Theoretical investigations on cluster formation in mass spectrometry / vorgelegt von Alexander Haack. Wuppertal, März 2020
Inhalt
- 1 Motivation
- 2 Introduction to Computational Chemistry
- 2.1 Electronic Structure Calculations
- 2.2 Nuclear Position and Movement
- 2.3 Thermochemistry
- 2.4 Reaction Dynamics
- 2.5 Collision Cross Section Modeling
- 3 Charge Retention/Charge Depletion in ESI-MS
- 3.1 Abstract
- 3.2 Introduction
- 3.3 Methods
- 3.4 Results and Discussion
- 3.4.1 Structure and Thermochemistry of the Different Clusters
- 3.4.2 Proton Transfer Paths
- 3.4.3 Multiply Charged Analytes
- 3.5 Conclusion
- 3.6 Supporting Information
- 3.7 Follow-up work
- 4 Modeling of Differential Ion Mobility
- 4.1 Abstract
- 4.2 Introduction
- 4.2.1 Mobility at low field strength
- 4.2.2 Mobility at high field strength
- 4.2.3 Differential Mobility Spectrometry
- 4.3 Computational Methods
- 4.3.1 Ab initio calculations
- 4.3.2 CCS calculations
- 4.3.3 Mobility calculations
- 4.3.4 Boltzmann weighting
- 4.3.5 Dispersion Plot calculation
- 4.4 Results and Discussion
- 4.4.1 Cluster structures
- 4.4.2 CCS fits: MD vs. rigid samples
- 4.4.3 Mobility calculations
- 4.4.4 Dispersion plots
- 4.5 Conclusion
- 4.6 Supporting Information
- 4.7 Follow-up work
- 5 Thermochemistry from MD Simulations
- 5.1 Abstract
- 5.2 Introduction
- 5.3 Theory and Methods
- 5.3.1 The quasiharmonic approximation (QHA)
- 5.3.2 Implementation and special considerations
- 5.3.3 Electronic structure and MD simulations
- 5.4 Results and Discussion
- 5.5 Summary and Conclusions
- 5.6 Appendix A - The Eckart Frame
- 5.7 Appendix B - Separating out Internal Rotation
- 5.8 Supporting Information
- 6 Summary and Outlook
- 6.1 Answering Questions from Experiment
- 6.2 Developing new Calculation Methods
- 6.3 General Conclusion
- References