UNIverse - Public Research Portal
Project cover

Intermolecular Interactions and the Role of Dynamics for Chemical Reactions in Complex Systems

Research Project
 | 
01.10.2019
 - 30.09.2022

The goal of this project is to develop, implement and apply computational strategies to characterize, understand and eventually predict properties of complex chemical and biochemical systems at a molecular level. To this end, techniques including multipolar force fields, (adiabatic) reactive molecular dynamics and neural network-based potential energy surfaces are further developed and used. Multipole force fields will be extended to treat general spectroscopic applications (1- and 2-dimensional infrared spectroscopy), using fluctuating multipoles and describing the energetics of the nuclear degrees of freedom with reproducing kernels. Applications include spectroscopic probes such as -CO, -NO and -N3 for which accurate, fully dimensional potential energy surfaces can be calculated. This will be used to characterize the site-specific dynamics and functional motions of proteins such as insulin, lysozyme, myoglobin and nitrophorin in solution. For insulin, analysis of motions at the dimerization interface will be used to quantify the physiologically relevant monomer/dimer equilibrium which is difficult to do with experimentally established, thermodynamic approaches. To account for vibrational coherences, partial linearized density matrix (PLDM) propagation will be generalized for vibrational dynamics (vPLDM). Nitrosylation of nitrophorin will investigate molecular determinants of NO-signaling in a protein. To study chemical reactions in the gas phase we will use machine learning within the PhysNet neural network architecture to generate fully-dimensional, reactive potential energy surfaces. Here, applications focus on systems relevant to atmospheric chemistry, including isomerization and decomposition reactions of acetaldehyde and pyruvic acid for which fragmentation patterns and final state distributions are important for subsequent reactions. In a next step, PhysNet will be used to investigate double proton transfer in the gas phase and in solution with the aim to characterize the role of solvent in chemical reactions at a molecular level. The present proposal involves two research themes: 1) reactive simulations in the gas- and condensed phase and 2) computational vibrational spectroscopy which both require accurate representations of the intermolecular interactions.

Funding

Intermolecular Interactions and the Role of Dynamics for Chemical Reactions in Complex Systems

SNF Projekt (GrantsTool), 10.2019-09.2022 (36)
PI : Meuwly, Markus.

Members (3)

Profile Photo

Markus Meuwly

Principal Investigator
MALE avatar

Luis Itza Vazquez Salazar

Project Member
MALE avatar

Juan Carlos San Vicente Veliz

Project Member