Understanding radiative transitions and relaxation pathways in plexcitons
Finkelstein-Shapiro, Daniel LU ; Mante, Pierre Adrien LU ; Sarisozen, Sema ; Wittenbecher, Lukas LU ; Minda, Iulia LU ; Balci, Sinan ; Pullerits, Tõnu LU and Zigmantas, Donatas LU
(2021)
In Chem
7(4).
p.1092-1107
- Abstract
Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic... (More)
Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.
(Less)
- author
- Finkelstein-Shapiro, Daniel
LU
; Mante, Pierre Adrien
LU
; Sarisozen, Sema
; Wittenbecher, Lukas
LU
; Minda, Iulia
LU
; Balci, Sinan
; Pullerits, Tõnu
LU
and Zigmantas, Donatas
LU
- organization
- publishing date
- 2021
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- cavity quantum electrodynamics, excitation energy dissipation, molecular aggregates, open quantum systems, plasmons, plexcitons, polaritons, SDG7: Affordable and clean energy, two-dimensional electronic spectroscopy
- in
- Chem
- volume
- 7
- issue
- 4
- pages
- 16 pages
- publisher
- Elsevier
- external identifiers
-
- scopus:85104061301
- ISSN
- 2451-9308
- DOI
- 10.1016/j.chempr.2021.02.028
- language
- English
- LU publication?
- yes
- id
- d77923ad-9fb6-419d-abd3-b23ea659fa0b
- date added to LUP
- 2021-04-20 12:22:10
- date last changed
- 2023-11-08 13:07:48
@article{d77923ad-9fb6-419d-abd3-b23ea659fa0b,
abstract = {{<p>Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.</p>}},
author = {{Finkelstein-Shapiro, Daniel and Mante, Pierre Adrien and Sarisozen, Sema and Wittenbecher, Lukas and Minda, Iulia and Balci, Sinan and Pullerits, Tõnu and Zigmantas, Donatas}},
issn = {{2451-9308}},
keywords = {{cavity quantum electrodynamics; excitation energy dissipation; molecular aggregates; open quantum systems; plasmons; plexcitons; polaritons; SDG7: Affordable and clean energy; two-dimensional electronic spectroscopy}},
language = {{eng}},
number = {{4}},
pages = {{1092--1107}},
publisher = {{Elsevier}},
series = {{Chem}},
title = {{Understanding radiative transitions and relaxation pathways in plexcitons}},
url = {{http://dx.doi.org/10.1016/j.chempr.2021.02.028}},
doi = {{10.1016/j.chempr.2021.02.028}},
volume = {{7}},
year = {{2021}},
}