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Register a new userFine and hyperfine interactions in $^{171}$YbOH and $^{173}$YbOH
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The odd isotopologues of ytterbium monohydroxide, $^{171,173}$YbOH, have been identified as promising molecules in which to measure parity (P) and time reversal (T) violating physics. Here we characterize the $tilde{A}^{2}Pi_{1/2}(0,0,0)-tilde{X}^2Sigma^+(0,0,0)$ band near 577 nm for these odd isotopologues. Both laser-induced fluorescence (LIF) excitation spectra of a supersonic molecular beam sample and absorption spectra of a cryogenic buffer-gas cooled sample were recorded. Additionally, a novel spectroscopic technique based on laser-enhanced chemical reactions is demonstrated and utilized in the absorption measurements. This technique is especially powerful for disentangling congested spectra. An effective Hamiltonian model is used to extract the fine and hyperfine parameters for the $tilde{A}^{2}Pi_{1/2}(0,0,0)$ and $tilde{X}^2Sigma^+(0,0,0)$ states. A comparison of the determined $tilde{X}^2Sigma^+(0,0,0)$ hyperfine parameters with recently predicted values (M. Denis, et al., J. Chem. Phys. $bf{152}$, 084303 (2020), K. Gaul and R. Berger, Phys. Rev. A $bf{101}$, 012508 (2020), J. Liu et al., J. Chem. Phys. $bf{154}$, 064110 (2021)) is made. The measured hyperfine parameters provide experimental confirmation of the computational methods used to compute the P,T-violating coupling constants $W_d$ and $W_M$, which correlate P,T-violating physics to P,T-violating energy shifts in the molecule. The dependence of the fine and hyperfine parameters of the $tilde{A}^{2}Pi_{1/2}(0,0,0)$ and $tilde{X}^2Sigma^+(0,0,0)$ states for all isotopologues of YbOH are discussed and a comparison to isoelectronic YbF is made.
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Polyatomic polar molecules are promising systems for future experiments that search for violation of time-reversal and parity symmetries due to their advantageous electronic and vibrational structure, which allows laser cooling, full polarisation of the molecule, and reduction of systematic effects [I. Kozyryev and N.R. Hutzler, Phys, Rev. Lett. {bf 119}, 133002 (2017)]. In this work we investigate the enhancement factor of the electric dipole moment of the electron ($E_text{eff}$) in the triatomic monohydroxide molecules BaOH and YbOH within the high-accuracy relativistic coupled cluster method. The recommended $E_text{eff}$ values of the two systems are 6.65 $pm$ 0.15 GV/cm and 23.4 $pm$ 1.0 GV/cm, respectively. We compare our results with similar calculations for the isoelectronic diatomic molecules BaF and YbF, which are currently used in experimental search for $P,T$-odd effects in molecules. The $E_text{eff}$ values prove to be very close, within about 1.5 $%$ difference in magnitude between the diatomic and the triatomic compounds. Thus, BaOH and YbOH have a similar enhancement of the electron electric dipole moment, while benefiting from experimental advantages, and can serve as excellent candidates for next-generation experiments.
Hyperfine structure (HFS) of atomic energy levels arises due to interactions of atomic electrons with a hierarchy of nuclear multipole moments, including magnetic dipole, electric quadrupole and higher rank moments. Recently, a determination of the magnetic octupole moment of the $^{173}mathrm{Yb}$ nucleus was reported from HFS measurements in neutral ${}^{173}mathrm{Yb}$ [PRA 87, 012512 (2013)], and is four orders of magnitude larger than the nuclear theory prediction. Considering this substantial discrepancy between the spectroscopically extracted value and nuclear theory, here we propose to use an alternative system to resolve this tension, a singly charged ion of the same $^{173}mathrm{Yb}$ isotope. Utilizing the substantial suite of tools developed around $mathrm{Yb}^+$ for quantum information applications, we propose to extract nuclear octupole and hexadecapole moments from measuring hyperfine splittings in the extremely long lived first excited state ($4f^{13}(^2!F^{o})6s^2$, $J=7/2$) of $^{173}mathrm{Yb}^+$. We present results of atomic structure calculations in support of the proposed measurements.
We report the first experimental determination of the hyperfine quenching rate of the $6s^2 ^1!S_0 (F=1/2) - 6s6p ^3!P_0 (F=1/2)$ transition in $^{171}$Yb with nuclear spin $I=1/2$. This rate determines the natural linewidth and the Rabi frequency of the clock transition of a Yb optical frequency standard. Our technique involves spectrally resolved fluorescence decay measurements of the lowest lying $^3!P_{0,1}$ levels of neutral Yb atoms embedded in a solid Ne matrix. The solid Ne provides a simple way to trap a large number of atoms as well as an efficient mechanism for populating $^3!P_0$. The decay rates in solid Ne are modified by medium effects including the index-of-refraction dependence. We find the $^3!P_0$ hyperfine quenching rate to be $(4.42pm0.35)times10^{-2} mathrm{s}^{-1}$ for free $^{171}$Yb, which agrees with recent ab initio calculations.
Nuclear spin levels play an important role in understanding magnetization dynamics and implementation and control of quantum bits in lanthanide-based single-molecule magnets. We investigate the hyperfine and nuclear quadrupole interactions for $^{161}$Dy and $^{163}$Dy nucleus in anionic DyPc$_2$ (Pc=phthalocyanine) single-molecule magnets, using multiconfigurational ab-initio methods (beyond density-functional theory) including spin-orbit interaction. The two isotopes of Dy are chosen because the others have zero nuclear spin. Both isotopes have the nuclear spin $I=5/2$, although the magnitude and sign of the nuclear magnetic moment differ from each other. The large energy gap between the electronic ground and first-excited Kramers doublets, allows us to map the microscopic hyperfine and quadrupole interaction Hamiltonian onto an effective Hamiltonian with an electronic pseudo-spin $S_{rm eff}=1/2$ that corresponds to the ground Kramers doublet. Our ab-initio calculations show that the coupling between the nuclear spin and electronic orbital angular momentum contributes the most to the hyperfine interaction and that both the hyperfine and nuclear quadrupole interactions for $^{161}$Dy and $^{163}$Dy nucleus are much smaller than those for $^{159}$Tb nucleus in TbPc$_2$ single-molecule magnets. The calculated separations of the electronic-nuclear levels are comparable to experimental data reported for $^{163}$DyPc$_2$. We demonstrate that hyperfine interaction for Dy Kramers ion leads to tunnel splitting (or quantum tunneling of magnetization) at zero field. This effect does not occur for TbPc$_2$ single-molecule magnets. The magnetic field values of the avoided level crossings for $^{161}$DyPc$_2$ and $^{163}$DyPc$_2$ are found to be noticeably different, which can be observed from experiment.
Precision calculations of the fine and hyperfine structure of muonic atoms are performed in a relativistic approach and results for muonic 205 Bi, 147 Sm, and 89 Zr are presented. The hyperfine structure due to magnetic dipole and electric quadrupole splitting is calculated in first order perturbation theory, using extended nuclear charge and current distributions. The leading correction from quantum electrodynamics, namely vacuum polarization in Uehling approximation, is included as a potential directly in the Dirac equation. Also, an effective screening potential due to the surrounding electrons is calculated, and the leading relativistic recoil correction is estimated.
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