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- Finkelstein-Shapiro, DanielNational Autonomous University of Mexico (author)
Non-Hermitian Hamiltonians for linear and nonlinear optical response : A model for plexcitons
- Article/chapterEnglish2023
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- AIP Publishing,2023
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- LIBRIS-ID:oai:lup.lub.lu.se:5e9b9535-0ab4-4db9-883e-662d96972119
- https://lup.lub.lu.se/record/5e9b9535-0ab4-4db9-883e-662d96972119URI
- https://doi.org/10.1063/5.0130287DOI
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- Language:English
- Summary in:English
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- In polaritons, the properties of matter are modified by mixing the molecular transitions with light modes inside a cavity. Resultant hybrid light-matter states exhibit energy level shifts, are delocalized over many molecular units, and have a different excited-state potential energy landscape, which leads to modified exciton dynamics. Previously, non-Hermitian Hamiltonians have been derived to describe the excited states of molecules coupled to surface plasmons (i.e., plexcitons), and these operators have been successfully used in the description of linear and third order optical response. In this article, we rigorously derive non-Hermitian Hamiltonians in the response function formalism of nonlinear spectroscopy by means of Feshbach operators and apply them to explore spectroscopic signatures of plexcitons. In particular, we analyze the optical response below and above the exceptional point that arises for matching transition energies for plasmon and molecular components and study their decomposition using double-sided Feynman diagrams. We find a clear distinction between interference and Rabi splitting in linear spectroscopy and a qualitative change in the symmetry of the line shape of the nonlinear signal when crossing the exceptional point. This change corresponds to one in the symmetry of the eigenvalues of the Hamiltonian. Our work presents an approach for simulating the optical response of sublevels within an electronic system and opens new applications of nonlinear spectroscopy to examine the different regimes of the spectrum of non-Hermitian Hamiltonians.
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- Mante, Pierre AdrienLund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LTH profilområde: Avancerade ljuskällor,LU profilområde: Ljus och material,Lunds universitets profilområden,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LTH Profile Area: Photon Science and Technology,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas(Swepub:lu)chem-pim (author)
- Balci, SinanIzmir Institute of Technology (author)
- Zigmantas, DonatasLund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LTH profilområde: Avancerade ljuskällor,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LTH Profile Area: Photon Science and Technology,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas(Swepub:lu)chph-dzi (author)
- Pullerits, TõnuLund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,LTH profilområde: Nanovetenskap och halvledarteknologi,LTH profilområden,LTH profilområde: Avancerade ljuskällor,LU profilområde: Ljus och material,Lunds universitets profilområden,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Nanoscience and Semiconductor Technology,LTH Profile areas,Faculty of Engineering, LTH,LTH Profile Area: Photon Science and Technology,Faculty of Engineering, LTH,LU Profile Area: Light and Materials,Lund University Profile areas(Swepub:lu)chph-tp (author)
- National Autonomous University of MexicoKemisk fysik (creator_code:org_t)
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