Light–Matter Response in Nonrelativistic Quantum Electrodynamics
Johannes Flick
Davis M. Welakuh
Michael Ruggenthaler
Heiko Appel
Angel Rubio
10.1021/acsphotonics.9b00768.s001
https://acs.figshare.com/articles/journal_contribution/Light_Matter_Response_in_Nonrelativistic_Quantum_Electrodynamics/10072649
We
derive the full linear-response theory for nonrelativistic quantum
electrodynamics in the long wavelength limit and provide a practical
framework to solve the resulting equations by using quantum-electrodynamical
density-functional theory. We highlight how the coupling between quantized
light and matter changes the usual response functions and introduces
cross-correlated light-matter response functions. These cross-correlation
responses lead to measurable changes in Maxwell’s equations
due to the quantum-matter-mediated photon–photon interactions.
Key features of treating the combined matter-photon response are that
natural lifetimes of excitations become directly accessible from first-principles,
changes in the electronic structure due to strong light-matter coupling
are treated fully nonperturbatively, and self-consistent solutions
of the back-reaction of matter onto the photon vacuum and vice versa
are accounted for. By introducing a straightforward extension of the
random-phase approximation for the coupled matter-photon problem,
we calculate the ab initio spectra for a real molecular system that
is coupled to the quantized electromagnetic field. Our approach can
be solved numerically very efficiently. The presented framework leads
to a shift in paradigm by highlighting how electronically excited
states arise as a modification of the photon field and that experimentally
observed effects are always due to a complex interplay between light
and matter. At the same time the findings provide a route to analyze
as well as propose experiments at the interface between quantum chemistry,
nanoplasmonics and quantum optics.
2019-10-29 19:03:21
random-phase approximation
matter-photon response
response functions
framework
matter changes
photon field
quantum optics
linear-response theory
wavelength limit
quantum chemistry
nonrelativistic quantum electrodynamics
Nonrelativistic Quantum Electrodynamics
cross-correlation responses
Key features
ab initio spectra
quantized electromagnetic field
matter-photon problem
quantized light
equation
photon vacuum
quantum-electrodynamical density-functional theory
cross-correlated light-matter response functions