Photochemistry in the strong coupling regime: A trajectory surface hopping scheme

Area of Science:

• Quantum chemistry
• Photochemistry
• Molecular spectroscopy

Background:

• Strong light-matter coupling modifies molecular properties by forming hybrid light-molecule states.
• Dynamical processes in these polaritonic systems are significantly altered.
• Existing models often neglect photon degrees of freedom and nonadiabatic events.

Purpose of the Study:

• To investigate photochemical processes under strong light-matter coupling.
• To develop a theoretical framework for describing polaritonic photochemistry.
• To explicitly include photon dynamics and nonadiabatic effects in chemical reactivity studies.

Main Methods:

• Extension of the direct trajectory surface hopping (TSH) scheme.
• Investigating photochemistry in systems exhibiting strong coupling between light and organic molecules.
• Incorporating photon degrees of freedom and nonadiabatic events into the dynamical description.

Main Results:

• The study provides a method to simulate photochemical reactions in the strong coupling regime.
• Demonstrates the importance of including photon dynamics for accurate reactivity descriptions.
• Highlights modifications in ground and excited state properties due to strong coupling.

Conclusions:

• The extended TSH scheme is suitable for describing photochemical polaritonic processes.
• Accurate modeling of photochemistry in strongly coupled systems requires accounting for light-matter interactions.
• This approach opens new avenues for controlling chemical reactions using light.