We present a method that uses dynamic decoupling of a multilevel quantum probe to distinguish small frequency shifts that depend on m_{j}^{2}, where m_{j}^{2} is the angular momentum of level |j⟩ along the quantization axis, from large noisy shifts that are linear in m_{j}, such as those due to magnetic field noise. Using this method we measured the electric-quadrupole moment of the 4D_{5/2} level in ^{88}Sr^{+} to be 2.973_{-0.033}^{+0.026}ea_{0}^{2}. Our measurement improves the uncertainty of this value by an order of magnitude and thus helps mitigate an important systematic uncertainty in ^{88}Sr^{+} based optical atomic clocks and verifies complicated many-body quantum calculations.
We have calculated quadrupole moments,
Qzz, of helium in several of its doubly excited states and in two of its singly excited Rydberg states, and of the alkaline-earth atoms Be, Mg, Ca, Sr, and Ba in their ground and low-lying excited states. The calculations use well-converged, frozen-core configuration-interaction (CI) wave functions and, for interpretive purposes, Hartree-Fock (HF) atomic wave functions and single-term, optimized, molecular rotor-vibrator (RV) wave functions. The quadrupole moments calculated using RV wave functions serve as a test of the validity of the correlated, moleculelike model, which has been used to describe the effects of electron correlation in these two-electron and pseudo-two-electron atoms. Likewise, the quadrupole moments calculated with HF wave functions test the validity of the independent-particle model. In addition to their predictive use and their application to testing simple models, the quadrupole moments calculated with CI wave functions reveal previously unavailable information about the electronic structure of these atoms. Experimental methods by which these quadrupole moments might be measured are also discussed. The quadrupole moments computed from CI wave functions are presented as predictions; measurements of
Qzz have been made for only two singly excited Rydberg states of He, and a value of
Qzz has been computed previously for only one of the states reported here. We present these results in the hope of stimulating others to measure some of these quadrupole moments.
We propose and experimentally demonstrate a scheme that realizes hyperfine averaging during a Ramsey interrogation of a clock transition. The method eliminates the need to average over multiple optical transitions, reduces the sensitivity of the clock to its environment, and reduces inhomogeneous broadening in a multi-ion clock. The method is compatible with autobalanced Ramsey spectroscopy, which facilitates the elimination of residual shifts due to imperfect implementation and ac stark shifts from the optical probe. We demonstrate the scheme using correlation spectroscopy of the ^{1}S_{0}↔^{3}D_{1} clock transition in a three-ion Lu^{+} clock. From the demonstration we are able to provide a measurement of the ^{3}D_{1} quadrupole moment, Θ(^{3}D_{1})=0.634(9)ea_{0}^{2}.