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Physical Review Letters

First Optical Hyperfine Structure Measurement in an Atomic Anion

Arne Fischer, C. Canali, Ulrich Warring, A. Kellerbauer, S. Fritzsche

Published Feb 18, 2010• 37 citations
Publisher

Abstract

We have investigated the hyperfine structure of the transition between the 5d{7}6s{2} {4}F{9/2}{e} ground state and the 5d{6}6s{2}6p {6}D{J}{o} excited state in the negative osmium ion by high-resolution collinear laser spectroscopy. This transition is unique because it is the only known electric-dipole transition in atomic anions and might be amenable to laser cooling. From the observed hyperfine structure in 187Os- and 189Os- the yet unknown total angular momentum of the bound excited state was found to be J=9/2. The hyperfine structure constants of the {4}F{9/2}{e} ground state and the {6}D{9/2}{o} excited state were determined experimentally and compared to multiconfiguration Dirac-Fock calculations. Using the knowledge of the ground and excited state angular momenta, the full energy level diagram of 192Os- in an external magnetic field was calculated, revealing possible laser cooling transitions.

DOI
10.1103/physrevlett.104.073004

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•Jan 1, 2015•1 citation
We have investigated the hyperfine structure of the transition between the 5d{7}6s{2} {4}F{9/2}{e} ground state and the 5d{6}6s{2}6p {6}D{J}{o} excited state in the negative osmium ion by high-resolution collinear laser spectroscopy. This transition is unique because it is the only known electric-dipole transition in atomic anions and might be amenable to laser cooling. From the observed hyperfine structure in 187Os- and 189Os- the yet unknown total angular momentum of the bound excited state was found to be J=9/2. The hyperfine structure constants of the {4}F{9/2}{e} ground state and the {6}D{9/2}{o} excited state were determined experimentally and compared to multiconfiguration Dirac-Fock calculations. Using the knowledge of the ground and excited state angular momenta, the full energy level diagram of 192Os- in an external magnetic field was calculated, revealing possible laser cooling transitions.
Laser cooling of neutral atoms or positive ions is today routinely employed in numerous experiments. Negative ions, in contrast, have distinct characteristics which hamper the application of lasers for cooling. But in 1999, the discovery of the unique bound–bound electric dipole transition in the negative osmium ion provided the motivation for a first cooling attempt. This thesis presents the first milestones toward the ultimate goal of laser cooling negative osmium, including high-resolution laser spectroscopy of the relevant bound–bound E1 transition. Its frequency – between the ground 4F9/2 and the 6DJe1 (bound) excited states – was determined to be 257.831190(35) THz in 192Os-, in agreement\nwith a previous measurement, but two orders of magnitude more precise. The determination of the resonant cross-section implicitly provided the corresponding Einstein A coefficient, which was found to be A ~ 330 s-1. Furthermore, the isotope shift of the E1 transition and the hyperfine structure constants of the ground and excited state were obtained, for the first time, from the analysis of the spectra of all naturally abundant isotopes. The hyperfine structure revealed the heretofore unknown total angular momentum of the excited state to be Je1 = 9/2. Finally, laser spectroscopy in an external magnetic field confirmed the expected line splitting for Os- due to the Zeeman effect. Based on all these experimental results the prospect of laser cooling negative osmium is reviewed.
Atomic anions are generally not amenable to optical spectroscopy because they are loosely bound systems and rarely have bound excited states. Until recently, there was only one known negative ion with a strong bound–bound electronic transition, the osmium anion Os − . The electric-dipole transition between the 4 F e 9/2 ground and 6 D o J excited state of this ion provides unique insight into the structure of atomic anions. In addition, it may enable the preparation of ultracold ensembles of negative ions. Laser excitation of the electric-dipole transition in Os − ions could be used to laser-cool them to microkelvin temperatures. If demonstrated to be successful, the technique would allow the cooling of any species of negatively charged ions - from subatomic particles to molecular anions - to ultracold temperatures by sympathetic cooling. We have been investigating the bound-bound electric-dipole transition in Os − by high-resolution laser spectroscopy with a view to using it for the first laser cooling of negative ions. The principle of the method, its potential applications, as well as experimental results are presented.
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 osmium ion ${\text{Os}}^{\ensuremath{-}}$ is one of very few atomic anions potentially suitable for laser cooling. We have made a measurement of the Zeeman splitting of a bound-bound transition in 192{}^{192}192${\text{Os}}^{\ensuremath{-}}$ by studying the laser excitation from the 5${d}^{7}666{s}^{2}$ 4{}^{4}4FFF9/2e{}_{9/2}^{e}9/2e​ ground to the 5${d}^{6}666{s}^{2}666p$ 6{}^{6}6DDD9/2o{}_{9/2}^{o}9/2o​ excited state in a homogeneous external magnetic field. The experimental Land\'e factors gJ=1.31(7){g}_{J}=1.31(7)gJ​=1.31(7) and gJ=1.50(8){g}_{J}=1.50(8)gJ​=1.50(8), respectively, agree well with calculated values. Both levels are found to split into 10 Zeeman sublevels, resulting in 28 allowed transitions of different relative intensities, in agreement with calculations based on pure and composite LSLSLS states. In view of the experimental results, the prospects for laser cooling of ${\text{Os}}^{\ensuremath{-}}$ are discussed.
The characteristics of atomic anions differ heavily from cations and neutral atoms, preventing the optical manipulation of their motion, with the remarkable exception of Os - . Since the negative osmium ion exhibits a bound–bound electric-dipole transition, we are currently exploring this unique feature with the aim of laser cooling. In the course of our experiments, we performed high-resolution laser spectroscopy on the relevant transition determining its frequency, cross-section and sub-level splitting in magnetic fields.
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.