2021-04-12T03:58:31Z
http://digital.csic.es/dspace-oai/request
oai:digital.csic.es:10261/209627
2020-12-12T23:53:53Z
com_10261_115
com_10261_3
col_10261_368
http://hdl.handle.net/10261/209627
10.1021/acsphotonics.9b00768
390267
Light-Matter response in Nonrelativistic Quantum Electrodynamics
ACS Publications
2019
Flick, Johannes
Welakuh, Davis M.
Ruggenthaler, Michael
Appel, Heiko
Rubio, Ángel
Strong light−matter coupling
Quantum-electrodynamical density functional theory
Benzene molecule
Linear-response theory
Excited states
2019-11-20
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 lightmatter 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.
German Research Foundation
European Research Council
Ministerio de Economía y Competitividad (España)