Scaling law for Kasha's rule in photoexcited molecular aggregates

• URL: http://arxiv.org/abs/2304.10236v3
• Date: Fri, 1 Dec 2023 09:53:15 GMT
• Title: Scaling law for Kasha's rule in photoexcited molecular aggregates
• Authors: Raphael Holzinger, Nico S. Bassler, Helmut Ritsch and Claudiu Genes
• Abstract summary: We study the photophysics of molecular aggregates from a quantum optics perspective. We focus on deriving scaling laws for the fast non-radiative relaxation of collective electronic excitations, referred to as Kasha's rule.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We study the photophysics of molecular aggregates from a quantum optics perspective, with emphasis on deriving scaling laws for the fast non-radiative relaxation of collective electronic excitations, referred to as Kasha's rule. Aggregates exhibit an energetically broad manifold of collective states with delocalized electronic excitations originating from near field dipole-dipole exchanges between neighboring monomers. Photo-excitation at optical wavelengths, much larger than the monomer-monomer average separation, addresses almost exclusively symmetric collective states, which for an arrangement known as H-aggregate, show an upward hypsochromic shift. The extremely fast subsequent non-radiative relaxation via intramolecular vibrational modes populates lower energy, subradiant states, resulting in an effective inhibition of fluorescence. Our analytical treatment allows for the derivation of an approximate scaling law of this relaxation process, linear in the number of available low energy vibrational modes and directly proportional to the dipole-dipole interaction strength between neighbouring monomers.

Related papers

• Influence of strong molecular vibrations on decoherence of molecular polaritons [0.0]
  We show that strong vibrational interactions give rise to multi phonon processes and suppress the light--matter coupling. We also find that vibrational Lamb shifts can substantially modify the polariton energies in the strong light--matter coupling limit.
  arXiv  Detail & Related papers  (2024-07-23T13:58:25Z)
• Dipole-dipole interactions mediated by a photonic flat band [44.99833362998488]
  We study the photon-dipole interactions between emitters dispersively coupled to the photonic analogue of a flat band (FB) We show that the strength of such photon-mediated interactions decays exponentially with distance with a characteristic localization length. We find that the localization length grows with the overlap between CLSs according to an analytically-derived universal scaling law valid for a large class of FBs both in 1D and 2D.
  arXiv  Detail & Related papers  (2024-05-30T18:00:05Z)
• Directional spontaneous emission in photonic crystal slabs [49.1574468325115]
  Spontaneous emission is a fundamental out-of-equilibrium process in which an excited quantum emitter relaxes to the ground state due to quantum fluctuations. One way to modify these photon-mediated interactions is to alter the dipole radiation patterns of the emitter, e.g., by placing photonic crystals near them. Our study delves into the interaction between these directional emission patterns and the aforementioned variables, revealing the untapped potential to fine-tune collective quantum optical phenomena.
  arXiv  Detail & Related papers  (2023-12-04T15:35:41Z)
• Propagation of light in cold emitter ensembles with quantum position correlations due to static long-range dipolar interactions [0.0]
  We analyze the scattering of light from dipolar emitters whose disordered positions exhibit correlations induced by static, long-range dipole-dipole interactions. The quantum-mechanical position correlations are calculated for zero temperature bosonic atoms or molecules using variational and diffusion quantum Monte Carlo methods. For stationary atoms in dense ensembles in the limit of low light intensity, the simulations yield solutions for the optical responses to all orders of position correlation functions that involve electronic ground and excited states.
  arXiv  Detail & Related papers  (2023-10-24T20:02:40Z)
• Photoinduced prethermal order parameter dynamics in the two-dimensional large-$N$ Hubbard-Heisenberg model [77.34726150561087]
  We study the microscopic dynamics of competing ordered phases in a two-dimensional correlated electron model. We simulate the light-induced transition between two competing phases.
  arXiv  Detail & Related papers  (2022-05-13T13:13:31Z)
• Correlated steady states and Raman lasing in continuously pumped and probed atomic ensembles [68.8204255655161]
  We consider an ensemble of Alkali atoms that are continuously optically pumped and probed. Due to the collective scattering of photons at large optical depth, the steady state of atoms does not correspond to an uncorrelated tensor-product state. We find and characterize regimes of Raman lasing, akin to the model of a superradiant laser.
  arXiv  Detail & Related papers  (2022-05-10T06:54:54Z)
• Tuning long-range fermion-mediated interactions in cold-atom quantum simulators [68.8204255655161]
  Engineering long-range interactions in cold-atom quantum simulators can lead to exotic quantum many-body behavior. Here, we propose several tuning knobs, accessible in current experimental platforms, that allow to further control the range and shape of the mediated interactions.
  arXiv  Detail & Related papers  (2022-03-31T13:32:12Z)
• Cooperative subwavelength molecular quantum emitter arrays [0.0]
  Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective excitations with super- or subradiant character. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles. We extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence.
  arXiv  Detail & Related papers  (2022-03-09T19:00:59Z)
• Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach [68.8204255655161]
  hierarchy of pure states (HOPS) provides a formally exact solution based on local, trajectories. Exploiting the localization of HOPS for the simulation of absorption spectra in large aggregares requires a formulation in terms of normalized trajectories.
  arXiv  Detail & Related papers  (2021-11-01T16:59:54Z)
• A superatom picture of collective nonclassical light emission and dipole blockade in atom arrays [0.0]
  We show that two-time, second-order correlations of scattered photons from planar arrays and chains of atoms display nonclassical features. For targeted subradiant modes, nonclassical nature of emitted light can be dramatically enhanced even compared with that of a single atom.
  arXiv  Detail & Related papers  (2020-05-08T21:54:04Z)
• Understanding Radiative Transitions and Relaxation Pathways in Plexcitons [0.0]
  Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of cavity quantum electrodynamics. We show that while the metal is responsible for destroying the coherence of the excitation, the molecular aggregate significantly participates in dissipating the energy. We show that the dynamics beyond a few femtoseconds has to be cast in the language of hot electron distributions and excitons.
  arXiv  Detail & Related papers  (2020-02-13T17:20:29Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.