English
 
User Manual Privacy Policy Disclaimer Contact us
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Light–Matter Response in Nonrelativistic Quantum Electrodynamics

MPS-Authors
/persons/resource/persons45976

Flick,  J.
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge;
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Department of Physics, University of Hamburg;

/persons/resource/persons199416

Welakuh,  D.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

/persons/resource/persons30964

Ruggenthaler,  M.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

/persons/resource/persons21304

Appel,  H.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

/persons/resource/persons22028

Rubio,  A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Computational Quantum Physics, Flatiron Institute;
Nano-Bio Spectroscopy Group, Departamento de Fisica de Materiales, Universidad del País Vasco;

External Ressource
Fulltext (public)

acsphotonics.9b00768.pdf
(Publisher version), 4MB

Supplementary Material (public)

ph9b00768_si_001.pdf
(Supplementary material), 281KB

Citation

Flick, J., Welakuh, D., Ruggenthaler, M., Appel, H., & Rubio, A. (2019). Light–Matter Response in Nonrelativistic Quantum Electrodynamics. ACS Photonics, 6(11), 2757-2778. doi:10.1021/acsphotonics.9b00768.


Cite as: http://hdl.handle.net/21.11116/0000-0005-3E34-C
Abstract
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.