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Facundo Tarasi1, Tchavdar N Todorov2, Carlos M Bustamante3

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This study introduces a quantum-electrodynamics model for electron dynamics interacting with photon and phonon baths. It reveals how semiclassical emission, dependent on coherences, contributes to collective behavior in materials like trans-polyacetylene.

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Area of Science:

  • Quantum dynamics
  • Condensed matter physics
  • Quantum electrodynamics

Background:

  • Describing electron dynamics in quantum systems requires accounting for energy exchange with photon and phonon baths.
  • Existing models often simplify interactions, potentially missing crucial quantum effects.

Purpose of the Study:

  • To develop a quantum-electrodynamics (QED) approach for electron dynamics coupled to photon and phonon baths.
  • To investigate the role of semiclassical emission within a full QED framework.
  • To analyze the response of the Su-Schrieffer-Heeger model in trans-polyacetylene to laser irradiation.

Main Methods:

  • Utilizing a dissipative quantum Liouville equation in the Redfield form.
  • Incorporating two driving terms for radiative and vibrational relaxation.
  • Analyzing the contributions of semiclassical emission and quantum driving terms.

Main Results:

  • A QED term was found to replicate semiclassical treatment of dissipated power.
  • Semiclassical emission depends on electronic coherences, while other QED terms depend on excited populations.
  • The Su-Schrieffer-Heeger model showed stepwise relaxation and subradiant states under pulsed laser excitation.
  • Vibrational dissipation led to rapid population of the conduction band minimum and a redshifted emission spectrum.

Conclusions:

  • The developed QED approach accurately describes electron dynamics with photon and phonon interactions.
  • Semiclassical emission is crucial for understanding collective quantum phenomena.
  • Laser irradiation induces distinct relaxation dynamics and spectral shifts depending on pulse characteristics and dissipation mechanisms.