Classical polarizable approaches have become the gold standard for simulating complex systems and processes in the condensed phase. These methods describe intrinsically dissipative polarizable media, requiring a formal definition within the framework of open quantum systems. We present a Hamiltonian formulation for the quantum dynamics of polarizable sources based on a generalized theory of the damped harmonic oscillator, using pseudoboson theory to characterize their coherent state dynamics. We then apply our theory to the study of the optical response of two plasmonic systems. Furthermore, by exploiting the phase-space formulation of quantum mechanics and the integrability of quadratic Hamiltonians, we derive a self-consistent relation for the emitted electric field of the polarizable medium under the semiclassical approximation, based on exact formulas for medium polarization. Finally, we derive the master equation describing the open dynamics of a quantum system interacting with the quantum polarizable medium, along with analytical expressions for correlation functions calculated over arbitrary Gaussian states.

Quantum dynamics of dissipative polarizable media

Rodriguez, Frank Ernesto Quintela
;
Lafiosca, Piero;Giovannini, Tommaso;Cappelli, Chiara
2025

Abstract

Classical polarizable approaches have become the gold standard for simulating complex systems and processes in the condensed phase. These methods describe intrinsically dissipative polarizable media, requiring a formal definition within the framework of open quantum systems. We present a Hamiltonian formulation for the quantum dynamics of polarizable sources based on a generalized theory of the damped harmonic oscillator, using pseudoboson theory to characterize their coherent state dynamics. We then apply our theory to the study of the optical response of two plasmonic systems. Furthermore, by exploiting the phase-space formulation of quantum mechanics and the integrability of quadratic Hamiltonians, we derive a self-consistent relation for the emitted electric field of the polarizable medium under the semiclassical approximation, based on exact formulas for medium polarization. Finally, we derive the master equation describing the open dynamics of a quantum system interacting with the quantum polarizable medium, along with analytical expressions for correlation functions calculated over arbitrary Gaussian states.
2025
Settore CHEM-02/A - Chimica fisica
Atomic & molecular structure; Interatomic & molecular potentials; Light-matter interaction; Atomic systems; Electronically polarized systems; Dipole approximation; Methods in electromagnetism; Quantum master equation
   MOdeling multiscala di molecole elettRonicamente Eccitate in vicinanza di nanostrutture PLASMONiche
   MORE-Plasmon
   MUR
   PNR2015-2020
   R20YTA2BKZ
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11384/154684
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