Elsevier

Chemical Physics

Volume 173, Issue 2, 15 June 1993, Pages 123-132
Chemical Physics

A quantum electrodynamical theory of induced circularly polarised luminescence

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Abstract

A theory of molecule-induced circulary polarised emission for a luminescent chiral-achiral pair employing the multipolar Hamiltonian in both the Schrödinger and Heisenberg formulations of Coulomb gauge quantum electrodynamics is presented. Chirality is induced in an achiral species via intermolecular coupling with a chiral molecule. In the Schrödinger picture time-dependent perturbation theory is used with intermolecular interaction involving virtual photon exchange. In the Heisenberg framework the electric dipole moment of the achiral molecule couples to the time-dependent Maxwell fields of the chiral source. The equivalence of the matrix element obtained for the process using both approaches in demonstrated. The transition rate is then derived for the differential spontaneous emission of left- and right-circularly polarised radiation. Various orientational averages are computed and the dependence of the rate expression on intermolecular separation is investigated.

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