On the Interplay Between Force, Temperature, and Electric Fields in the Rupture Process of Mechanophores
Year: 2024
Type: article
Abstract: The use of oriented external electric fields (OEEFs) shows promise as an alternative approach to chemical catalysis. The ability to target a specific bond by aligning it with a bond-weakening electric field may be beneficial in mechanochemical reactions, which use mechanical force to selectively rupture bonds. Previous computational studies have focused on a static description of molecules in OEEFs, neglecting to test the influence of thermal oscillations on molecular stability. Here, we performed ab initio molecular dynamics (AIMD) simulations based on density functional theory (DFT) to investigate the behaviour of a model mechanophore under the simultaneous influence of thermal and electric field effects. We show that the change in bond length caused by a strong electric field is largely independent of the temperature, both without and with mechanical stretching forces applied to the molecule. The amplitude of thermal oscillations increases with increasing field strength and temperature, but at low temperatures, the application of mechanical force leads to an additional increase in amplitude. Our research shows that methods for applying mechanical force and OEEFs can be safely combined and included in an AIMD simulation at both low and high temperatures, allowing researchers to computationally investigate mechanochemical reactions in realistic application scenarios.
Source: ChemPhysChem
Authors: Tarek Scheele, Tim Neudecker
Institution: University of Bremen
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,330
Funder: Deutsche Forschungsgemeinschaft
OpenAlex ID: W4400935804