General calculation of 4f−5d4f-5d transition rates for rare-earth ions using many-body perturbation theory

The $4f-5d$ transition rates for rare-earth ions in crystals can be calculated with an effective transition operator acting between model $4f^N$ and $4f^{N-1}5d$ states calculated with effective Hamiltonian, such as semi-empirical crystal Hamiltonian. The difference of the effective transition operator from the original transition operator is the corrections due to mixing in transition initial and final states of excited configurations from both the center ion and the ligand ions. These corrections are calculated using many-body perturbation theory. For free ions, there are important one-body and two-body corrections. The one-body correction is proportional to the original electric dipole operator with magnitude of approximately 40% of the uncorrected electric dipole moment. Its effect is equivalent to scaling down the radial integral \ME {5d} r {4f}, to about 60% of the uncorrected HF value. The two-body correction has magnitude of approximately 25% relative to the uncorrected electric dipole moment. For ions in crystals, there is an additional one-body correction due to ligand polarization, whose magnitude is shown to be about 10% of the uncorrected electric dipole moment.Comment: 10 pages, 1 figur

Calculation of single-beam two-photon absorption transition rate of rare-earth ions using effective operator and diagrammatic representation

Effective operators needed in single-beam two-photon transition calculations have been represented with modified Goldstone diagrams similar to the type suggested by Duan and co-workers [J. Chem. Phys. 121, 5071 (2004) ]. The rules to evaluate these diagrams are different from those for effective Hamiltonian and one-photon transition operators. It is verified that the perturbation terms considered contain only connected diagrams and the evaluation rules are simplified and given explicitly.Comment: 10 preprint pages, to appear in Journal of Alloys and Compound

Conservation of connectivity of model-space effective interactions under a class of similarity transformation

Effective interaction operators usually act on a restricted model space and give the same energies (for Hamiltonian) and matrix elements (for transition operators etc.) as those of the original operators between the corresponding true eigenstates. Various types of effective operators are possible. Those well defined effective operators have been shown being related to each other by similarity transformation. Some of the effective operators have been shown to have connected-diagram expansions. It is shown in this paper that under a class of very general similarity transformations, the connectivity is conserved. The similarity transformation between hermitian and non-hermitian Rayleigh-Schr\"{o}dinger perturbative effective operators is one of such transformation and hence the connectivity can be deducted from each other.Comment: 12 preprint page

Calculation of single-beam two-photon absorption rate of lanthanides: effective operator method and perturbative expansion

Perturbative contributions to single-beam two-photon transition rates may be divided into two types. The first, involving low-energy intermediate states, require a high-order perturbation treatment, or an exact diagonalization. The other, involving high energy intermediate states, only require a low-order perturbation treatment. We show how to partition the effective transition operator into two terms, corresponding to these two types, in such a way that a many-body perturbation expansion may be generated that obeys the linked cluster theorem and has a simple diagrammatic representation.Comment: 11 preprint page

Local Field effects on the radiative lifetime of emitters in surrounding media: virtual- or real-cavity model?

For emitters embedded in media of various refractive indices, different macroscopic or microscopic theoretical models predict different dependencies of the spontaneous emission lifetime on refractive index. Among those models are the two most promising models: the virtual-cavity model and the real-cavity model. It is a priori not clear which model is more relevant for a given situation. By close analysis of the available experimental results and examining the assumptions underlying the two models, we reach a consistent interpretation of the experimental results and give the criteria which model should apply for a given situation.Comment: 12 pages with 4 figure