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Journal of the Optical Society of America B

Investigations on the 1_S_0 λ_1→ 1_P^0_1 λ_2→ 1_S_0 nonresonant——→ M+ photoionization pathway for selective ionization of rare calcium and strontium isotopes

Manda Sankari, Pragada V. Kiran Kumar, Manda V. Suryanarayana

Published Jul 1, 2004• 5 citations
Publisher

Abstract

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.

DOI
10.1364/josab.21.001369

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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.
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 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.
Isotopic selectivity calculations are carried out for minor calcium isotopes against the major isotope 40 Ca for the single-resonance two-step and double-resonance three-step photoionization schemes with narrow-band lasers by using spectral simulation (SS) and modified spectrum (MS) approaches. The results of these calculations are compared with the density matrix (DM) results reported in the literature. It is noted that the values of isotopic selectivity from the SS approach do not agree with those from the DM approach whereas the MS approach, considering hole burning in the Doppler-broadened atomic spectrum, predicts selectivity values which are in good agreement with the DM results. It is argued that one can adequately use the simple MS approach rather than the complex DM approach for the calculation of isotopic selectivity of multi-step photoionization with single-frequency lasers.
Optical selectivities of calcium isotopes have been calculated for the 4s 2 1 S 0 4s4p 1 P 1 4s4d 1 D 2 →Ca + double-resonance ionization scheme using the spectral simulation (SS) approach. Optical selectivities obtained by the SS approach are in good agreement with the results obtained by the density matrix formalism. Studies on the effect of laser detuning and linewidth on optical selectivities indicate that lasers with 50 MHz linewidth for both the excitation steps can yield an optical selectivity of 2.2 × 10 5 , which is adequate for selective excitation of the 41 Ca isotope for certain applications.
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.