Related papers: First-principles, atomistic thermodynamics for oxi…
Understanding of the complex behavior of particles at surfaces requires detailed knowledge of both macroscopic and microscopic processes that take place; also certain processes depend critically on temperature and gas pressure. To link…
Previous and present "academic" research aiming at atomic scale understanding is mainly concerned with the study of individual molecular processes possibly underlying materials science applications. Appealing properties of an individual…
The phase diagram of oxygen is investigated for pressures from 50 to 130~GPa and temperatures up 1200 K using first principles theory. A metallic molecular structure with the $P6_3/mmc$ symmetry ($\eta^{'}$ phase) is determined to be…
Using a first-principles parameterized lattice-gas Hamiltonian we study the adsorbate ordering behavior at atomic steps of a Pd(100) surface exposed to an oxygen environment. We identify a wide range of gas-phase conditions comprising near…
The possible formation of oxides or thin oxide films (surface oxides) on late transition metal surfaces is recently being recognized as an essential ingredient when aiming to understand catalytic oxidation reactions under technologically…
Microcanonical statistics can be well applied to non-extensive systems like nuclei, atomic clusters and systems at phase transitions of first order with inhomogeneous configurations like phase separation. No thermodynamic limit has to be…
In this study, an efficient first-principles approach for calculating the thermodynamic properties of mixed metal oxides at high temperatures is demonstrated. More precisely, this procedure combines density functional theory and harmonic…
Here we first develop the thermodynamics of microcanonical phase transitions of first and second order in systems which are thermodynamically stable in the sense of van Hove. We show how both kinds of phase transitions can unambiguously be…
First-principles molecular dynamics simulation based on a plane wave/pseudopotential implementation of density functional theory is adopted to investigate atomic scale energy transport for semiconductors (silicon and germanium). By imposing…
We employ a multiscale modeling approach to study the surface structure and composition of a Pd(100) model catalyst in reactive environments. Under gas phase conditions representative of technological CO oxidation (~1 atm, 300-600 K) we…
We investigate catalysis in the framework of elementary thermal operations, leveraging the distinct features of such operations to illuminate catalytic dynamics. As groundwork, we establish new technical tools that enhance the computability…
As an aid to the development of hydrogen separation membranes, we predict the temperature dependent phase diagrams using first principles calculations combined with thermodynamic principles. Our method models the phase diagram without…
We establish an analytical criterion for dynamical thermalization within harmonic systems, applicable to both classical and quantum models. Specifically, we prove that thermalization of various observables, such as particle energies in…
Understanding thermodynamics in liquids at the atomic level is challenging because of strong atomic interactions and lack of symmetry. Recent prior theoretical works have focused on describing heat capacity of liquids in terms of…
Using very long molecular dynamics simulation runs, temperature protocols spanning up to five orders of magnitude in time-scales are performed to investigate thermally activated structural relaxation in a model amorphous solid. The…
Microcanonical thermodynamics (MT) is analysed for phase transitions of first and second order in finite systems. The transiton temperature, the latent heat and the surface tension of first order transitions can easily be determined by MT…
The turn-over frequency of the catalytic oxidation of CO at RuO2(110) was calculated as function of temperature and partial pressures using ab initio statistical mechanics. The underlying energetics of the gas-phase molecules, dissociation,…
We propose a relationship between thermodynamic phase transitions and ground-state quantum phase transitions in systems with variable Hamiltonian parameters. It is based on a link between zeros of the canonical partition function at complex…
In this paper we present a modeling approach to bridge the atomistic with macroscopic scales in crystalline materials. The methodology combines identification and modeling of the controlling unit processes at microscopic level with the…
We introduce a novel procedure for computing the (mu,T)-dependent pressure in continuum QCD; and therefrom obtain a complex phase diagram and predictions for thermal properties of the system, providing the in-medium behaviour of the trace…