Non-Hermitian Hamiltonians for linear and nonlinear optical response : A model for plexcitons
Finkelstein-Shapiro, Daniel LU ; Mante, Pierre Adrien LU ; Balci, Sinan ; Zigmantas, Donatas LU
and Pullerits, Tõnu
LU
(2023)
In Journal of Chemical Physics
158(10).
- Abstract
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... (More)
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.
(Less)
- author
- Finkelstein-Shapiro, Daniel
LU
; Mante, Pierre Adrien
LU
; Balci, Sinan
; Zigmantas, Donatas
LU
and Pullerits, Tõnu
LU
- organization
- publishing date
- 2023-03-14
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Chemical Physics
- volume
- 158
- issue
- 10
- article number
- 104104
- publisher
- American Institute of Physics (AIP)
- external identifiers
-
- scopus:85149856288
- pmid:36922135
- ISSN
- 0021-9606
- DOI
- 10.1063/5.0130287
- language
- English
- LU publication?
- yes
- id
- 5e9b9535-0ab4-4db9-883e-662d96972119
- date added to LUP
- 2023-05-05 08:37:41
- date last changed
- 2024-06-29 03:50:00
@article{5e9b9535-0ab4-4db9-883e-662d96972119,
abstract = {{<p>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.</p>}},
author = {{Finkelstein-Shapiro, Daniel and Mante, Pierre Adrien and Balci, Sinan and Zigmantas, Donatas and Pullerits, Tõnu}},
issn = {{0021-9606}},
language = {{eng}},
month = {{03}},
number = {{10}},
publisher = {{American Institute of Physics (AIP)}},
series = {{Journal of Chemical Physics}},
title = {{Non-Hermitian Hamiltonians for linear and nonlinear optical response : A model for plexcitons}},
url = {{http://dx.doi.org/10.1063/5.0130287}},
doi = {{10.1063/5.0130287}},
volume = {{158}},
year = {{2023}},
}