The role of dark polariton states for electronic strong coupling in molecules

• URL: http://arxiv.org/abs/2504.20798v1
• Date: Tue, 29 Apr 2025 14:13:07 GMT
• Title: The role of dark polariton states for electronic strong coupling in molecules
• Authors: Lucas Borges, Thomas Schnappinger, Markus Kowalewski,
• Abstract summary: Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities.<n>We analyze the higher excitation of the Tavis-Cummings model along with a three-level system that resembles photochemical reactions.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities, as demonstrated in numerous experiments over the last few years. These experiments are typically interpreted in terms of the Jaynes-Cummings or Tavis-Cummings models under the assumption that the molecular ensemble is only excited by a single photon. In such a model, two polariton states compete with an overwhelming number of dark states, inhibiting polaritonic reactions entropically. We analyze the higher excitation manifolds of the Tavis-Cummings model along with a three-level system that resembles photochemical reactions. We demonstrate that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable.

Related papers

• The role of spectator modes in the quantum-logic spectroscopy of single trapped molecular ions [41.94295877935867]
  We study the role of spectator modes not directly involved in a measurement protocol relying on a state-dependent optical-dipole force. We identify a Debye-Waller-type effect that modifies the response of the two-ion string to the force and show that cooling all normal modes of the string allows for the detection of the rovibrational ground state of a N$+$ molecular ion.
  arXiv  Detail & Related papers  (2025-04-03T14:37:24Z)
• Optical lattice quantum simulator of dynamics beyond Born-Oppenheimer [45.29832252085144]
  We propose a platform based on ultra-cold fermionic molecules trapped in optical lattices to simulate nonadiabatic effects.<n>We benchmark our proposal by studying the scattering of an electron or a proton against a hydrogen atom.
  arXiv  Detail & Related papers  (2025-03-30T14:46:26Z)
• Room-temperature optical spin polarization of an electron spin qudit in a vanadyl -- free base porphyrin dimer [35.34500698545813]
  Photoexcited organic chromophores appended to molecular qubits can serve as a source of spin initialization or multi-level qudit generation for quantum information applications. Time-resolved electron paramagnetic resonance (TREPR) experiments carried out at both 85 K and room temperature reveal the formation of a long-lived spin-polarized quartet state. Exploiting this phenomenon affords the possibility of using photoinduced triplet states in porphyrins for quantum information as a resource to polarize and magnetically couple molecular electronic or nuclear spin qubits and qudits.
  arXiv  Detail & Related papers  (2024-08-04T18:08:20Z)
• Ultra-strong trion-polaritons [0.0]
  Trion-polaritons (TP) in microcavity semiconductors are a promising avenue for realizing strong polariton interactions and many-body polariton phases. We develop a quantum field theoretical formalism to study the formation of trion-polaritons in a microcavity semiconductor doped with itinerant electrons.
  arXiv  Detail & Related papers  (2024-03-15T21:26:35Z)
• 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)
• Driving chemical reactions with polariton condensates [0.0]
  We study the effect of vibrational polariton condensation on the kinetics of electron transfer processes. Compared with excitation with infrared laser sources, the condensate changes the reaction yield significantly. Our results offer tantalizing opportunities to use condensates for driving chemical reactions.
  arXiv  Detail & Related papers  (2021-06-23T04:57:35Z)
• Catalysis by Dark States in Vibropolaritonic Chemistry [0.0]
  Experimental changes in thermally-activated reaction kinetics due to polariton formation appear entropically unlikely. We show that the overlooked dark modes, while parked at the same energy as bare molecular vibrations, are robustly delocalized across $sim$2-3 molecules.
  arXiv  Detail & Related papers  (2021-04-15T03:29:03Z)
• Superreaction: the collective enhancement of a reaction rate by molecular polaritons in the presence of energy fluctuations [0.0]
  Molecular polaritons are hybrid states of light and matter formed by the strong coupling between molecular electronic or vibrational excitations and an optical cavity. We show that, by exploiting the collective character of molecular polaritons, a superreaction can be realized. The underlying mechanism is shown to be the enhancement of quantum coherence between different donors as the light-matter interaction becomes stronger.
  arXiv  Detail & Related papers  (2021-03-30T08:46:37Z)
• Resonant enhancement of three-body loss between strongly interacting photons [47.30557822621873]
  Rydberg polaritons provide an example of a rare type of system where three-body interactions can be as strong or even stronger than two-body interactions. We show how the shape and strength of dissipative three-body forces can be universally enhanced for Rydberg polaritons.
  arXiv  Detail & Related papers  (2020-10-19T18:21:49Z)
• Demonstration of dipolar-induced enhancement of parametric effects in polariton waveguides [40.96261204117952]
  Exciton-polaritons are hybrid light-matter excitations arising from the non-fluidative coupling of a photonic mode and an excitonic resonance. We show that dipolar interactions can be used to enhance parametric effects such as self-phase modulation in waveguide polaritons.
  arXiv  Detail & Related papers  (2020-05-22T20:45:31Z)
• Optically pumped spin polarization as a probe of many-body thermalization [50.591267188664666]
  We study the spin diffusion dynamics of 13C in diamond, which we dynamically polarize at room temperature via optical spin pumping of engineered color centers. We find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength. Our results open intriguing opportunities to study the onset of thermalization in a system by controlling the internal interactions within the bath.
  arXiv  Detail & Related papers  (2020-05-01T23:16:33Z)
• Polarized Fock States for Polariton Photochemistry [0.0]
  We use the polarized Fock states to describe the coupled molecule-cavity hybrid system in quantum electrodynamics. The molecular permanent dipoles polarize the photon field by displacing its vector potential, leading to non-orthogonality between the Fock states of two different polarized photon fields.
  arXiv  Detail & Related papers  (2020-05-01T03:51:19Z)

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.