Effects of the electron-phonon interaction for rare earth ions (RE) in crystals are multi-phonon relaxation, vibronic bands, band broadening depending on temperature or non-resonant energy transfer assisted by phonons. Since the Stark splitting for RE ions are of the order of lattice phonon energy, it could arise and other related effects, especially in the approximation of quasi-resonant processes. If the distance between two Stark levels is close to the region of resonance phonon spectrum, then electron-phonon interaction creates mixed vibronic states, which causes changes in the optical spectral lines (widening, asymmetry, splitting or displacement). The modeling of interaction of the electron-phonon resonance for RE ion Yb3+ in three different laser crystals is the purpose of this paper. Keywords: electron-phonon interaction, rare earth ions, adaptive application.
Effects of the electron-phonon interaction for rare earth ions (RE) in crystals are multi-phonon relaxation, vibronic bands, band broadening depending on temperature or non-resonant energy transfer assisted by phonons. Since the Stark splitting for RE ions are of the order of lattice phonon energy, it could arise and other related effects, especially in the approximation of quasi-resonant processes. If the distance between two Stark levels is close to the region of resonance phonon spectrum, then electron-phonon interaction creates mixed vibronic states, which causes changes in the optical spectral lines (widening, asymmetry, splitting or displacement). The modeling of interaction of the electron-phonon resonance for RE ion Yb3+ in three different laser crystals is the purpose of this paper. Keywords: electron-phonon interaction, rare earth ions, adaptive application.
A systematic analysis of decoherence rates due to electron–phonon interactions for optical transitions of rare-earth dopant ions in crystals is presented in the frame of the point charge model. For this model, the large value of any one of the matrix elements of the unit tensor operator U ( k ) of rank k for transitions within the 4f-electronic configuration, viz. U2, U4 or U6, is enough to ensure the strong optical transition between different levels, while the Stark–Stark transitions within the multiplet can be characterized by the matrix element U2 alone, the influence of elements U4, U6 being of much smaller order of magnitude and neglected. The circumstance that exactly such Stark–Stark transitions within the multiplet define the efficiency of electron–phonon interaction and, consequently, the decoherence rate (except for the case of lowest, less than approximately 2–4 K, temperatures), enables selection of optical transitions which are strong enough and at the same time are characterized by relatively small decoherence rates. Correspondingly, these optical transitions, provided that they lie in an appropriate spectral range and the gap to the nearest neighboring energy level is large enough (>500 cm−1) to prevent eventual fast phonon-assisted relaxation, should be considered as prospective for subsequent use in quantum informatics processing and communication. The list of such pre-selected transitions is given; the applicability area and limitations of our approach are discussed.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,
We describe a general numerical method for calculating short-pulse laser propagation in rare-earth-doped materials, which are very important as gain materials for solid-state lasers, fiber lasers and optical amplifiers. The split-step, finite difference method simultaneously calculates changes in the laser pulse as it propagates through the material and calculates the dynamic populations of the rare-earth energy levels at any position within the material and for times during and after the laser pulse has passed through the material. Many traditional theoretical and numerical analyses of laser pulse propagation involve approximations and assumptions that limit their applicability to a narrow range of problems. Our numerical method, however, is more comprehensive and includes the processes of single- and multi-photon absorption, excited state absorption (ESA), energy transfer, upconversion, stimulated emission, cross relaxation, radiative relaxation and non-radiative relaxation. In the models, the rare-earth dopants can have an arbitrary number of energy levels. We are able to calculate the electron population density of every electronic level as a function of, for example, pulse energy, dopant concentration and sample thickness. We compare our theoretical results to published experimental results for rare-earth ions such as Er3+, Yb3+, Tm3+ and Ho3+.
The enhanced laser cooling performance of rare-earth-ion-doped nanocrystalline powders is predicted, compared to the bulk material, using Yb3+:Y2O3 as the model material. This is achieved by enhancing the off-resonance, phonon-assisted absorption, which is proportional to the three factors considered in this paper: the dopant concentration, the pumping field energy, and the excitation coefficient. Using the energy transfer theory for concentration quenching, the optimum concentration corresponding to the maximum cooling power is found to be considerably larger than the currently used value, suggesting noticeable enhancement effects for laser cooling. The pumping field energy is enhanced in random nanopowders compared with bulk crystals under the same irradiation, due to the multiple scattering of photons. Photons are thus localized in the medium and do not propagate through, increasing the photon absorption of the pumping beam (and it is shown that the reabsorption of the fluorescence is negligible). Using molecular dynamics simulations, the phonon density of states (DOS) of the nanopowder is calculated, and found to have broadened modes, and extended small tails at low and high frequencies. The second-order electronic transition rate for the anti-Stokes luminescence is calculated using the Fermi golden rule, which includes the influence of this phonon DOS, and is shown to have enhancement effects on the laser cooling efficiency using nanopowders. It is finally concluded that these three enhancement mechanisms are essentially to increase the population of the three participating carriers (electron, photon, and phonon) in the interacting volume, and this also points out directions for enhancing laser cooling performance in bulk materials.
A vibronic model of laser cooling for crystals doped with Yb3+ ions is proposed. The model involves the stimulated Raman adiabatic passage pumping through dipole-allowed 4f–5d transitions, electron transitions between Stark-split sublevels due to vibronic interaction, and anti-Stokes fluorescence from the excited ion state. Dynamics of the cooling process are described by the density matrix formalism. It is shown that the cooling power in the case of vibronic interaction is higher at least by a factor of 3.4 compared to the case of electron–phonon interaction. In the proposed model, an increase in the cooling power yields deeper and faster refrigeration of a crystal doped with Yb3+ ions. Estimations show that, on cooling by the stimulated Raman adiabatic passage pumping, the temperature of a crystal with an irradiated volume of 2.12×10−4 cm3 can reach 64 K in a time of 2 s. In the proposed model, the cooling temperature is 30 K lower and the cooling process is 100 times faster compared to the traditional model of direct pumping. The estimates are applicable to present-day materials of technologically attainable purity.
We study the photon-echo attenuation by various dynamical processes in rare-earth-ion-doped crystals. The experimental investigations concentrate on a Pr3+:Eu3+:Nd3+ codoped Y2SiO5 crystal at low temperatures. Two-pulse photon-echo intensities are measured as a function of the pulse intensities when either the Pr3+ or the Eu3+ ions are excited. For the quantitative interpretation we consider primarily excitation-induced frequency shifts (EFS) by diagonal and off-diagonal interactions and show that for the systems under consideration EFS are dominated by diagonal interactions. The observed echo attenuation by EFS is compared with the predictions calculated from independent Stark-field measurements and reasonable agreement is obtained. The broadening by spin-ion interactions, by nonequilibrium phonons and the dependence of the echo attenuation on the frequency position in the inhomogeneously broadened band are further investigated.