Seven new schemes have been theoretically studied using the density-matrix approach for the ns2(1S0)→nsnp(3P01 or 1P01)→nsms(1S0) and the ns2(1S0)→nsnp(3P01 or 1P01)→np2(1S0 or 1D2) double optical resonance photoionization pathways to establish the possibility of selective ionization of the rare strontium 90Sr isotope for continuous wave laser excitation. The double-resonance excitation is followed by photoionization using a 488 nm photon. Density-matrix equations for the double-resonance ionization have been numerically integrated by incorporating the effects of Doppler broadening, velocity-dependent interaction times, time varying Rabi frequencies, and laser bandwidths. All the optical selectivity calculations were carried out on a high-speed parallel processing machine. Theoretical computations on five previously studied photoionization pathways have also been performed and tabulated for the sake of completeness. The conditions for obtaining optimum optical selectivities have been evaluated. This study results in seven new photoionization pathways. The optical selectivities are a few orders higher compared to the previously studied photoionization schemes for five out of the seven schemes studied. The remaining two schemes are slightly better than the previously studied schemes.
Seven new schemes have been theoretically studied using the density-matrix approach for the ns2(1S0)→nsnp(3P01 or 1P01)→nsms(1S0) and the ns2(1S0)→nsnp(3P01 or 1P01)→np2(1S0 or 1D2) double optical resonance photoionization pathways to establish the possibility of selective ionization of the rare strontium 90Sr isotope for continuous wave laser excitation. The double-resonance excitation is followed by photoionization using a 488 nm photon. Density-matrix equations for the double-resonance ionization have been numerically integrated by incorporating the effects of Doppler broadening, velocity-dependent interaction times, time varying Rabi frequencies, and laser bandwidths. All the optical selectivity calculations were carried out on a high-speed parallel processing machine. Theoretical computations on five previously studied photoionization pathways have also been performed and tabulated for the sake of completeness. The conditions for obtaining optimum optical selectivities have been evaluated. This study results in seven new photoionization pathways. The optical selectivities are a few orders higher compared to the previously studied photoionization schemes for five out of the seven schemes studied. The remaining two schemes are slightly better than the previously studied schemes.
Optical selectivities have been calculated by use of the density matrix approach for ns2 1S0−nsnp 1P10− nsms (or np2) 1S0 double-resonance photoionization pathways to establish the possibility of selective ionization of rare calcium and strontium isotopes for continuous-wave laser excitation. Numerical integration of the density matrix equations for double-resonance ionization has been carried out by incorporation of the effects of Doppler broadening, velocity-dependent interaction times, time-varying Rabi frequencies, and laser bandwidths. The conditions for obtaining optimum selectivities have been evaluated. This study results in five new photoionization pathways (two for calcium and three for strontium) whose optical selectivities were found to be a few orders higher than the previously studied photoionization schemes. The effect of laser linewidth of the excitation lasers and Doppler width have also been investigated.
Optical selectivity calculations have been carried out for the 91Zr isotope for two-color resonant three-photon photoionization schemes. The density-matrix equations of motion were solved numerically for collinear, counterpropagating, linearly polarized laser beams having Gaussian temporal profile. Calculations were carried out incorporating the effects of Doppler broadening, magnetic sublevel degeneracy, and laser bandwidths. The selectivities and ion yields were determined for various Rabi frequencies and ionization rates. Thereby, the optimal Rabi frequencies for the first and second excitation steps and ionizaton rate for the ionizaton step were determined. The ionization efficiency as a function of detuning of the excitation lasers was also investigated. Two of the photoionization schemes investigated yielded a selectivity of ∼10, with an ion yield of ∼23%.
Lineshapes for double-resonance three-photon ionization have been evaluated using the density matrix formalism. Experimental conditions were incorporated by considering realistic distributions for atomic velocity and angular divergence, as well as spatial laser intensity profiles. Results for the 4s2 1S0→4s4p 1P1→4s4d 1D2→Ca+ ionization scheme of calcium are discussed and compared with experimental measurements. The calculations accurately reproduce isotopic selectivities achieved in the experiment. Moreover, these measurements have been carried out with dynamic range of >106, revealing many subtle effects of simultaneously present coherent and incoherent excitation processes.
Ytterbium enriched in 176Yb is used for the production of the 177Lu radioisotope, which has applications in cancer treatment. We have theoretically studied the two-step resonant, three-step photoionization of the 176Yb isotope using the density-matrix approach. To simulate experimentally realistic conditions, the Doppler averaging, magnetic sublevel degeneracy, time-varying Rabi frequencies, ionization rate, angular divergence, and laser bandwidth have all been incorporated into the theoretical model. Calculations have been carried out to identify the optimized Rabi frequencies for evaluating the separation factor. The effect of the laser line shape on the excitation profile has also been thoroughly studied. We could obtain large separation factors of ~5000 for the 176Yb isotope, and the excitation conditions identified in this work may be utilized in the separation of the desired isotope.
Numerical computations of ionization efficiency and isotope selectivity of 176 L u have been carried out for the following three-step ladder type photoionization scheme, 5 d 6 s 2 2 D 3 / 2 ( 0.0 c m − 1 ) − − − ⟶ 540.4068 n m 5 d 6 s 6 p 4 F 5 / 2 o ( 18504.58 c m − 1 ) − − − ⟶ 535.0626 n m 5 d 6 s 7 s 4 D 3 / 2 ( 37193.98 c m − 1 ) − − − ⟶ 618.0061 n m 53375 c m − 1 A u t o i o n i z a t i o n S t a t e → L u + , by invoking the density matrix formalism for the laser–atom interactions. Equations of motion have been derived for the odd isotopes by inclusion of hyperfine levels. The line shapes and their effect on the ionization efficiency and isotope selectivity have been discussed in detail. The effects of power of excitation and ionization lasers, spectral bandwidths, pulse delays, Doppler broadening of the atomic ensemble on the ionization efficiency, and degree of enrichment have been presented. Optimum conditions for the power of excitation, detunings, and other system parameters for the selective yet efficient photoionization of 176 L u have been identified.
Selective photoionization of ytterbium isotope is studied numerically based on a three-step photoionization scheme, 4f146s2 1S0 (0 cm−1) → 4f146s6p 3P1 (17992.008 cm−1) → (4f136s26p) (7/2, 3/2)2 (35196.98 cm−1) → auto-ionization state (52353 cm−1) → Yb+, by the density matrix theory with the consideration of atomic hyperfine structures and magnetic sublevels. To examine the physical model, the numerical isotopic abundance of ytterbium is compared with that from mass spectroscopy experiment, showing that they are in good agreement with each other. The excitation process and ionization process of ytterbium, especially for odd isotopes, are discussed and analyzed in detail on this basis. The effects of frequency detuning, power densities, spectral bandwidths, polarization of two excitation lasers, and atomic Doppler broadening on the total ionization yield and isotopic abundance are investigated numerically and the optimal excitation conditions for 176Yb enrichment are identified semi-quantitatively.