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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Manipulation of spectra of output radiation of dopant energetic donor-acceptor pair by pump light power

A E Dmitriev, Yelena I. Dmitriyeva, Oleg M. Parshkov, Nina E. Popova

Published May 26, 1999• 1 citation
Publisher

Abstract

Theoretical treatment of the effects of external pulse field on the emission and absorption of two impurity centers has been attempted. Good overlapping of emission band of one center (donor of energy) with the absorption band of another center (acceptor of energy) is assumed, so that radiative and non-radiative energy transfer may take place. Mathematical model is based on the system of reduced Maxwell equations for magnitudes of field components and Bogolubov's equations for elements of multiparticle density matrix of donor-acceptor complex. Numerical solution is obtained for NaCl:Cu, Mn and KCl:Pb,Eu crystals. These materials are differing in the value of transition dipole moment of acceptor absorption. It is low for the first medium while for KCl:Pb,Eu it is comparable to that one for the donor emission. It turns out that in the case of low value of transition dipole moment the luminescence of both components of donor-acceptor pair takes place. On the contrary, only acceptor emission exists in the case of high value of transition dipole moment of acceptor when the pump intensity is low. Simultaneous luminescence of donor and acceptor occurs when pump intensity is enough. So, in the systems of such kind the emission may be changed over from one frequency to another through the power level of pump radiation.

DOI
10.1117/12.349233

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Theoretical treatment of the effects of external pulse field on the emission and absorption of two impurity centers has been attempted. Good overlapping of emission band of one center (donor of energy) with the absorption band of another center (acceptor of energy) is assumed, so that radiative and non-radiative energy transfer may take place. Mathematical model is based on the system of reduced Maxwell equations for magnitudes of field components and Bogolubov's equations for elements of multiparticle density matrix of donor-acceptor complex. Numerical solution is obtained for NaCl:Cu, Mn and KCl:Pb,Eu crystals. These materials are differing in the value of transition dipole moment of acceptor absorption. It is low for the first medium while for KCl:Pb,Eu it is comparable to that one for the donor emission. It turns out that in the case of low value of transition dipole moment the luminescence of both components of donor-acceptor pair takes place. On the contrary, only acceptor emission exists in the case of high value of transition dipole moment of acceptor when the pump intensity is low. Simultaneous luminescence of donor and acceptor occurs when pump intensity is enough. So, in the systems of such kind the emission may be changed over from one frequency to another through the power level of pump radiation.
A theoretical study is made of the influence of changes in the relaxation of a three-level system in a resonance field on the dispersion, absorption, and difference between the populations of levels activated by noncoherent pumping. This change in the relaxation is due to a tendency of a thermal reservoir to create an additional difference between the populations of quasienergy states that appear under the influence of the resonance field. It is shown that as a consequence there is a considerable change in the nature of the interaction with the radiation field in laser crystals with three-level active centers when the pump power is close to the threshold. The lasing conditions are found subject to such changes. It is shown that the threshold pump power can be reduced in this case to a value at which the difference between the populations of the active levels vanishes and lasing appears because of an inversion of the populations in a system of quasienergy levels. Under transient conditions the lasing frequency near the threshold should then depend on the pump
We treat the interaction between an electromagnetic radiation bath and a material system in the semi-classical picture: the radiation is treated according to the Maxwell equations, but the process of emission/absorption is described through the concept of a photon; on the other hand, the material system is modelled according to quantum mechanics, assuming a discrete two-level energy spectrum. This very simple model allows one to elaborate the elementary theory of the absorption/emission coefficients, both for the spontaneous and for the stimulated processes which will be described within the electric dipole approximation. Selection rules for allowed transitions are eventually obtained and the nature of high-order transition is briefly outlined. Finally, a qualitative description of the light amplification by stimulated emission of radiation is presented.
A new theoretical model describing the emission and absorption dynamics in an ensemble of molecules under intense coherent pulsed pumping is developed on the basis of the concepts of cooperative light-induced luminescence (CLIL). The CLIL development is described within the framework of formalism of the system density matrix in the space of photon wave functions. It is shown that the fast growth of CLIL relates to the development of coherent states of the quantum field in the area of efficient cooperative interactions of molecules (coherence volume). A system of equations for the calculation of CLIL energy, population of excited states, and optical absorption of the system in dependence on the laser pump energy density is solved. The theoretical results obtained are in good agreement with the experimental data.
The coherent energy transfer efficiency of a pair of two-level atoms is studied theoretically and its mathematical expression has been deduced. The problem of atoms coherent energy transfer theory is treated by quantum perturbation theory and equivalent method replacing atomic dipole field with light field of the same frequency. The detuning between the donor atom transition frequency and the acceptor atom transition frequency has been studied in the theory. With the increase of the detuning of the two-atomic transition frequency, the energy transfer efficiency decays rapidly. In the case of two-atomic transition frequency resonance, the coherent resonance energy transfer efficiency is directly proportional to the square of the sine of the minus three power of the distance between two atoms and the energy transfer efficiency is periodically decaying over time. The coherent resonance energy transfer efficiency is inversely proportional to the six power of the distance between the two atoms in the first-order approximation.