Impact of hydrophobicity and confinement on the structure and dynamics of water at interfaces / Frederik Maria Zysk ; [Supervised by: Prof. Dr. Thomas D. Kühne, Prof. Dr. Matthias Bauer]. Paderborn, 2023
Inhalt
- Motivation
- Methodology
- Fundamentals
- Semi-Empirical Methods
- Neglect of Diatomic Differential Overlap
- Overlap Matrix
- Core-Terms
- Two-Electron Integrals
- Fock Matrix Elements
- Two-Center Repulsion Integral
- Electrostatic Long-Range Scheme
- Modified Neglect of Diatomic Overlap
- PM6
- PM6-FM
- DFT Theory
- ALMO
- SFG
- Accuracy of DFT Functionals
- Unravelling the relationship between the H-Bond strength and the reorientation dynamics at the water/air interface
- Introduction
- Computational Details
- Ring Polymer Molecular Dynamics (RPMD) simulation
- ALMO EDA
- Surface-specific velocity-velocity correlation function
- Results
- Instantaneous water/air layer
- Reorientation dynamics of OH groups
- H2O, HDO and D2O reorientation dynamics
- Water layer SFG calculation
- H-Bond energy and asymmetry
- Relationship between short-time dynamics and H-bond strength
- Conclusion
- Impact of hydrophobicity and pore size on structure and dynamics inside nanopores
- Introduction
- Computational Details
- Results
- Pore densities and the Gibbs dividing surface
- H-Bond coordination numbers
- Diffusion coefficients by MSD calculations
- Radial diffusion calculated by MSD
- Power spectra of water inside nanopores
- Surface-specific SFG spectra inside nanopores
- Angular distribution and diffusion based on the dipole angle
- Conclusion
- Influence of polarity on water structure in trimethylsilanol (TMS) functionalized and hydrophilic pores
- Introduction
- Computational Details
- Results
- Characterization of simulated pore systems based on surface area, effective diameter, and functional group density
- Radial Density Distribution of water and defining functional group elements
- Coordination number of water molecules with itself and the hydroxyl Surface
- Analysis of water structure at the surface based on velocity-velocity surface specific SFG calculations
- Analysis of water structure at the surface based angular distribution analysis
- Conclusion
- Impact of hydrophobicity on the gas self-diffusion of oxygen and water vapor in mesoporous silica pores
- Appendix