相关论文: First-principles statistical mechanics approach to…
We employ a first-principles lattice-gas Hamiltonian (LGH) approach to determine the lateral interactions between O atoms adsorbed on the Pd(100) surface. With these interactions we obtain an ordering behavior at low coverage that is in…
Present knowledge of the function of materials is largely based on studies (experimental and theoretical) that are performed at low temperatures and ultra-low pressures. However, the majority of everyday applications, like e.g. catalysis,…
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…
The methodology of deriving an adatom lattice-gas Hamiltonian (LGH) from first principles (FP) calculations is revisited. Such LGH cluster expansions compute a large set of lateral pair-, trio-, quarto interactions by solving a set of…
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…
We present a first-principles based multiscale modeling approach to heterogeneous catalysis that integrates first-principles kinetic Monte Carlo simulations of the surface reaction chemistry into a fluid dynamical treatment of the…
We describe a first-principles statistical mechanics approach enabling us to simulate the steady-state situation of heterogeneous catalysis. In a first step density-functional theory together with transition-state theory is employed to…
Using a lattice-gas model with pairwise interactions, we study the ordered structures, coverage dependence of the heat of adsorption, and other experimentally observable behavior of adsorbed CO overlayers on Pd(100) single crystal surfaces.…
We present a first-principles atomistic thermodynamics framework to describe the structure, composition and segregation profile of an alloy surface in contact with a (reactive) environment. The method is illustrated with the application to…
Fabrication, handling and disposal of nuclear fuel materials require comprehensive knowledge of their surface morphology and reactivity. Due to unavoidable contact with air components (even at low partial pressures), UN samples contain…
A series of First Principles calculations is undertaken to characterize and explain the enhancement of the catalytic activity of oxygen on top of very disordered nanomaterials of Pt. As the adsorption of OH fragment on top of the surfaces…
This work represents the first chapter of a project on the foundations of first-principle calculations of the electron transport in crystals at finite temperatures. We are interested in the range of temperatures, where most electronic…
We show that the dynamics of kinetically constrained models of glass formers takes place at a first-order coexistence line between active and inactive dynamical phases. We prove this by computing the large-deviation functions of suitable…
In a previous contribution, Phys. Rev. Lett 107, 230601 (2011), we have proposed a method to treat first order phase transitions at low temperatures. It describes arbitrary order parameter through an analytical expression $W$, which depends…
A new combination of first principle molecular dynamics (MD) simulations with a rate equation model presented in the preceding paper (paper I) is applied to analyze in detail the scattering of argon atoms from a platinum (111) surface. The…
We perform all-electron path integral Monte Carlo (PIMC) and density functional theory molecular dynamics (DFT-MD) calculations to explore warm dense matter states of oxygen. Our simulations cover a wide density-temperature range of…
Graphene oxide (GO) materials are widely studied, and yet their atomic-scale structures remain to be fully understood. Here we show that the chemical and configurational space of GO can be rapidly explored by advanced machine-learning…
We assess heat and mass transfer limitations in in situ studies of model catalysts with a first-principles based multiscale modeling approach that integrates a detailed description of the surface reaction chemistry and the macro-scale flow…
The qualitative solvent- and temperature-dependent conformational behavior of a peptide in the proximity of solid substrates with different adsorption properties is investigated by means of a simple lattice model. The resulting pseudophase…
Results of X-ray diffraction experiments on solid oxygen at low temperature and at pressures up to 10 GPa are presented.A careful sample preparation and annealing around 240 K allowed to obtain very good diffraction patterns in the…