Unlike conventional three-level GSA/ESA upconversion system,a four-level GSA/ESA upconversion system containing a nonradiative process is presented.The dynamic process and luminescent properties of the upconversion are analyzed theoretically by rate equation model.The results show that the rise process of the upconversion is dominated by the nonradiative relaxation rate of the middle nonradiative level,while the decay process is mainly governed by the relaxation rate of the final excited state level.
Unlike conventional three-level GSA/ESA upconversion system,a four-level GSA/ESA upconversion system containing a nonradiative process is presented.The dynamic process and luminescent properties of the upconversion are analyzed theoretically by rate equation model.The results show that the rise process of the upconversion is dominated by the nonradiative relaxation rate of the middle nonradiative level,while the decay process is mainly governed by the relaxation rate of the final excited state level.
The possibilities to obtain efficient 3-?m lasing in erbium systems on the self-saturated transition 4/ 11/2?4/13/2 are analyzed. In the frame of the mathematical model based on analytical expressions for population inversion, photon flux density, and quantum efficiency, obtained in the stationary regime, and which explains the main characteristics of 3-?m generation, the influence of various interaction mechanisms such as cross-relaxations, transfer to impurities, excited-state absorption (ESA) and so on is analyzed. It is shown that, although ESA from the terminal laser level could improve the generation characteristics, the driving mechanism for 3-?m erbium lasers is the cooperative upconversion from the terminal laser level.
We report a theoretical investigation of effective four-photon absorption (4PA) process and propose a two-step 4PA model of three-photon- induced excited-state absorption (ESA). Based on three-level rate-equation theory, we find an analytical result for the effective 4PA coefficient that depends on the three-photon absorption (3PA) cross-section, excited-state photophysical properties, and laser pulse duration. We present the analytical theory of the z-dependent nonlinear transmission for straightforwardly yet unambiguously evaluating the 3PA and effective 4PA coefficients simultaneously.
A detailed analysis of the non-exponential behaviour of the kinetics of the initial laser level for three-micron generation 4I11/2, in ErAG (Erbium Aluminium Garnet) crystals (laser transition 4I11/2 →4I13/2), excited in the 4H11/2 level with short laser pulses of variable intensity, is performed. The observed non-exponentiality of the 4I11/2 decay and its dependence on the energy of the exciting pulse cannot be satisfactorily described with a rate equation modelling which includes only two-ion energy transfer processes among Er3+ ions as up-conversion from the terminal laser level (4I13/2), up-conversion from the initial one. and cross-relaxation from 4I9/2 and 4S3/2 (thermalised, at room temperature, with 2H11/2) Our analysis has shown that the inclusion of three-ion up-conversion processes from both initial and terminal three-micron laser levels leads to an excellent agreement between experimental and theoretical non-exponentiality of the 4I11/2 decay for various pumping intensities and allows the estimation of the three-ion up-conversion rates The best agreement with the experimental non-exponentialities was obtained ω111 = ω222 = 2 x 10-34 cm6s-1 and q2 = 0.9, where ω111 and ω222 represent the rates of three-ion upconversion from 4I13/2 and 4I11/2, respectively, and q2 is the ratio o two-ion up-conversio rates.
The ability to modify the character of fluorescent emission by a laser-controlled, optically nonlinear process has recently been shown theoretically feasible, and several possible applications have already been identified. In operation, a pulse of off-resonant probe laser beam, of sufficient intensity, is applied to a system exhibiting fluorescence, during the interval of excited-state decay following the initial excitation. The result is a rate of decay that can be controllably modified, the associated changes in fluorescence behavior affording new, chemically specific information. In this paper, a two-level emission model is employed in the further analysis of this all-optical process; the results should prove especially relevant to the analysis and imaging of physical systems employing fluorescent markers, these ranging from quantum dots to green fluorescence protein. Expressions are presented for the laser-controlled fluorescence anisotropy exhibited by samples in which the fluorophores are randomly oriented. It is also shown that, in systems with suitably configured electronic levels and symmetry properties, fluorescence emission can be produced from energy levels that would normally decay nonradiatively.
In this work we have developed a kinetics model of energy transfer from the host lattice to the localized core excited states of rare-earth isoelectronic structured traps (REI traps). The presence of low-lying empty core orbitals in rare-earth impurities introduces new excitation and recombination phenomena. To adequately describe the energy transfer to a REI trap, the buildup and decay kinetics of rare-earth luminescence, we consider six separate states of the REI impurity (unoccupied, electron occupied, electron occupied excited, exciton occupied, excited electron occupied, and excited exciton occupied). The energy-transfer processes occur through an Auger mechanism where the recombination energy of the bound electron with a free hole is transferred nonradiatively to the core states, or energy can be transferred from the bound exciton on a REI trap to the core states. If the initial and final states are not resonant (in both mechanisms), the energy mismatch must be accommodated by emission or absorption of phonons. Furthermore we discuss details of several quenching processes, which are incorporated into the kinetics equations. We derive two sets of differential equations for semi-insulating and n-type semiconductors governing the kinetics of rare-earth luminescence. Equations have been solved by a numerical method to derive the time dependence of the rise and decay kinetics as a function of excitation intensity. The numerically simulated luminescence rise and decay times show a good overall quantitative agreement with experimental data obtained for InP:Yb, over a wide range of generation rates.
We have visited the nonradiative electron transfer process between optically active ions in luminescent materials. In contrast to the earlier formulations using multipolar expansion of instantaneous coulomb interaction between electrons, we have utilized a quantum electrodynamics (QED) approach to study the process of energy transfer from an excited ion to another. Such energy transfers occur in both sensitized luminescence and cross relaxations in the excited state. We have here investigated the nonradiative energy transfer processes specifically mediated by electric dipole moment-magnetic dipole moment and magnetic electric dipole moment-magnetic dipole moment interactions using a Feynman diagrammatic method. We have shown how experimentally relevant transfer rates could be obtained using a QED formulation involving discrete energy levels and spectral line shape function for emission and absorption profiles of interactive ions. Additional features of the dependence of the energy transfer rates on the interionic distance arising from retarded interaction potential have been pointed out.