Esta es la versión de autor del artículo publicado en: This is an author produced version of a paper published in:El acceso a la versión del editor puede requerir la suscripción del recurso Access to the published version may require subscription
AbstractWe present an overview of the general concepts of polaritonic chemistry with organic molecules, i.e., the manipulation of chemical structure that can be achieved through strong coupling between confined light modes and organic molecules. Strong coupling and the associated formation of polaritons, hybrid light-matter excitations, leads to energy shifts in such systems that can amount to a large fraction of the uncoupled transition energy. This has recently been shown to significantly alter the chemical structure of the coupled molecules, which opens the possibility to manipulate and control reactions. We discuss the current state of theory for describing these changes and present several applications, with a particular focus on the collective effects observed when many molecules are involved in strong coupling.Keywords polaritonic chemistry, photochemistry, organic molecules, quantum optics 1 When the coherent energy exchange between a confined light mode and a quantum emitter becomes faster than the decay and decoherence of either constituent, the system enters into the regime of strong coupling or vacuum Rabi splitting. 1,2 The fundamental excitations of the system are then polaritons, hybrid light-matter excitations. This requires a large (collective)where N is the number of involved emitters, µ is their transition dipole moment, and E 1ph ∝ V −1/2 is the electric field strength associated with one photon in the light mode (with V its effective mode volume). The figure of merit for a material is thus its dipole density µ 2 N/V , with organic materials presenting a particularly favorable case due to their large dipole moments and high possible density. In addition, the large binding energies of Frenkel excitons in organic materials make them stable at room-temperature. This has allowed reaching the strong-coupling regime with a large variety of electromagnetic (EM) modes, 3 such as cavity photons, 4-8 surface plasmon polaritons, [9][10][11][12] surface lattice resonances, 13,14 and localized surface plasmons. 15,16 Typical Rabi frequencies range from ≈ 100 meV to more than 1 eV, a significant fraction of the uncoupled transition energy, for a wide range of organic materials such as dye molecules, J-aggregates, and even carbon nanotubes. 17,18 By using localized surface plasmon modes with extreme-subwavelength light confinement, recent experiments have achieved strong coupling at room temperature even down to the single-emitter level. [19][20][21] The mixed light-matter character of organic polaritons enables a large number of interesting applications (see Ref. 22 for a recent review discussing polaritonic devices, including a comparison between organic and inorganic materials), such as polariton lasing and/or Bose-Einstein condensation 23-25 including nonlinear ...