Understanding radiative transitions and relaxation pathways in plexcitons

Daniel Finkelstein-Shapiro, Pierre Adrien Mante, Sema Sarisozen, Lukas Wittenbecher, Iulia Minda, Sinan Balci, Tõnu Pullerits, Donatas Zigmantas

Research output: Contribution to journalArticlepeer-review


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.

Original languageEnglish
Pages (from-to)1092-1107
Number of pages16
Issue number4
Publication statusPublished - 2021

Subject classification (UKÄ)

  • Atom and Molecular Physics and Optics
  • Physical Chemistry

Free keywords

  • cavity quantum electrodynamics
  • excitation energy dissipation
  • molecular aggregates
  • open quantum systems
  • plasmons
  • plexcitons
  • polaritons
  • SDG7: Affordable and clean energy
  • two-dimensional electronic spectroscopy


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