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Updated: Jul 8, 2025
00:07
A Photonic System for Generating Unconditional Polarization-Entangled Photons Based on Multiple Quantum Interference
Published on: September 5, 2019
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Simulating the Excited-State Dynamics of Polaritons with Ab Initio Multiple Spawning.
Bhaskar Rana1,2, Edward G Hohenstein1,2, Todd J Martínez1,2
1Department of Chemistry and The PULSE Institute, Stanford University, Stanford, California 94305, United States.
The Journal of Physical Chemistry. A
|December 18, 2023
Summary
Polaritonic chemistry uses light-matter hybrid states to control chemical reactions. This study introduces a GPU-accelerated model to simulate these polaritonic states, demonstrating control over molecular photoreactions.
Area of Science:
- Quantum Chemistry
- Chemical Physics
- Computational Chemistry
Background:
- Polaritonic chemistry explores hybrid light-matter states (polaritons) formed by strong coupling between molecules and photons.
- These polaritons can significantly influence photochemical reaction pathways.
- Cavity-enhanced effects can even occur via coupling to vacuum field fluctuations.
Purpose of the Study:
- To develop a first-principles model for simulating nonadiabatic dynamics of polaritonic states in optical cavities.
- To investigate the manipulation of photochemical reaction pathways using cavity coupling.
- To explore cavity-based control over the ordering of molecular excited states.
Main Methods:
- Development of a GPU-accelerated computational model for polaritonic dynamics.
- Simulation of a single salicylideneaniline (SA) molecule strongly coupled to a cavity photon.
- Utilizing complete active space configuration interaction (CASCI) and the ab initio multiple spawning (AIMS) method.
- Employing a Jaynes-Cummings-type Hamiltonian.
Main Results:
- Demonstrated manipulation of photodeactivation pathway branching ratios for SA molecule via cavity coupling.
- Showcased the ability to halt photoreactions within an optical cavity.
- Investigated cavity-induced control over the energy ordering of bright and dark excited states.
Conclusions:
- First-principles modeling of polaritonic chemistry is feasible and powerful.
- Optical cavities offer a means to control molecular reaction dynamics and excited-state properties.
- This approach opens new avenues for designing chemical reactions using light-matter interactions.
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