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Optics and Spectroscopy

Study of a Selective Photoionization Scheme of 177Lu

Aleksei B D'yachkov, Aleksei A. Gorkunov, Anton V. Labozin, Sergei M. Mironov, Gleb O. Tsvetkov, Vladislav Ya. Panchenko, Valerii A Firsov

Published Dec 1, 2018• 21 citations
Publisher

Abstract

The hyperfine structure of transitions in the three-step scheme 5d6s22D3/2–5d6s6p4F $$_{{5/2}}^{^\circ }$$ –5d6s7s4D3/2– (53 375 cm–1) $$_{{1/2}}^{^\circ }$$ of lutetium ionization is studied for 175Lu, 176Lu, and 177Lu isotopes using the photoionization laser spectroscopy method. Values of the magnetic dipole (A) and electric quadrupole (B) interaction constants are determined, as well as the energies, the isotope shifts, and the radiative lifetimes for the 5d6s7s4D3/2 and (53 375 cm–1) $$_{{1/2}}^{^\circ }$$ levels.

DOI
10.1134/s0030400x19020127

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The hyperfine structure of transitions in the three-step scheme 5d6s22D3/2–5d6s6p4F 5/2∘_{{5/2}}^{^\circ }5/2∘​ –5d6s7s4D3/2– (53 375 cm–1) 1/2∘_{{1/2}}^{^\circ }1/2∘​ of lutetium ionization is studied for 175Lu, 176Lu, and 177Lu isotopes using the photoionization laser spectroscopy method. Values of the magnetic dipole (A) and electric quadrupole (B) interaction constants are determined, as well as the energies, the isotope shifts, and the radiative lifetimes for the 5d6s7s4D3/2 and (53 375 cm–1) 1/2∘_{{1/2}}^{^\circ }1/2∘​ levels.
The photoionization spectrum in the second step of the three-step lutetium photoionization scheme 5d6s2 2D3/2 – 5d6s6p4 F5/2oF_{{5/2}}^{{\text{o}}}F5/2o​ – 5d6s7s4D3/2 – (53 375 cm–1 )1/2o)_{{1/2}}^{{\text{o}}})1/2o​ has been measured. The effect of two-photon transitions has been studied experimentally compared to one-photon transitions.
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.
We have measured and analyzed the hyperfine structure of two lines, one at 583 nm and one at 401 nm, of the only stable fermionic isotope of atomic erbium as well as determined its isotope shift relative to the four most-abundant bosonic isotopes. Our work focuses on the $J\ensuremath{\rightarrow}J+1$ laser cooling transitions from the [Xe]4f126s2(3H6)[\text{Xe}]4{f}^{12}6{s}^{2}{(}^{3}{H}_{6})[Xe]4f126s2(3H6​) ground state to two levels of the excited [Xe]4f126s6p[\text{Xe}]4{f}^{12}6s6p[Xe]4f126s6p configuration, which are of major interest for experiments on quantum degenerate dipolar Fermi gases. From a fit to the observed spectra of the strong optical transition at 401 nm we find that the magnetic dipole and electric quadrupole hyperfine constants for the excited state are ${A}_{e}/h=\ensuremath{-}100.1(3)\phantom{\rule{0.28em}{0ex}}\mathrm{MHz}$ and ${B}_{e}/h=\ensuremath{-}3079(30)\phantom{\rule{0.28em}{0ex}}\mathrm{MHz}$, respectively. The hyperfine spectrum of the narrow transition at 583 nm, was previously observed and accurate Ae{A}_{e}Ae​ and Be{B}_{e}Be​ coefficients are available. A simulated spectrum based on these coefficients agrees well with our measurements. We have also determined the hyperfine constants using relativistic configuration-interaction ab initio calculations. The agreement between the ab initio and fitted data for the ground state is better than 0.1%, while for the two excited states the agreement is 1% and 11% for the Ae{A}_{e}Ae​ and Be{B}_{e}Be​ constants, respectively.
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.
The highly excited even levels of the lutetium atom are studied by two-step resonance ionisation spectroscopy. Four Rydberg series, 6s 2 ns 2 S 1/2 (n=17-76), 6s 2 nd 2 D 3/2 (n=14-105), 6s 2 nd 2 D 5/2 (n=19-87) and 6s 2 ng 2 G 9/2 (n=21-61), are measured and analysed. A very weak perturbation from an unassigned J= 3 / 2 even valence level is observed around 6s 2 52d 2 D 3/2 as a dip of ion signals induced by a decrease of radiative lifetimes in the perturbed Rydberg states. Small dips observed in nearby 6s 2 ns 2 S 1/2 and 6s 2 nd 2 D 5/2 Rydberg states are interpreted as the influence of the quadrupole hyperfine interaction of 175 Lu (I= 7 / 2 ).