Light-matter hybrid-orbital-based first-principles methods: the influence of the polariton statistics

Journal of Chemical Theory and Computation
Florian BuchholzAngel Rubio

Abstract

A detailed understanding of strong matter-photon interactions requires first-principle methods that can solve the fundamental Pauli-Fierz Hamiltonian of non-relativistic quantum electrodynamics efficiently. A possible way to extend well-established electronic-structure methods to this situation is to embed the Pauli-Fierz Hamiltonian in a higher-dimensional light-matter hybrid auxiliary configuration space. In this work we show the importance of the resulting hybrid Fermi-Bose statistics of the polaritons, which are the new fundamental particles of the ``photon-dressed'' Pauli-Fierz Hamiltonian for systems in cavities. We show that violations of these statistics can lead to unphysical results. We present an efficient way to ensure the proper symmetry of the underlying wave functions by enforcing representability conditions on the dressed one-body reduced density matrix. We further present a general prescription how to extend a given first-principles approach to polaritons and as an example introduce polaritonic Hartree-Fock theory. While being a single-reference method in polariton space, polaritonic Hartree-Fock is a multi-reference method in the electronic space, i.e. it describes electronic correlations. We also discuss poss...Continue Reading

References

Aug 25, 2004·Physical Review Letters·J BellessaJ Mugnier
Jan 12, 2012·Angewandte Chemie·James A HutchisonThomas W Ebbesen
Dec 24, 2014·Reports on Progress in Physics·P Törmä, W L Barnes
May 30, 2015·Physical Review Letters·Johannes Feist, Francisco J Garcia-Vidal
Nov 18, 2015·Journal of Chemical Theory and Computation·Stefan VuckovicPaola Gori-Giorgi
Dec 3, 2015·Proceedings of the National Academy of Sciences of the United States of America·Johannes FlickAngel Rubio
Feb 8, 2016·The Journal of Chemical Physics·Markus KowalewskiShaul Mukamel
Apr 3, 2016·The Journal of Chemical Physics·Prasoon Saurabh, Shaul Mukamel
Apr 6, 2016·Journal of Chemical Theory and Computation·Lin Lin
Jun 15, 2016·Nature·Rohit ChikkaraddyJeremy J Baumberg
Jun 25, 2016·Physical Review Letters·Felipe Herrera, Frank C Spano
Oct 7, 2016·Faraday Discussions·Kochise BennettShaul Mukamel
Oct 22, 2016·Physical Review Letters·Jino GeorgeThomas W Ebbesen
Mar 10, 2017·Proceedings of the National Academy of Sciences of the United States of America·Johannes FlickAngel Rubio
Jul 28, 2017·Journal of Chemical Theory and Computation·Hoi Ling LukGerrit Groenhof
Sep 25, 2017·Nano Letters·Andreas BayerChristoph Lange
Sep 28, 2017·Physical Review Letters·David PlankensteinerClaudiu Genes
Nov 15, 2017·Nature Communications·Simone De Liberato
Jun 13, 2018·Nature Communications·Kati StraniusKarl Börjesson
Jul 3, 2018·ACS Photonics·Charles MöhlJana Zaumseil
Jan 5, 2019·Physical Review Letters·Oriol Vendrell
Jun 8, 2019·Physical Review Letters·Michael ReitzClaudiu Genes
Sep 7, 2019·Journal of Chemical Theory and Computation·Uliana MordovinaAngel Rubio
Oct 24, 2019·The Journal of Chemical Physics·Yu ZhangSergei Tretiak
Dec 4, 2019·ACS Photonics·Florian BuchholzAngel Rubio
Dec 4, 2019·ACS Photonics·Johannes FlickAngel Rubio

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