurations
•Small number of atoms•Few configurations
First-principles Thermodynamic Calculations
http://cms.northwestern.edu/atat
Configurational disorder
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Thermodynamic data
Quantum Mechanical Calculations
Lattice model &Monte Carlo Simulations
Electronic excitationsLattice vibrationsConfigurational disorder
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The Cluster Expansion Formalism
Sanchez, Ducastelle and Gratias (1984)
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Coupled Sublattices MulticomponentCluster Expansion
Example: binary fcc sublattice withternary octahedral sites sublattice
Occupation variables: i 0, ,ni 1
E1 , ,n JSame basic form:
Sanchez, Ducastelle and Gratias (1984)Tepesch, Garbulski and Ceder (1995)
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Cluster expansion fit
Which structures andwhich clustersto include in the fit?
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Cross-validation
Example of polynomial fit:
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A matter of time...Ti
me
Human
Computer
1980 2005
Time needed to complete a given first-principles calculation
The procedure needs to be automated
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Automated Cluster Expansion Construction
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Application to Ti-Al AlloysSimple lattice input file
Simple ab initio code input file
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Ground States Search
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Thermodynamic data
Quantum Mechanical Calculations
Lattice model &Monte Carlo Simulations
Electronic excitationsLattice vibrationsConfigurational disorder
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Monte Carlo output:Free energies
Cao-MgO system Ti-Al system
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Calculated phase diagram
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Van de Walle, Asta and Ceder (2002),Murray (1987) (exp.) Many other examples…
hcp Ti
DO19Ti3Al
Likely source of the discrepancy:Vibrational entropy.
Fultz, Nagel, Antony, et al. (1993-1999)
Ceder, Garbulsky, van de Walle (1994-2002)
de Fontaine, Althoff, Morgan (1997-2000)
Zunger, Ozolins, Wolverton (1998-2001)
Temperature scale problem
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Thermodynamic data
Quantum Mechanical Calculations
Lattice model &Monte Carlo Simulations
Electronic excitationsLattice vibrationsConfigurational disorder
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The Cluster Expansion Formalism
E1, ,n
F1, ,n JT
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Coarse-Graining of the Free EnergyGraphically:
Formally: (Ceder (1993), Garbulski and Ceder (1994-1996))
F 1 ln i eEi 1 ln i eEi
1 ln eF
F 1 ln i eEiwhere
kBT1
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First-principles lattice dynamics
Least-squares fit toSpring model
First-principles data
ThermodynamicProperties
Phonon density of states
Computationallyintensive!
Direct force constant method(Wei and Chou (1992), Garbuski and Ceder (1994), among many others)
Must be done formany configurations!
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Transferable Force Constants
van de Walle and Ceder (2000,2002)
Relationship holds across different structures on the same lattice (here fcc is shown).
Chemical bond type andbond length:Good predictorof nearest-neighbor force constants(stretching and bending terms)
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Further tests...Wu, Ceder, van de Walle (2002)
Au-Au bonds
Pd-Pd bonds
Cu-Cu bonds
Cu-Pd bonds
Au-Pd bonds
Au-Cu bonds
Accuracy ~ 0.03 kB
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Length-Dependent TransferableForce Constants (LDTFC)
van de Walle and Ceder (2000,2002)
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Calculated Ti-Al Phase Diagram
Assessed Phase Diagram:I. Ohnuma et al., ActaMater. 48, 3113 (2000)
1st-Principles Calculations:van de Walle and Asta
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Ti-Al Thermodynamic Properties1st-Principles Calculations vs.
Measurements
-45
-40
-35
-30
-25
-20
-15
-10
-5
0
0 0.1 0.2 0.3 0.4 0.5Al Concentration
∆H
(kJ/
mol
e)
Calorimetry(Kubaschewski and Dench, 1955)
FLMTO-LDA
VASP-GGA
-30
-25
-20
-15
-10
-5
0
0 0.1 0.2 0.3 0.4
Al Concentration
∆G
(kJ/
mol
e)
α
α2
EMF Measurements(Samokhval et al., 1971)
Monte-CarloCalculations
Gibbs Free Energies (T=960 K)Heats of Formation
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Thermodynamic data
Quantum Mechanical Calculations
Lattice model &Monte Carlo Simulations
Electronic excitationsLattice vibrationsConfigurational disorder
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Electronic Excitations
F1, ,n JT
Electronic DOS
Finite-temperature DFT
Fermi-Dirac Distribution
012345678
-4 -2 0Energy (eV)
Den
sity
of S
tate
s
T-independent DOS and charge density
Electronic Free energy
Advantage: Get Felec “for free”
FelecT EelecT Eelec0 TSelecT
EelecT f,Tgd
SelecT kB f ,T ln f ,T 1 f ,T ln1 f,Tgd
g
f,T
Cluster expansion: Or: any other model of electronic entropy
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Outline
• Example of ab initio calculations• Why ab initio Thermodynamics?• Methods• Applications
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Ordering in the Cu-Li system?
Ordered Cu4Li phase also suggested by
Borgsttedt & Gumiński (1996),
Krauss, Mendelson, Gruen, et al. (1986),
Old & Trawena (1981).
Widely used assessments
do not include ordered phases
(Pelton (1986), Saunders (1998)).
Evidence from EMF measurements
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Calculated Thermodynamic datafor Cu-Li system
Tsimulation = 950 KTmeasurement = 885 K
2 adjustable parameters:Tsimulation + chemical potential of Li (liq)
bcc
fcc
B32
1st order transition
2nd order transition
Phase diagram Electromotive Force (EMF)
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Antiphase Boundary
Diffuse Antiphase Boundary
Creation of a plane with easy dislocation motion:Work softening
after passage of 1 dislocation after passage of 2 dislocations
after passage of 1 dislocation after passage of 2 dislocations
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Short-range order and diffuse antiphaseboundary energy calculations
Calculated diffuse X-ray scattering in Ti-Al hcp solid-solution
Energy cost of creating a diffuse anti-phase boundary in a Ti-Al hcp short-range ordered alloy by sliding k dislocations
Neeraj (2000)
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Phase Field Modeling of System
Zhu, Wang, Ardell, Zhou, Liu & Chen (2004)
L12 Ni3AlNi-rich fccsolid solution
Free energy:
Thermodynamic term “gradient energy” termphase fields
Input parameters needed: Bulk thermodynamic data, Kinetic coefficients,Interfacial free energy,Interface width
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Interface Width & CoalescenceIn phase field modeling:
Interface width usually a numerical parameter.
Can get correct behavior with a larger-than-physical width
except if modeling of coalescence required.
φ
x
φ
x
Wider Interface Increased coalescence
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Ni3Al/Ni (001)
Lattice model
Diffuse Coherent Interface
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Interfacial ThermodynamicsNi3Al/Ni (001) diffuse coherent interface
Interfacial free energy Interface width
Important input for mesoscale phase field simulations:
provides the “gradient energy” term
1 nm
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Search for new compounds
Hart, Blum, Walorski & Zunger, Nat. Mat. 4, 391 (2005)
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Search for new compounds in theAl-Mo-Ni system
E
AlNi
Al (fcc)
Mo (bcc)
Ni (fcc)
NiAl (B2)Ni3Al (L12)
Mo
plotted with MEDIT, INRIA-Rocquencourt.
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Ni
Predicted Nano-StructuredCompound
Al
MoAlMo2Ni2
1 nm
(fcc)
(bcc)
plotted with MEDIT, INRIA-Rocquencourt.
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x
y
Nanostructured Electrolyte(for fuel cell applications)
Superlattices
70000-atom simulation
Material: CexSm1-xOyVac2-y
Optimal composition
~25 nm
CexSm1-xOy
O
Interface
Forbidden composition
van de Walle & Ellis, Phys. Rev. Lett. 98, 266101 (2007)
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First-principles determination ofStructure-Property Relationships
Example: Configuration-strain coupling
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More Structure-Property Relationship!
Useful input for design and optimization of optoelectronic devices
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Interatomic Potential Constructionfrom Quantum-Mechanics
Radiation damage in nuclear fuel for advanced burner Reactors: modeling and experimental validation (PI: N. Jensen, UC Davis; Student: P. Tiwary)
E
d
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Calculated phase diagramsTi-Al
fcc + L12
T (K)
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Locating Phase Transitions andEquation of State (EOS) Calculations
T
P
solid
liquid
Ramalingam, Asta, van de Walle & Hoyt, Interface Sci., 10: 149, 2002
Phase coexistence method Free Energy Equalization
dPdT 1
THBHA
VBVA
T,P
G
Boundary tracing:
A B
V
P
T
Equation of state
PSAAP Center for the Predictive Modeling and Simulation of High Energy DensityDynamic Response of Materials (PI: M. Ortiz, Caltech).