arXiv:2409.09873 · Physical Review A

Spectroscopy of electric dipole and quadrupole transitions in Ra + 224

Spencer Kofford, Haoran Li, Robert Kwapisz, Roy Ready, Akshay Sawhney, Oi Chee Cheung, Mingyu Fan, Andrew M. Jayich

Published Mar 4, 2025• 2 citations

Abstract

We report on spectroscopy of the low-lying electronic transitions in $^{224}\mathrm{Ra}^{+}$. We measured the frequencies of the $^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}P_{1/2}$ cooling transition, the $^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}D_{5/2}$ clock transition, the $^{2}D_{3/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}$ electric dipole transition, and the $^{2}D_{5/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}$ cleanout transition. From these measurements we calculate the frequencies of the $^{2}D_{3/2}\ensuremath{\leftrightarrow}^{2}P_{1/2}$ repump transition, the $^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}D_{3/2}$ electric quadrupole transition, and the $^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}$ electric dipole transition. The ion's low charge-to-mass ratio and convenient wavelengths make ${}^{224}{\mathrm{Ra}}^{+}$ a promising optical clock candidate.

DOI: 10.1103/physreva.111.032802

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arXiv:2409.09873 · Physical Review A

Spectroscopy of electric dipole and quadrupole transitions in Ra + 224

Spencer Kofford, Haoran Li, Robert Kwapisz, Roy Ready, Akshay Sawhney, Oi Chee Cheung, Mingyu Fan, Andrew M. Jayich

Published Mar 4, 2025• 2 citations

arXiv HTML PDF

Abstract

We report on spectroscopy of the low-lying electronic transitions in

^{224}\mathrm{Ra}^{+}

. We measured the frequencies of the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}P_{1/2}

cooling transition, the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}D_{5/2}

clock transition, the

^{2}D_{3/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}

electric dipole transition, and the

^{2}D_{5/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}

cleanout transition. From these measurements we calculate the frequencies of the

^{2}D_{3/2}\ensuremath{\leftrightarrow}^{2}P_{1/2}

repump transition, the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}D_{3/2}

electric quadrupole transition, and the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}

electric dipole transition. The ion's low charge-to-mass ratio and convenient wavelengths make

{}^{224}{\mathrm{Ra}}^{+}

a promising optical clock candidate.

DOI: 10.1103/physreva.111.032802

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Measurements of electric quadrupole transition frequencies in Ra+226

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

We report the first driving of the $7s{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}\ensuremath{\rightarrow}6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{3/2}$ and $7s{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}\ensuremath{\rightarrow}6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{5/2}$ electric quadrupole (E2) transitions in ${\mathrm{Ra}}^{+}$ . We measure the frequencies of both E2 transitions and two other low-lying transitions in $^{226}\mathrm{Ra}^{+}$ that are important for controlling the radium ion's motional and internal states: $6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{3/2}\ensuremath{\rightarrow}7p{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}^{o}$ and $6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{5/2}\ensuremath{\rightarrow}7p{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}^{o}$.We report the first driving of the $7s{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}\ensuremath{\rightarrow}6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{3/2}$ and $7s{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}\ensuremath{\rightarrow}6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{5/2}$ electric quadrupole (E2) transitions in ${\mathrm{Ra}}^{+}$. We measure the frequencies of both E2 transitions and two other low-lying transitions in $^{226}\mathrm{Ra}^{+}$ that are important for controlling the radium ion's motional and internal states: $6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{3/2}\ensuremath{\rightarrow}7p{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}^{o}$ and $6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{5/2}\ensuremath{\rightarrow}7p{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}^{o}$.

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C. A. Holliman, Mingyu Fan, A. Contractor +2 more

We report the first operation of a ${\mathrm{Ra}}^{+}$ optical clock, a promising high-performance clock candidate. The clock uses a single trapped $^{226}{\mathrm{Ra}}^{+}$ 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 ${D}_{5/2}$ state to the ${S}_{1/2}$ state Land\'e $g$ -factors: ${g}_{D}/{g}_{S}=0.598\text{ }805\text{ }3(11)$ . A ${\mathrm{Ra}}^{+}$ 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 report the first operation of a ${\mathrm{Ra}}^{+}$ optical clock, a promising high-performance clock candidate. The clock uses a single trapped $^{226}{\mathrm{Ra}}^{+}$ 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 ${D}_{5/2}$ state to the ${S}_{1/2}$ state Land\'e $g$-factors: ${g}_{D}/{g}_{S}=0.598\text{ }805\text{ }3(11)$. A ${\mathrm{Ra}}^{+}$ 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.

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High-Resolution Spectroscopy of $^{173}$ Yb $^{+}$ IonsHigh-Resolution Spectroscopy of $^{173}$Yb$^{+}$ Ions

J. Jiang, A. V. Viatkina, Saaswath JK +7 more

Compared to other stable isotopes of $\rm{Yb}^+$ , $^{173}\rm{Yb}^+$ has a richer hyperfine structure, which leads to more favorable clock transitions, spectroscopic techniques for probing new physics, and more sophisticated quantum computing architectures. However, to date, its electronic spectrum remains poorly characterized. Here, we report on efficient laser cooling, state preparation, and detection of a single trapped $^{173}\rm{Yb}^+$ ion. The previously unobserved $^2\!S_{1/2} \rightarrow {}^2\!D_{3/2}$ electric quadrupole transition at 436 nm is coherently excited, and the isotope shift between $^{171}\rm{Yb}^+$ and $^{173}\rm{Yb}^+$ on this transition is determined with an uncertainty of 1.4 Hz. Using microwave spectroscopy, we resolve the hyperfine structure (HFS) of the ${}^2\!D_{3/2}$ state with a relative uncertainty below $10^{-8}$ . From the HFS measurement data, we infer for ${}^{173}$ Yb a nuclear magnetic octupole moment $Ω= -0.062(8)\,({\rm b} \times μ_N)$ with uncertainty reduced by more than 2 orders of magnitude compared to previous studies. The data also allow us to determine hyperfine anomalies for the ${}^2\!S_{1/2}$ and ${}^2\!D_{3/2}$ states.Compared to other stable isotopes of $\rm{Yb}^+$, $^{173}\rm{Yb}^+$ has a richer hyperfine structure, which leads to more favorable clock transitions, spectroscopic techniques for probing new physics, and more sophisticated quantum computing architectures. However, to date, its electronic spectrum remains poorly characterized. Here, we report on efficient laser cooling, state preparation, and detection of a single trapped $^{173}\rm{Yb}^+$ ion. The previously unobserved $^2\!S_{1/2} \rightarrow {}^2\!D_{3/2}$ electric quadrupole transition at 436 nm is coherently excited, and the isotope shift between $^{171}\rm{Yb}^+$ and $^{173}\rm{Yb}^+$ on this transition is determined with an uncertainty of 1.4 Hz. Using microwave spectroscopy, we resolve the hyperfine structure (HFS) of the ${}^2\!D_{3/2}$ state with a relative uncertainty below $10^{-8}$. From the HFS measurement data, we infer for ${}^{173}$Yb a nuclear magnetic octupole moment $Ω= -0.062(8)\,({\rm b} \times μ_N)$ with uncertainty reduced by more than 2 orders of magnitude compared to previous studies. The data also allow us to determine hyperfine anomalies for the ${}^2\!S_{1/2}$ and ${}^2\!D_{3/2}$ states.

physics.atom-phCross-listedarXiv:2601.09585Physical Review LettersJan 15, 20261 citation

We report on spectroscopy of the low-lying electronic transitions in

^{224}\mathrm{Ra}^{+}

. We measured the frequencies of the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}P_{1/2}

cooling transition, the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}D_{5/2}

clock transition, the

^{2}D_{3/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}

electric dipole transition, and the

^{2}D_{5/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}

cleanout transition. From these measurements we calculate the frequencies of the

^{2}D_{3/2}\ensuremath{\leftrightarrow}^{2}P_{1/2}

repump transition, the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}D_{3/2}

electric quadrupole transition, and the

^{2}S_{1/2}\ensuremath{\leftrightarrow}^{2}P_{3/2}

electric dipole transition. The ion's low charge-to-mass ratio and convenient wavelengths make

{}^{224}{\mathrm{Ra}}^{+}

a promising optical clock candidate.

{\mathrm{Ra}}^{+}

. We measure the frequencies of both E2 transitions and two other low-lying transitions in

^{226}\mathrm{Ra}^{+}

that are important for controlling the radium ion's motional and internal states: $6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{3/2}\ensuremath{\rightarrow}7p{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}^{o}$ and $6d{\phantom{\rule{0.16em}{0ex}}}^{2}{D}_{5/2}\ensuremath{\rightarrow}7p{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}^{o}$.

We explore the potential of the electric quadrupole transitions

7s\,^2S_{1/2}

6d\,^2D_{3/2}

6d\,^2D_{5/2}

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

^+

candidates with

A=

223 - 229 are identified. In particular, we show that the transition

7s\,^2S_{1/2}\,(F=2,m_F=0)

6d\,^2D_{3/2}\,(F=0,m_F=0)

at 828 nm in

^{223}

^+

, 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^{-17}

. With more experimental effort, the

^{223,225,226}

^+

clocks could be pushed to a projected performance reaching the

10^{-18}

level.

We explore the potential of the electric quadrupole transitions

7s {}^{2}{S}_{1/2}

6d {}^{2}{D}_{3/2}

6d {}^{2}{D}_{5/2}

{}^{A}

{}^{+}

candidates, with

A=

223--229, are identified. In particular, we show that the transition

7s {}^{2}{S}_{1/2} (F=2,{m}_{F}=0)

6d {}^{2}{D}_{3/2} (F=0,{m}_{F}=0)

at 828 nm in

^{223}\mathrm{Ra}

{}^{+}

^{223,225,226}\mathrm{Ra}

{}^{+}

clocks could be pushed to a projected performance reaching the ${10}^{\ensuremath{-}18}$ level.

{\mathrm{Ra}}^{+}

for optical frequency standard studies. Our calculations of the lifetimes of the metastable

6d

states using the relativistic coupled-cluster theory suggest that they are sufficiently long for

{\mathrm{Ra}}^{+}

to be considered as a potential candidate for an atomic clock. This is further corroborated by our studies of the hyperfine interactions, dipole and quadrupole polarizabilities, and quadrupole moments of the appropriate states of this system.

We report the first operation of a

{\mathrm{Ra}}^{+}

optical clock, a promising high-performance clock candidate. The clock uses a single trapped

^{226}{\mathrm{Ra}}^{+}

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

{D}_{5/2}

state to the

{S}_{1/2}

state Land\'e

g

-factors:

{g}_{D}/{g}_{S}=0.598\text{ }805\text{ }3(11)

. A

{\mathrm{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.

High-Resolution Spectroscopy of

^{173}

^{+}

Ions

Compared to other stable isotopes of

\rm{Yb}^+

^{173}\rm{Yb}^+

has a richer hyperfine structure, which leads to more favorable clock transitions, spectroscopic techniques for probing new physics, and more sophisticated quantum computing architectures. However, to date, its electronic spectrum remains poorly characterized. Here, we report on efficient laser cooling, state preparation, and detection of a single trapped

^{173}\rm{Yb}^+

ion. The previously unobserved

^2\!S_{1/2} \rightarrow {}^2\!D_{3/2}

electric quadrupole transition at 436 nm is coherently excited, and the isotope shift between

^{171}\rm{Yb}^+

and

^{173}\rm{Yb}^+

on this transition is determined with an uncertainty of 1.4 Hz. Using microwave spectroscopy, we resolve the hyperfine structure (HFS) of the

{}^2\!D_{3/2}

state with a relative uncertainty below

10^{-8}

. From the HFS measurement data, we infer for

{}^{173}

Yb a nuclear magnetic octupole moment

Ω= -0.062(8)\,({\rm b} \times μ_N)

with uncertainty reduced by more than 2 orders of magnitude compared to previous studies. The data also allow us to determine hyperfine anomalies for the

{}^2\!S_{1/2}

and

{}^2\!D_{3/2}

states.