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Physical Review A

Experimental and theoretical study of bound and quasibound states of Ce−

C. W. Walter, N. D. Gibson, Y. G. Li, Daniel Matyas, R.M. Alton, S.E. Lou, R. L. Field, D. Hanstorp, Lin Pan, Donald R. Beck

Published Sep 21, 2011• 51 citations
Publisher

Abstract

The negative ion of cerium is investigated experimentally with tunable infrared laser photodetachment spectroscopy and theoretically with relativistic configuration interaction in the continuum formalism. The relative cross section for neutral atom production is measured with a crossed ion-beam--laser-beam apparatus over the photon energy range of 0.54--0.75 eV. A rich resonance spectrum is revealed near the threshold with, at least, 12 peaks observed due to transitions from bound states of ${\mathrm{Ce}}^{\ensuremath{-}}$ to either bound or quasibound excited states of the negative ion. Theoretical calculations of the photodetachment cross sections enable identification of the transitions responsible for the measured peaks. Two of the peaks are due to electric dipole-allowed bound-bound transitions in ${\mathrm{Ce}}^{\ensuremath{-}}$, making cerium only the second atomic negative ion that has been demonstrated to support multiple bound states of opposite parity. In addition, combining the experimental data with the theoretical analysis determines the electron affinity of cerium to be 0.628(10) eV and the fine structure splitting of the ground state of ${\mathrm{Ce}}^{\ensuremath{-}}$ (${}^{4}\phantom{\rule{-0.16em}{0ex}}{H}_{7/2}--{}^{4}\phantom{\rule{-0.16em}{0ex}}{H}_{9/2}$) to be 0.097 75(4) eV.

DOI
10.1103/physreva.84.032514

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Physical Review Letters•Aug 5, 2014•61 citations
The negative ion of cerium is investigated experimentally with tunable infrared laser photodetachment spectroscopy and theoretically with relativistic configuration interaction in the continuum formalism. The relative cross section for neutral atom production is measured with a crossed ion-beam--laser-beam apparatus over the photon energy range of 0.54--0.75 eV. A rich resonance spectrum is revealed near the threshold with, at least, 12 peaks observed due to transitions from bound states of Ce\ensuremath−{\mathrm{Ce}}^{\ensuremath{-}}Ce\ensuremath− to either bound or quasibound excited states of the negative ion. Theoretical calculations of the photodetachment cross sections enable identification of the transitions responsible for the measured peaks. Two of the peaks are due to electric dipole-allowed bound-bound transitions in Ce\ensuremath−{\mathrm{Ce}}^{\ensuremath{-}}Ce\ensuremath−, making cerium only the second atomic negative ion that has been demonstrated to support multiple bound states of opposite parity. In addition, combining the experimental data with the theoretical analysis determines the electron affinity of cerium to be 0.628(10) eV and the fine structure splitting of the ground state of Ce\ensuremath−{\mathrm{Ce}}^{\ensuremath{-}}Ce\ensuremath− (4H7/2−−4H9/2{}^{4}\phantom{\rule{-0.16em}{0ex}}{H}_{7/2}--{}^{4}\phantom{\rule{-0.16em}{0ex}}{H}_{9/2}4H7/2​−−4H9/2​) to be 0.097 75(4) eV.
The negative ion of lanthanum, La–\mathrm{L}{\mathrm{a}}^{\text{--}}La–, has one of the richest bound state spectra observed for an atomic negative ion and has been proposed as a promising candidate for laser-cooling applications. In the present experiments, La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– was investigated using tunable infrared photodetachment spectroscopy. The relative signal for neutral atom production was measured with a crossed ion-beam--laser-beam apparatus over the photon energy range 585--920 meV (2120--1350 nm) to probe the continuum region above the La neutral atom ground state. Eleven prominent peaks were observed in the La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– photodetachment cross section due to resonant excitation of quasibound transient negative ion states in the continuum, which subsequently autodetach. In addition, thresholds were observed for photodetachment from several bound states of La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– to both ground and excited states of La. The present results provide information on the excited state structure and dynamics of La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– that depend crucially on multielectron correlation effects.
Negative ions are unique quantum systems where electron correlation plays a decisive role in determining their properties. The lack of optically allowed transitions prevents traditional optical spectroscopy and the electron affinity is, therefore, for most elements, the only atomic quantity that can be determined with high accuracy. In this work, we present a high-precision experimental determination of the electron affinity of cesium. A collinear laser-ion beam apparatus was used to investigate the partial photodetachment cross section for the cesium anion, leaving the neutral atom in the 6p 2P3/2 excited state. A resonance ionization scheme was used to obtain final-state selectivity, which enabled the investigation of a sharp onset of the cross section associated with a Wigner s -wave threshold behavior. The electron affinity was determined to be 0.4715983(38)eV . Published by the American Physical Society 2024
The first experimental studies of Os(-) reveal the presence of two very strong resonances. One state is a narrow shape resonance lying only 3.52(12) meV above the ground state detachment threshold, while the other is bound by 11.48(12) meV. Convincing evidence that these states have odd parity is presented, making Os(-) the only known atomic negative ion with bound states of opposite parity. Additionally, the binding energies for the Os(-) ground state ((4)F(e)(9/2)) and first excited state ((4)F(e)(7/2)) are measured to be 1.077 80(12) eV and 0.553(3) eV, respectively.
This study reinterprets an earlier experimental photoelectron kinetic energy spectrum of the negative ion of lanthanum [A. M. Covington, D. Calabrese, J. S. Thompson, and T. J. Kvale, J. Phys. B 31, L855 (1998)] by carrying out relativistic configuration interaction (RCI) photodetachment calculations. The results confirm the earlier RCI calculation for the electron affinity of lanthanum (0.545 eV) [S. M. O'Malley and D. R. Beck, Phys. Rev. A 79, 012511 (2009)] and revise it to a slightly larger value of 0.550 eV, thus modifying the experimental interpretation of $0.47\ifmmode\pm\else\textpm\fi{}0.02$ eV. The calculation also yields the binding energies of the other thirteen bound states of ${\mathrm{La}}^{\ensuremath{-}}$. Good agreement has been found when these energies are compared to the results of a recent experimental study on ${\mathrm{La}}^{\ensuremath{-}}$ [C. W. Walter, N. D. Gibson, D. J. Matyas, C. T. Crocker, K. A. Dungan, B. R. Matola, and J. Rohl\'en, Phys. Rev. Lett. 113, 063001 (2014)]. Finally, our analysis confirms the transition energy for the potential laser cooling transition of ${}^{3}{F}_{2}^{e}\ensuremath{\rightarrow}{}^{3}{D}_{1}^{o}$ in ${\mathrm{La}}^{\ensuremath{-}}$.
We have observed a threshold in the electron photodetachment cross section of ${^{88}S\mathrm{r}}^{\ensuremath{-}}$ ions at a photon energy $h\ensuremath{\nu}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1.820\mathrm{eV}$ and assign it to a ppp-wave transition from the 5s25p2P{5s}^{2}5p^{2}P5s25p2P ground state in ${\mathrm{Sr}}^{\ensuremath{-}}$ to the 5s5p3P5s5p^{3}P5s5p3P state in neutral Sr. The measurement was made with a new technique combining the tunable laser photodetachment threshold method with accelerator mass spectrometry. We determine for the first time the electron affinity of Sr to be $48\ifmmode\pm\else\textpm\fi{}6\mathrm{meV}$, much smaller than predicted in recent calculations. The 2P1/2^{2}P_{1/2}2P1/2​- 2P3/2^{2}P_{3/2}2P3/2​ fine splitting of the ${\mathrm{Sr}}^{\ensuremath{-}}$ ground state is estimated to be $26\ifmmode\pm\else\textpm\fi{}8\mathrm{meV}$.
Despite the tremendous advances in laser cooling of neutral atoms and positive ions, no negatively charged ion has been directly laser cooled. The negative ion of lanthanum, La(-), has been proposed as the best candidate for laser cooling of any atomic anion [ and , Phys. Rev. A 81, 032503 (2010)]. Tunable infrared laser photodetachment spectroscopy is used to measure the bound-state structure of La(-), revealing a spectrum of unprecedented richness with multiple bound-bound electric dipole transitions. The potential laser-cooling transition ((3)F(2)(e)→(3)D(1)(o)) is identified and its excitation energy is measured. The results confirm that La^{-} is a very promising negative ion for laser-cooling applications.