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Progress of Theoretical Physics

A Theory of Frenkel Excitons Using a Two-Level-Atom Model

Shôzô Takeno, Mahito Mabuchi

Published Dec 1, 1973• 27 citations
Publisher

Abstract

A formal, regorous theory of Frenkel excitons interacting with an external electromagnetic field is doveloped within the framework of a two-level-atom model in which the dipole approximation is employed in describing the atom-field (taken as a c-number) interaction. The model exciton Hamiltonian is shown to be identical in form with the Heisenberg model Hamiltonian for S=1/2 spins with anisotropic long-range exchange interactions. Instead of treating excitons as a non-ideal Bose gas, atomic polarization operators and level population defference are taken up as two fundamental quantities to describe Frenkel excitons. A pair of equations satisfied by these two quantities are derived. It is shown that Frenkel excitons are generally expressed as quantum-mechanical nonlinear polarization waves, the nonlinearity being characterized by the level population. A discussion is given on the interrelationship between such polarization waves and those derivable from the classical Drude-Lorentz model. With the aid of several approximation procedures similar to those employed in nonlinear optics, a set of equations describing nonlinear exciton-photon coupled modes are derived. Brief discussion is given on the eigenfrequencies of nonlinear Frenkel excitons and nonlinear polaritons. The existence of nonlinear exciton-photon coupled modes whose properties are different from those of polariton modes is suggested.

DOI
10.1143/ptp.50.1848

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A formal, regorous theory of Frenkel excitons interacting with an external electromagnetic field is doveloped within the framework of a two-level-atom model in which the dipole approximation is employed in describing the atom-field (taken as a c-number) interaction. The model exciton Hamiltonian is shown to be identical in form with the Heisenberg model Hamiltonian for S=1/2 spins with anisotropic long-range exchange interactions. Instead of treating excitons as a non-ideal Bose gas, atomic polarization operators and level population defference are taken up as two fundamental quantities to describe Frenkel excitons. A pair of equations satisfied by these two quantities are derived. It is shown that Frenkel excitons are generally expressed as quantum-mechanical nonlinear polarization waves, the nonlinearity being characterized by the level population. A discussion is given on the interrelationship between such polarization waves and those derivable from the classical Drude-Lorentz model. With the aid of several approximation procedures similar to those employed in nonlinear optics, a set of equations describing nonlinear exciton-photon coupled modes are derived. Brief discussion is given on the eigenfrequencies of nonlinear Frenkel excitons and nonlinear polaritons. The existence of nonlinear exciton-photon coupled modes whose properties are different from those of polariton modes is suggested.
A quantum theory of nonlinear excitations in a matter-photon system is developed by generalizing the conventional two-level-atom model of a matter in several directions, on the assumption that the overlapping of atomic wave functions on different atomic sites is negligible.The model matter Hamiltonian is shown to be expressible in a generalized form' of the Heisenberg model Hamiltonian with anisotropic long-range exchange interactions with spin operators replaced by quasi-Pauli operators.From approxirpate formal solutions of a set of nonlinear equations satisfied by the quasi-Pauli operators ~nd photon operators, brief discussion is given on nonlinear Frenkel excitons and nonlinear exciton-photon coupled modes.An attempt is made to formulate a theory of higher-order nonlinear physical properties of the matter-photon system by including interactions of magnetic as •well as electric dipoles of atoms with photons.A brief discussion is also given on the coherence properties. of the matter-photon system which are characterized by the simultaneo~s existence of •a photon coherent state and an atomic-polarization coherent state.*> Throughout this paper, we will often use a simplified .notation l, rather than l 1, whenever appropriate, to avoid the use of complicated symbols.Also, the complex conjugate of a quantity• A is denoted by A*.
Interactions of nonlinear Frenkel excitons with an intense external radiation field (rf) are studied by taking the atomic polarization, the atomic population difference and the electric field as a set of variables to study the coherence and nonlinearity properties of the exciton-rf system. To equations for these quantities, terms are added phenomenologicaly to take care of pumping and dissipative effects. Two kinds of solutions are obtained under certain conditions, one representing the existence of the stationary coherent polarization and the macroscopic number of photons with wave number equal to that of the excitons and another envelope-kink-like, steady exciton-rf coupled modes around the stationary coherent states
Dynamical and statistical behaviors of Frenkel excitons in a matter system consisting of N two-level-atoms and interacting with an external field are studied with the molecular field and random phase approximations. Existence of a phase transition is suggested both in the exciton system and exciton-photon coupled system. This phase transition is the second order transition whose order parameter is the polarizability. A new type of condensation of the photon-exciton coupled wave, in which a macroscopic number of excitons and photons participate, has been found as a result of appreciable contribution of photons to the phase transition. When the incident light is coherent, the condition of phase transition is modified by photon induced exciton-exciton interaction. The energy dispersion of elementary excitations is derived.
Theories which have been used to describe the quantized electromagnetic field interacting with a nonlinear dielectric medium are either phenomenological or derived by quantizing the macroscopic Maxwell equations. Here we take a different approach and derive a Hamiltonian describing interacting fields from one which contains both field and matter degrees of freedom. The medium is modeled as a collection of two-level atoms, and these interact with the electromagnetic field. The atoms are grouped into effective spins and the the Holstein-Primakoff representation of the spin operators is used to expand them in inverse powers of the total spin. When the lowest order term of the interaction is combined with the free atomic and field Hamiltonians, a Hamiltonian describing a theory of noninteracting polaritons results. When higher order terms are expressed in terms of polariton operators standard nonlinear optical interactions emerge. These are then compared to the results of phenomenological and macroscopic theories. The theory is also used to derive an effective Hamiltonian describing counterpropagating modes in a nonlinear medium.
Quantum electrodynamics of two identical two-level atoms placed within a frequency dispersive medium whose polariton spectrum has a gap due to photon coupling to a medium excitation (exciton, optical phonon, etc.) is studied within the framework of the dipole resonance (rotating-wave) approximation. For finite interatomic distances a polariton-atom bound state lying within the polaritonic gap is shown to be split into a doublet due to an effective atom-atom interaction. Evaluating the splitting as a function of the interatomic separation, we estimate a width of a polariton-impurity band when a system of spatially correlated atoms is present. The results obtained for the case of two atoms are then generalized to the case of an atomic chain (a one-dimensional atomic lattice). The equations describing a propagation of a band polariton are derived and the expressions for the band polariton spectrum and its effective mass are obtained. The model under consideration has quite a general structure and is applied to the case of photonic-band-gap materials as well. Numerical calculations are presented for SiC semiconductors.