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dc.contributor.authorFlick, Johannes-
dc.contributor.authorWelakuh, Davis M.-
dc.contributor.authorRuggenthaler, Michael-
dc.contributor.authorAppel, H.-
dc.contributor.authorRubio, Angel-
dc.identifierdoi: 10.1021/acsphotonics.9b00768-
dc.identifierissn: 2330-4022-
dc.identifier.citationACS Photonics 6(11): 2757-2778 (2019)-
dc.description.abstractWe 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.-
dc.description.sponsorshipJ.F. acknowledges financial support from the Deutsche Forschungsgemeinschaft (DFG) under Contract No. FL 997/1-1, and all of us acknowledge financial support from the European Research Council (ERC-2015-AdG-694097), the Cluster of Excellence ‘Advanced Imaging of Matter’ (AIM), Grupos Consolidados (IT1249-19) and SFB925 “Light induced dynamics and control of correlated quantum systems”-
dc.publisherACS Publications-
dc.subjectStrong light−matter coupling-
dc.subjectQuantum-electrodynamical density functional theory-
dc.subjectBenzene molecule-
dc.subjectLinear-response theory-
dc.subjectExcited states-
dc.titleLight-Matter response in Nonrelativistic Quantum Electrodynamics-
dc.contributor.funderGerman Research Foundation-
dc.contributor.funderEuropean Research Council-
dc.contributor.funderMinisterio de Economía y Competitividad (España)-
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