• Corpus ID: 248798657

Ultrafast collapse of molecular polaritons in photoswitch-nanoantennas at room temperature

  title={Ultrafast collapse of molecular polaritons in photoswitch-nanoantennas at room temperature},
  author={Joel Kuttruff and Marco Romanelli and Esteban Pedrueza-Villalmanzo and Jonas Allerbeck and Jacopo Fregoni and Valeria Saavedra-Becerril and Joakim Andr'easson and Daniele Brida and Alexandre Dmitriev and Stefano Corni and Nicol{\`o} Maccaferri},
Molecular polaritons are hybrid light-matter states that emerge when a molecular transition strongly interacts with photons in a resonator. At optical frequencies, this interaction unlocks a way to explore and control new chemical phenomena at the nanoscale. Achieving such a control at ultrafast timescales, however, is an outstanding challenge, as it requires a deep understanding of the dynamics of the collectively coupled molecular excitation and the light modes. Here, we investigate the… 

Figures from this paper


Femtosecond Photophysics of Molecular Polaritons.
This Perspective focuses on the collective aspects of strongly coupled molecular systems and how this pertains to the dynamical response of such systems, and how the ultrafast time and spectral resolution make pump-probe spectroscopy an ideal tool to reveal the energy-transfer pathways from polariton states to other molecular states of functional interest.
Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light–Molecule Coupling
This work studied a molecular chromophore under strong coupling with the optical mode of a Fabry–Perot cavity resonant to the first electronic absorption band to provide new physical insight into the role of two-particle polaritonic states in explaining transient signatures in hybrid light–matter coupling systems consistent with analogous many-body systems.
Single-photon nonlinearity at room temperature.
Stable excitons dressed with high-energy molecular vibrations are utilized, allowing for single-photon nonlinear operation at ambient conditions, and opens new horizons for practical implementations like sub-picosecond switching, amplification and all-optical logic at the fundamental quantum limit.
Theoretical Challenges in Polaritonic Chemistry
Polaritonic chemistry exploits strong light–matter coupling between molecules and confined electromagnetic field modes to enable new chemical reactivities. In systems displaying this functionality,
Reversible switching of ultrastrong light-molecule coupling
The light-molecule interaction in the system enters the regime of ultrastrong coupling, where the energy splitting is substantial fraction of the coupled transition energies, and new phenomena such squeezed vacuum state and generation of entangled photon pairs are predicted.
Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures.
An ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure is demonstrated and a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plAsmonic circuits.
Aluminum Nanoantenna Complexes for Strong Coupling between Excitons and Localized Surface Plasmons.
We study the optical dynamics in complexes of aluminum nanoantennas coated with molecular J-aggregates and find that they provide an excellent platform for the formation of hybrid exciton-localized
Ultrafast Transmission Modulation and Recovery via Vibrational Strong Coupling.
It is found that the Rabi splitting recovers with the characteristic vibrational relaxation lifetime and anisotropy decay of uncoupled W(CO)6, implying that polaritons are not directly involved in the relaxation the authors observe after the first few ps.
Ultrafast all-optical switching enabled by epsilon-near-zero-tailored absorption in metal-insulator nanocavities
Ultrafast control of light−matter interactions is fundamental in view of new technological frontiers of information processing. However, conventional optical elements are either static or feature