Real time dynamical properties of biomolecules from ab initio quantum dynamics

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The inclusion of nuclear quantum effects (NQE) in the evaluation of real-time dynamical observables from computer simulations is a standing challenge, especially in the realm of ab initio electronic structure calculations of realistic materials and molecules. In this project, I propose to explore methodological solutions and application challenges for the inclusion of nuclear quantum effects in auto-correlation functions evaluated from first-principles path integral simulations. I will develop new ways to reduce the cost and accelerate the convergence of ring-polymer and centroid ab initio molecular dynamics (AIMD). I also plan to explore new concepts and techniques of obtaining quantum auto-correlation functions free of the spurious effects known to exist in the two above mentioned methods. The expertise in Prof. Manolopoulos group in Oxford will be very important for these developments. I will apply the developed framework for the evaluation of AIMD-derived, NQE-containing, anharmonic IR spectra of medium to large biomolecules. I will calculate gas-phase spectra and include solvation effects through stepwise hydration, up to full hydration, always including NQE. These spectra will have unparalleled accuracy, thus helping enormously the interpretation of experimental data and bringing precious insight for the characterization of polypeptide and protein structure. As a final application challenge, I plan to describe the structure and dynamics of proton-pump channels, where I hope to have experimental support of Oxford-based groups.