Abstract
Polaritonic chemistry has ushered in new avenues for controlling molecular dynamics. However, two key questions remain: (i) Can classical light sources elicit the same effects as certain quantum light sources on molecular systems? (ii) Can semiclassical treatments of light-matter interactions capture nontrivial quantum effects observed in molecular dynamics? This work presents a quantum-classical approach addressing issues of realizing cavity chemistry effects without actual cavities. It also highlights the limitations of the standard semiclassical light-matter interaction. It is demonstrated that classical light sources can mimic quantum effects up to the second order of light-matter interaction provided that the mean-field contribution, the symmetrized two-time correlation function, and the linear response function are the same in both situations. Numerical simulations show that the quantum-classical method aligns more closely with exact quantum molecular-only dynamics for quantum light states such as Fock states, superpositions of Fock states, and vacuum squeezed states than does the conventional semiclassical approach.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.