Molecular vibrations act as unique fingerprints, offering detailed insights into chemical bonds and molecular interactions. This Ph.D. thesis focuses on advancing computational methods to simulate these vibrations, particularly within complex molecular environments. The work introduces notable advancements in multiscale embedding methods, a powerful approach that enables precise modeling of crucial molecular regions while efficiently accounting for their surroundings. A major contribution is the advancement of the fragment[1]based polarizable embedding quantum mechanics (PE-QM) approach for vibrational analysis. This includes the development of methodologies for accurate and efficient modeling of vibrational spectroscopies, such as harmonic infrared (IR) and Raman. Extensions toward nonlinear vibrational spectroscopy are also explored, laying the groundwork for studying higher-order vibrational phenomena. Central to this research is the development of PyFraME, an open-source software package designed to streamline and automate workflows for fragment-based multiscale embedding calculations. By integrating theoretical innovations with high-performance computing, PyFraME provides a versatile platform for exploring molecular properties in complex environments. These advancements establish a robust foundation for investigating complex biomolecular systems and nonlinear vibrational phenomena with PE-QM, unlocking new possibilities for understanding complex biomolecular processes.
Principal Supervisor:
Associate Professor Jógvan Magnus Haugaard Olsen, DTU Chemistry
Co-supervisor:
Professor Klaus Braagaard Møller, DTU Chemistry
Examiners:
Professor Piotr de Silva, DTU Energy
Professor Jacob Kongsted, University of Southern Denmark
Professor Patrick Norman, KTH Royal Institute of Technology, Sweden
Chairperson:
Associate Professor Janus Juul Eriksen, DTU Chemistry