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Physical Review Letters

Candidate for Laser Cooling of a Negative Ion: Observations of Bound-Bound Transitions in La−

C. W. Walter, N. D. Gibson, Daniel Matyas, Clayton Crocker, Kristina Dungan, Brad Matola, Johan Rohlén

Published Aug 5, 2014• 61 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.113.063001

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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.
The bound-bound transition from the 5d²6s² ³F_2 ground state to the 5d6s²6p ³D_1 excited state in negative lanthanum has been proposed as a candidate for laser cooling, which has not yet been achieved for negative ions. Anion laser cooling holds the potential to allow the production of ultracold ensembles of any negatively charged species. In this work the aforementioned transition was studied in a beam of negative La ions by high-resolution laser spectroscopy. The center-of-gravity frequency of the transition was measured to be 96.592 80(10) THz. Seven of the nine expected hyperfine structure resonances were resolved. The observed peaks were unambiguously assigned to the predicted hyperfine transitions by a fit. From the determined hyperfine structure for this transition it was concluded that only three lasers would be required to cool and re-pump all hyperfine levels. Furthermore, the observed relative transition amplitudes suggest that in resonance the transitions are saturated at a laser power of 45 W/m². A rough estimate of the transition cross section confirms that La‾ is a promising candidate for the first laser cooling of negative ions.
The bound-bound transition from the 5d^{2}6s^{2} ^{3}F_{2}^{e} ground state to the 5d6s^{2}6p ^{3}D_{1}^{o} excited state in negative lanthanum has been proposed as a candidate for laser cooling, which has not yet been achieved for negative ions. Anion laser cooling holds the potential to allow the production of ultracold ensembles of any negatively charged species. We have studied the aforementioned transition in a beam of negative La ions by high-resolution laser spectroscopy. The center-of-gravity frequency was measured to be 96.592 80(10) THz. Seven of the nine expected hyperfine structure transitions were resolved. The observed peaks were unambiguously assigned to the predicted hyperfine transitions by a fit, confirmed by multiconfigurational self-consistent field calculations. From the determined hyperfine structure we conclude that La^{-} is a promising laser cooling candidate. Using this transition, only three laser beams would be required to repump all hyperfine levels of the ground state.
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.
The bound-bound transition from the 5d26s2 3Fe2 ground state to the 5d6s26p 3D° 2 excited state in negative lanthanum has been proposed as a candidate for laser cooling, which has not yet been achieved for negative ions. Anion laser cooling holds the potential to allow the production of ultracold ensembles of any negatively charged species. In this work the aforementioned transition was studied in a beam of negative La ions by high-resolution laser spectroscopy. The center-of-gravity frequency of the transition was measured to be 96.592 80(10) THz. Seven of the nine expected hyperfine structure resonances were resolved. The observed peaks were unambiguously assigned to the predicted hyperfine transitions by a fit. From the determined hyperfine structure for this transition it was concluded that only three lasers would be required to cool and re-pump all hyperfine levels. Furthermore, the observed relative transition amplitudes suggest that in resonance the transitions are saturated at a laser power of 45 Wm-2. A rough estimate of the transition cross section confirms that La- is a promising candidate for the first laser cooling of negative ions.
Laser cooling is a well-established technique for the creation of ensembles of ultracold neutral atoms or positive ions. This ability has opened many exciting new research fields over the past 40 years. However, no negatively charged ions have been directly laser cooled because a cycling transition is very rare in atomic anions. Efforts of more than a decade currently have La^{-} as the most promising candidate. We report on experimental and theoretical studies supporting Th^{-} as a new promising candidate for laser cooling. The measured and calculated electron affinities of Th are, respectively, 4901.35(48) cm^{-1} and 4832 cm^{-1}, or 0.607 690(60) and 0.599 eV, almost a factor of 2 larger than the previous theoretical value of 0.368 eV. The ground state of Th^{-} is determined to be 6d^{3}7s^{2} ^{4}F_{3/2}^{e} rather than 6d^{2}7s^{2}7p ^{4}G_{5/2}^{o}. The consequence of this is that there are several strong electric dipole transitions between the bound levels arising from configurations 6d^{3}7s^{2} and 6d^{2}7s^{2}7p in Th^{-}. The potential laser-cooling transition is ^{2}S_{1/2}^{o}↔^{4}F_{3/2}^{e} with a wavelength of 2.6 μm. The zero nuclear spin and hence lack of hyperfine structure in Th^{-} reduces the potential complications in laser cooling as encountered in La^{-}, making Th^{-} a new and exciting candidate for laser cooling.
The negative ion of lanthanum has one of the richest bound-state spectra observed for an atomic negative ion and it has been proposed as a promising candidate for laser cooling, which has not yet been achieved for any negatively charged system. In the present study, radiative decays of low-lying excited states of ${\mathrm{La}}^{\ensuremath{-}}$ were experimentally investigated at the DESIREE cryogenic electrostatic ion-beam storage ring facility using state-selective photodetachment over storage times of up to 800 s. Independently, the transition rates for the relevant states were calculated using a high-precision hybrid theoretical approach. The measured lifetime of the lowest excited state of ${\mathrm{La}}^{\ensuremath{-}}$ (3F3e)({}^{3}{F}_{3}^{e})(3F3e​) of 132(20) s agrees very well with the theoretical calculations and previous predictions. However, a puzzling discrepancy exists for the next-higher state 3F4e{}^{3}{F}_{4}^{e}3F4e​, with the experiments yielding a lifetime $\ensuremath{\sim}4$ times shorter than calculated, highlighting the challenges for this complex ion. The results provide valuable insights into the prospects for laser cooling ${\mathrm{La}}^{\ensuremath{-}}$.