2024-03-29T08:39:43Zhttp://digital.csic.es/dspace-oai/requestoai:digital.csic.es:10261/2096272021-12-28T15:52:03Zcom_10261_115com_10261_3col_10261_368
00925njm 22002777a 4500
dc
Flick, Johannes
author
Welakuh, Davis M.
author
Ruggenthaler, Michael
author
Appel, H.
author
Rubio, Angel
author
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.
ACS Photonics 6(11): 2757-2778 (2019)
http://hdl.handle.net/10261/209627
10.1021/acsphotonics.9b00768
http://dx.doi.org/10.13039/501100003329
http://dx.doi.org/10.13039/501100001659
http://dx.doi.org/10.13039/501100000781
31788500
Strong light−matter coupling
Quantum-electrodynamical density functional theory
Benzene molecule
Linear-response theory
Excited states
Light-Matter response in Nonrelativistic Quantum Electrodynamics