Photoinduced Molecular Dynamics in Solution: Multiscale Modelling and the Link to Ultrafast Experiments

Description

This book explores novel computational strategies for simulating excess energy dissipation alongside transient structural changes in photoexcited molecules, and accompanying solvent rearrangements. It also demonstrates in detail the synergy between theoretical modelling and ultrafast experiments in unravelling various aspects of the reaction dynamics of solvated photocatalytic metal complexes. Transition metal complexes play an important role as photocatalysts in solar energy conversion, and the rational design of metal-based photocatalytic systems with improved efficiency hinges on the fundamental understanding of the mechanisms behind light-induced chemical reactions in solution. Theory and atomistic modelling hold the key to uncovering these ultrafast processes. Linking atomistic simulations and modern X-ray scattering experiments with femtosecond time resolution, the book highlights previously unexplored dynamical changes in molecules, and discusses the development of theoretical and computational frameworks capable of interpreting the underlying ultrafast phenomena. Front Matter ....Pages i-xxxviii Front Matter ....Pages 1-1 Filming Motion at the Atomic Scale of Time (Gianluca Levi)....Pages 3-11 The Diplatinum Complex PtPOP (Gianluca Levi)....Pages 13-17 Outline of the Thesis (Gianluca Levi)....Pages 19-20 Front Matter ....Pages 21-21 Nuclear Dynamics (Gianluca Levi)....Pages 23-27 Density Functional Methods (Gianluca Levi)....Pages 29-70 The Quantum Mechanics/Molecular Mechanics Method (Gianluca Levi)....Pages 71-86 Front Matter ....Pages 87-87 Observing Molecular Motion in Solution with X-Rays (Gianluca Levi)....Pages 89-97 Simulating and Analysing X-Ray Diffuse Scattering Signals (Gianluca Levi)....Pages 99-107 Front Matter ....Pages 109-109 Gas-Phase Molecular Geometry (Gianluca Levi)....Pages 111-123 Computational Details of the QM/MM BOMD Simulations (Gianluca Levi)....Pages 125-141 Equilibrium Solution Structure (Gianluca Levi)....Pages 143-155 Coherent Vibrational Dynamics in the Ground State (Gianluca Levi)....Pages 157-163 Dynamics of Excited-State Bond Formation (Gianluca Levi)....Pages 165-186 Front Matter ....Pages 187-187 Summarizing Results and Outlook (Gianluca Levi)....Pages 189-193 Back Matter ....Pages 195-208