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arXiv:2211.05313 · Optical and Quantum Sensing and Precision Metrology II

Ion optical clocks with three electronic states

C. A. Holliman, Mingyu Fan, Andrew M. Jayich

Published Mar 8, 2023• 0 citations
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Abstract

Optical clocks are the apotheosis of precision measurement, but they require frequent maintenance by scientists. The supporting laser systems are a particularly demanding component of these instruments. To reduce complexity and increase robustness we propose an optical clock with trapped alkali-like ions that use the S1/2 → D3/2 electric quadrupole transition. Compared to traditional group-II ion clocks this reduces the number of laser wavelengths required, and uses hyperfine state preparation and readout techniques enabled by the nuclear spin I = 1/2. We consider 225Ra+ as a candidate system for a clock with three electronic states, and discuss the potential to help realize a transportable optical clock.

DOI
10.1117/12.2657190

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Optical clocks are the apotheosis of precision measurement, but they require frequent maintenance by scientists. The supporting laser systems are a particularly demanding component of these instruments. To reduce complexity and increase robustness we propose an optical clock with trapped alkali-like ions that use the S1/2 → D3/2 electric quadrupole transition. Compared to traditional group-II ion clocks this reduces the number of laser wavelengths required, and uses hyperfine state preparation and readout techniques enabled by the nuclear spin I = 1/2. We consider 225Ra+ as a candidate system for a clock with three electronic states, and discuss the potential to help realize a transportable optical clock.
We report the first operation of a Ra+{\mathrm{Ra}}^{+}Ra+ optical clock, a promising high-performance clock candidate. The clock uses a single trapped 226Ra+^{226}{\mathrm{Ra}}^{+}226Ra+ ion and operates on the $7s\text{ }^{2}{S}_{1/2}\ensuremath{\rightarrow}6d\text{ }^{2}{D}_{5/2}$ electric quadrupole transition. By self-referencing three pairs of symmetric Zeeman transitions, we demonstrate a frequency instability of $1.1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}13}/\sqrt{\ensuremath{\tau}}$, where $\ensuremath{\tau}$ is the averaging time in seconds. The total systematic uncertainty is evaluated to be $\mathrm{\ensuremath{\Delta}}\ensuremath{\nu}/\ensuremath{\nu}=9\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}$. Using the clock, we realize the first measurement of the ratio of the D5/2{D}_{5/2}D5/2​ state to the S1/2{S}_{1/2}S1/2​ state Land\'e ggg-factors: gD/gS=0.598 805 3(11){g}_{D}/{g}_{S}=0.598\text{ }805\text{ }3(11)gD​/gS​=0.598 805 3(11). A Ra+{\mathrm{Ra}}^{+}Ra+ optical clock could improve limits on the time variation of the fine structure constant, $\stackrel{\ifmmode \dot{}\else \textperiodcentered \fi{}}{\ensuremath{\alpha}}/\ensuremath{\alpha}$, in an optical frequency comparison. The ion also has several features that make it a suitable system for a transportable optical clock.
We explore the potential of the electric quadrupole transitions 7s 2S1/27s\,^2S_{1/2}7s2S1/2​ - 6d 2D3/26d\,^2D_{3/2}6d2D3/2​, 6d 2D5/26d\,^2D_{5/2}6d2D5/2​ in radium isotopes as single-ion optical frequency standards. The frequency shifts of the clock transitions due to external fields and the corresponding uncertainties are calculated. Several competitive A^AARa+^++ candidates with A=A=A= 223 - 229 are identified. In particular, we show that the transition 7s 2S1/2 (F=2,mF=0)7s\,^2S_{1/2}\,(F=2,m_F=0)7s2S1/2​(F=2,mF​=0) - 6d 2D3/2 (F=0,mF=0)6d\,^2D_{3/2}\,(F=0,m_F=0)6d2D3/2​(F=0,mF​=0) at 828 nm in 223^{223}223Ra+^++, with no linear Zeeman and electric quadrupole shifts, stands out as a relatively simple case, which could be exploited as a compact, robust, and low-cost atomic clock operating at a fractional frequency uncertainty of 10−1710^{-17}10−17. With more experimental effort, the 223,225,226^{223,225,226}223,225,226Ra+^++ clocks could be pushed to a projected performance reaching the 10−1810^{-18}10−18 level.
The 435 mum171Yb+transition is a good candidate for an atomic clock based on an optical transition. We have stored single171Yb ions for several months in RF traps. The ions are cooled, repumped and the clock transition is interrogated by (frequency-doubled) diode lasers. The interrogation laser linewidth was 30 Hz determining the resolvable linewidth of the Yb+transition interrogated. The absolute frequency of this transition was measured using an optical comb generator, self referenced by broadening the spectrum to above one octave, with respect to a Cs fountain clock. Of all systematic frequency shifts to which this transition is subject an estimate indicates that the electric quadruple shift appears is the largest. To obtain a magnitude of the quadruple shift (and the quadruple moment) the clock frequencies of two independently stored and cooled171Yb ions were compared while varying the static electric field in one trap. The measured frequency shift amounting to ~1 Hz/V. This result would seem to permit clocks with much higher accuracy than the clocks based on microwave transition, particularly if the technique of aligning the ions with respect to the electric field were applicable. Anticipating even more precise clocks, we are presently investigating a blue nuclear transition in229Th. Such a nuclear transition should be even better shielded from environmental influences than transitions in the electron shell. This nuclear transition has not yet been directly optically observed. We are presently investigating the luminescence after incoherent broad band optical excitation. The triply ionized223Th is then a suitable system for trapped single ion spectroscopy. The cooling transition lies conveniently in the near infrared and the nuclear clock transition can be read out by nuclear/electron shell double resonance
For the past 15 years, tremendous progress within the fields of laser stabilization, optical frequency combs and atom cooling and trapping have allowed the realization of optical atomic clocks with unrivaled performances. These instruments can perform frequency comparisons with fractional uncertainties well below 10-17, finding applications in fundamental physics tests, relativistic geodesy and time and frequency metrology. Even though most optical clocks are currently laboratory setups, several proposals for using these clocks for field measurements or within an optical clock network have been published, and most of time and frequency metrology institutes have started to develop transportable optical clocks. For the purpose of this special issue, we chose to focus on trapped-ion optical clocks. Even though their short-term fractional frequency stability is impaired by a lower signal-to-noise ratio, they offer a high potential for compactness: trapped ions demand low optical powers and simple loading schemes, and can be trapped in small vacuum chambers. We review recent advances on the clock key components, including ion trap and ultra-stable optical cavity, as well as existing projects and experiments which draw the picture of what future transportable, single-ion optical clocks may resemble.
A multi-ion optical clock with 5×10−19\mathbf{5 \times 10^{-19}}5×10−19 uncertainty
Today's most accurate clocks are based on laser spectroscopy of electronic transitions in single trapped ions and feature fractional frequency uncertainties below 1×10−181\times10^{-18}1×10−18. Scaling these systems to multiple, simultaneously interrogated ions reduces measurement times, driving recent advances in multi-ion clocks. However, maintaining state-of-the-art systematic uncertainties while increasing the number of ions remains a central challenge. Here, we report on a multi-ion optical atomic clock with a fractional frequency uncertainty of 5.3×10−195.3\times10^{-19}5.3×10−19 and up to 10 \Sr ions. Ion-resolved state detection enables minimization of position-dependent shifts, with residual effects suppressed below the 10−2010^{-20}10−20-level. Clock operation with eight to ten ions reduces the measurement time by a factor of 4.8 compared to single-ion operation. A comparison with an established \Yb single-ion clock yields an unperturbed frequency ratio of 0.6926711632159660405(20)0.6926711632159660405(20)0.6926711632159660405(20), with a statistical uncertainty of 0.9×10−180.9\times10^{-18}0.9×10−18 and a combined uncertainty of 2.9×10−182.9\times 10^{-18}2.9×10−18. These results demonstrate robust multi-ion clock operation with reduced averaging time and state-of-the-art accuracy.
We explore the potential of the electric quadrupole transitions 7s2S1/27s {}^{2}{S}_{1/2}7s2S1/2​-6d2D3/26d {}^{2}{D}_{3/2}6d2D3/2​, 6d2D5/26d {}^{2}{D}_{5/2}6d2D5/2​ in radium isotopes as single-ion optical frequency standards. The frequency shifts of the clock transitions due to external fields and the corresponding uncertainties are calculated. Several competitive A{}^{A}ARa+{}^{+}+ candidates, with A=A=A= 223--229, are identified. In particular, we show that the transition 7s2S1/2(F=2,mF=0)7s {}^{2}{S}_{1/2} (F=2,{m}_{F}=0)7s2S1/2​(F=2,mF​=0)-6d2D3/2(F=0,mF=0)6d {}^{2}{D}_{3/2} (F=0,{m}_{F}=0)6d2D3/2​(F=0,mF​=0) at 828 nm in 223Ra^{223}\mathrm{Ra}223Ra+{}^{+}+, with no linear Zeeman and electric quadrupole shifts, stands out as a relatively simple case, which could be exploited as a compact, robust, and low-cost atomic clock operating at a fractional frequency uncertainty of ${10}^{\ensuremath{-}17}$. With more experimental effort, the 223,225,226Ra^{223,225,226}\mathrm{Ra}223,225,226Ra+{}^{+}+ clocks could be pushed to a projected performance reaching the ${10}^{\ensuremath{-}18}$ level.