A Multi-method Atomistic Study of Protective Nitride Coatings: from Crystalline to Amorphous Materials
Research output: Thesis › Doctoral Thesis
Standard
2023.
Research output: Thesis › Doctoral Thesis
Harvard
APA
Vancouver
Author
Bibtex - Download
}
RIS (suitable for import to EndNote) - Download
TY - BOOK
T1 - A Multi-method Atomistic Study of Protective Nitride Coatings: from Crystalline to Amorphous Materials
AU - Nayak, Ganesh Kumar
N1 - no embargo
PY - 2023
Y1 - 2023
N2 - Diffusion plays an important role in the properties of solids, which governs the kinetics of microstructural changes and processes of mass transport. The diffusional phenomena are most widespread in metals, alloys, and metastable and chemically complex solid solutions, mainly at elevated temperatures. For instance, the kinetics in metastable phases, such as oxidation, mixing, intermixing, thermal decompositions, and phase formation, are attributed to the diffusional rearrangement of atoms. Atomistic simulations have provided unprecedented insight into various material properties, with ab initio calculations, in particular, being highly successful in raising the level of understanding close to that of experimental observations. However, diffusion dynamics have been challenging due to the time scale limitation of ab initio molecular dynamics for the infrequent event of jump processes. In contrast, the nudged elastic band method (NEB) based on the transition state theory (TST) can be employed to overcome this shortcoming. This method can calculate the 0 K migration energy barrier of a diffusion process from a static density functional theory (DFT) calculation and the finite temperature diffusion quantities by considering the free energy contribution from phonon. However, the model of an amorphous system, considering the size limitation of ab initio methods to a few hundred atoms, is not large enough to represent real materials. Hence, one needs to consider the large-scale atomistic simulations to predict the properties accurately. In the present thesis, we present the mass transport-related phenomena in B1 nitride coatings using the diffusion migration barriers by the 0 K NEB calculations. In part of the thesis, we use phonon thermodynamics to extend the 0 K calculations to quantify the diffusion of the finite temperatures and pressures (pre-exponential coefficients and activation energies). Further, we train a machine learning interatomic potential (MLIP) and use it in large-scale molecular dynamics to study the structural and elastic properties of amorphous silicon nitrides. Many chemical environments in B1 nitride solid solutions provide a different value of vacancy formation energy and migration energy barriers, namely an "envelope". We use the envelope method to predict phase formation in ternary nitrides. Furthermore, we establish a relation between lattice distortion and sluggish diffusion in high-entropy nitrides (HEN) using the envelope methods.
AB - Diffusion plays an important role in the properties of solids, which governs the kinetics of microstructural changes and processes of mass transport. The diffusional phenomena are most widespread in metals, alloys, and metastable and chemically complex solid solutions, mainly at elevated temperatures. For instance, the kinetics in metastable phases, such as oxidation, mixing, intermixing, thermal decompositions, and phase formation, are attributed to the diffusional rearrangement of atoms. Atomistic simulations have provided unprecedented insight into various material properties, with ab initio calculations, in particular, being highly successful in raising the level of understanding close to that of experimental observations. However, diffusion dynamics have been challenging due to the time scale limitation of ab initio molecular dynamics for the infrequent event of jump processes. In contrast, the nudged elastic band method (NEB) based on the transition state theory (TST) can be employed to overcome this shortcoming. This method can calculate the 0 K migration energy barrier of a diffusion process from a static density functional theory (DFT) calculation and the finite temperature diffusion quantities by considering the free energy contribution from phonon. However, the model of an amorphous system, considering the size limitation of ab initio methods to a few hundred atoms, is not large enough to represent real materials. Hence, one needs to consider the large-scale atomistic simulations to predict the properties accurately. In the present thesis, we present the mass transport-related phenomena in B1 nitride coatings using the diffusion migration barriers by the 0 K NEB calculations. In part of the thesis, we use phonon thermodynamics to extend the 0 K calculations to quantify the diffusion of the finite temperatures and pressures (pre-exponential coefficients and activation energies). Further, we train a machine learning interatomic potential (MLIP) and use it in large-scale molecular dynamics to study the structural and elastic properties of amorphous silicon nitrides. Many chemical environments in B1 nitride solid solutions provide a different value of vacancy formation energy and migration energy barriers, namely an "envelope". We use the envelope method to predict phase formation in ternary nitrides. Furthermore, we establish a relation between lattice distortion and sluggish diffusion in high-entropy nitrides (HEN) using the envelope methods.
KW - first-principle calculation
KW - density function theory
KW - ab initio molecular dynamics
KW - classical molecular dynamics
KW - machine learning interatomic potential
KW - wear protection
KW - nitride protective coatings
KW - B1 nitrides
KW - amorphous nitrides
KW - chemical complex nitrides
KW - high-entropy nitrides
KW - nitride solid solutions
KW - solid lubricant protective coatings
KW - vanadium aluminium nitrides
KW - titanium aluminium nitrides
KW - titanium nitrides
KW - titanium silicon nitrides
KW - silicon nitrides
KW - sluggish diffusion
KW - lattice distortion
KW - diffusion
KW - lattice diffusion
KW - vacancy formation energy
KW - migration energy barriers
KW - migration free energy
KW - phonons
KW - thermodynamics
KW - linear thermal expansion
KW - nudged elastic band
KW - alloying
KW - d-element impurities
KW - enthalpy of formation
KW - activation energy
KW - elastic properties
KW - temperature-dependent elastic properties
KW - crystal orbital Hamilton population
KW - bonding
KW - anti-bonding
KW - First-Principle-Berechnung
KW - Dichtefunktionaltheorie
KW - Ab initio Molekulardynamik
KW - Klassische Molekulardynamik
KW - Maschinell gelernte interatomare Potenziale
KW - Verschleißschutz
KW - Nitridische Schutzschichten
KW - B1-Nitride
KW - Amorphe Nitride
KW - Chemisch komplexe Nitride
KW - Hochentropie-Nitride
KW - Nitrid-Mischkristalle
KW - Festschmierstoff-Schutzbeschichtung
KW - Vanadiumsluminium-Nitride
KW - Titanaluminiumnitride
KW - Titansiliziumnitride
KW - Siliziumnitride
KW - Träge Diffusion
KW - Gitterverzerrung
KW - Diffusion
KW - Gitterdiffusion
KW - Leerstellenbildungsenergie
KW - Migrationsenergiebarrieren
KW - freie Migrationsenergien
KW - Phononen
KW - Thermodynamik
KW - Lineare thermische Expansion
KW - Nudged-Elastic-Band-Methode
KW - Legieren
KW - D-Element Verunreinigungen
KW - Bildungsenthalpie
KW - Aktivierungsenergie
KW - Elastische Eigenschaften
KW - Temperaturabhängige elastische Eigenschaften
KW - Crystal Orbital Hamilton Population
KW - Bindungen
KW - Anti-Bindungen
U2 - 10.34901/mul.pub.2023.286
DO - 10.34901/mul.pub.2023.286
M3 - Doctoral Thesis
ER -