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  The relevance of degenerate states in chiral polaritonics

Bustamante, C., Sidler, D., Ruggenthaler, M., & Rubio, A. (2024). The relevance of degenerate states in chiral polaritonics. The Journal of Chemical Physics, 161(24): 244101. doi:10.1063/5.0235935.

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Supplementary material: encompasses additional simulation data that is provided for the chiral cavity with an externally applied magnetic field
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 Creators:
Bustamante, C.1, 2, Author           
Sidler, D.1, 2, 3, Author           
Ruggenthaler, M.1, 2, 4, Author           
Rubio, A.1, 2, 4, Author           
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Center for Free-Electron Laser Science, ou_persistent22              
3Laboratory for Materials Simulations, Paul Scherrer Institut, ou_persistent22              
4The Hamburg Center for Ultrafast Imaging, ou_persistent22              

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Free keywords: Magnetic properties, Quasiparticle, Computational electromagnetics, Magnetic dipole moment, Optical cavity, Isomerism, Chirality, Operator theory, Degenerate energy levels, Spontaneous symmetry breaking
 Abstract: In this work, we theoretically explore whether a parity-violating/chiral light–matter interaction is required to capture all relevant aspects of chiral polaritonics or if a parity-conserving/achiral theory is sufficient (e.g., long-wavelength/dipole approximation). This question is non-trivial to answer since achiral theories (Hamiltonians) still possess chiral solutions. To elucidate this fundamental theoretical question, a simple GaAs quantum ring model is coupled to an effective chiral mode of a single-handedness optical cavity in dipole approximation. The bare matter GaAs quantum ring possesses a non-degenerate ground state and a doubly degenerate first excited state. The chiral or achiral nature (superpositions) of the degenerate excited states remains undetermined for an isolated matter system. However, inside our parity-conserving description of a chiral cavity, we find that the dressed eigenstates automatically (ab initio) attain chiral character and become energetically discriminated based on the handedness of the cavity. In contrast, the non-degenerate bare matter state (ground state) does not show energetic discrimination inside a chiral cavity within a dipole approximation. Nevertheless, our results suggest that the handedness of the cavity can still be imprinted onto these states (e.g., angular momentum and chiral current densities). Overall, the above findings highlight the relevance of degenerate states in chiral polaritonics. In particular, because recent theoretical results for linearly polarized cavities indicate the formation of a frustrated and highly degenerate electronic ground state under collective strong coupling conditions, which, likewise, is expected to form in chiral polaritonics and, thus, could be prone to chiral symmetry breaking effects.

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Language(s): eng - English
 Dates: 2024-08-302024-12-052024-12-232024-12-28
 Publication Status: Issued
 Pages: -
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2408.16695
DOI: 10.1063/5.0235935
 Degree: -

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Project name : This work was supported by the RouTe Project (Project No. 13N14839), financed by the Federal Ministry of Education and Research [Bundesministerium fur Bildung und Forschung (BMBF)] and supported by the European Research Council (Grant No. ERC-2015-AdG694097), the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG), EXC 2056 (Project ID 390715994), and the Grupos Consolidados (Grant No. IT1249-19). The Flatiron Institute is a division of the Simons Foundation. C. M. Bustamante, thanks to the Alexander von Humboldt-Stiftung for the financial support from the Humboldt Research Fellowship.
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Source 1

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Title: The Journal of Chemical Physics
  Abbreviation : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: - Volume / Issue: 161 (24) Sequence Number: 244101 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226