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Mapping Molecular Polariton Transport via Pump-Probe Microscopy.

Piper Fowler-Wright1, Michael Reitz1, Joel Yuen-Zhou1

  • 1Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093, United States.

Nano Letters
|May 5, 2026
PubMed
Summary

We show how to model molecular polariton transport in optical cavities using pump-probe spectroscopy. This method reveals how molecular dephasing and dark excitons influence polariton movement and velocity.

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Area of Science:

  • Condensed Matter Physics
  • Quantum Optics
  • Spectroscopy

Background:

  • Molecular polaritons are hybrid light-matter quasiparticles confined in optical cavities.
  • Understanding their transport properties is crucial for developing novel optoelectronic devices.
  • Current methods often lack the resolution to fully characterize complex transport dynamics.

Purpose of the Study:

  • To develop a microscopic modeling approach for extracting molecular polariton transport properties.
  • To extend semiclassical cavity spectroscopy to multimode light-matter interactions.
  • To analyze the influence of molecular dephasing and exciton populations on polariton transport.

Main Methods:

  • Mean-field treatment of the light-matter Hamiltonian.
  • Perturbative expansion of light and matter components.
Keywords:
group velocity renormalizationlight−matter interactionorganic microcavitiespolariton transportstrong couplingultrafast spectroscopy

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  • Spatial coarse-graining and simulation of pump-probe microscopy experiments.

    • Main Results:

    • Computed differential transmission spectra revealing spatially resolved transient dynamics.
    • Demonstrated that molecular dephasing and dark excitons drive polariton subgroup velocity transport.
    • Correlated velocity renormalization with excitonic weight and dephasing rates.

    Conclusions:

    • The developed model provides full access to spatially resolved transient spectra.
    • Spectroscopic observables are essential for characterizing transport in polaritonic systems.
    • Transport velocity is tunable via molecular dephasing, exciton hopping, and annihilation rates.