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arXiv:2507.16760 · Physical Review X

Ultracold High-Spin Σ -State Polar Molecules for New Physics Searches

A. Ciamei, Adam M. Koza, Marcin Gronowski, Michał Tomza

Published Jan 27, 2026• 0 citations
arXivHTMLPDF

Abstract

We propose high-spin Σ -state polar molecules assembled from ultracold atoms to probe charge-parity-violating physics beyond the standard model. We identify YbCr as a prime candidate to search for the electric dipole moment of the electron. We show that the combination of relativistic ytterbium and high-spin chromium, amenable to magnetoassociation, leads to molecules with easy-to-polarize parity doublets and large intramolecular electric fields. Based on results for molecular constants, we predict a sensitivity of δ d e = ( 6 × 10 − 31 / n day ) e cm via standard spin-precession measurements, assess the experimental feasibility, and discuss potential extensions to more advanced quantum control as well as searches of the nuclear magnetic quadrupole moment. This work paves the way to next-generation searches for new physics with ultracold molecules in both the leptonic and hadronic sectors.

DOI
10.1103/wlq7-9p41

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•Mar 1, 2020•1 citation
We propose high-spin Σ -state polar molecules assembled from ultracold atoms to probe charge-parity-violating physics beyond the standard model. We identify YbCr as a prime candidate to search for the electric dipole moment of the electron. We show that the combination of relativistic ytterbium and high-spin chromium, amenable to magnetoassociation, leads to molecules with easy-to-polarize parity doublets and large intramolecular electric fields. Based on results for molecular constants, we predict a sensitivity of δ d e = ( 6 × 10 − 31 / n day ) e cm via standard spin-precession measurements, assess the experimental feasibility, and discuss potential extensions to more advanced quantum control as well as searches of the nuclear magnetic quadrupole moment. This work paves the way to next-generation searches for new physics with ultracold molecules in both the leptonic and hadronic sectors.
Abstract We explore the possibilities for a next-generation electron-electric-dipole-moment experiment using ultracold heteronuclear diatomic molecules assembled from a combination of radium and another laser-coolable atom. In particular, we calculate their ground state structure and their sensitivity to parity- and time-reversal ( P , T ) violating physics arising from flavor-diagonal charge-parity ( CP ) violation. Among these species, the largest P , T -violating molecular interaction constants—associated for example with the electron electric dipole moment—are obtained for the combination of radium (Ra) and silver (Ag) atoms. A mechanism for explaining this finding is proposed. We go on to discuss the prospects for an electron EDM search using ultracold, assembled, optically trapped RaAg molecules, and argue that this system is particularly promising for rapid future progress in the search for new sources of CP violation.
The properties of the electronic ground state of the polar and paramagnetic chromium--closed-shell-atom molecules have been investigated. State-of-the-art ab initio techniques have been applied to compute the potential energy curves for the chromium--alkaline-earth-metal-atom, CrXXX (X=BeX=\mathrm{Be}X=Be, Mg, Ca, Sr, Ba), and chromium--ytterbium, CrYb, molecules in the Born-Oppenheimer approximation for the high-spin ${X}^{7}{\ensuremath{\Sigma}}^{+}$ electronic ground state. The spin restricted open-shell coupled cluster method restricted to single, double, and noniterative triple excitations, RCCSD(T), was employed and the scalar relativistic effects within the Douglas-Kroll-Hess Hamiltonian or energy-consistent pseudopotentials were included. The permanent electric dipole moments and static electric dipole polarizabilities were computed. The leading long-range coefficients describing the dispersion interaction between the atoms at large interatomic distances C6{C}_{6}C6​ are also reported. The molecules under investigation are examples of species possessing both large magnetic and electric dipole moments making them potentially interesting candidates for ultracold many-body physics studies.
Heavy polar diatomic molecules are the leading candidates in searches for the permanent electric-dipole moment of the electron (eEDM). Next-generation eEDM search experiments ideally require extremely large coherence times, in large ensembles of trapped molecules that have a high sensitivity to the eEDM. We consider a family of molecules, mercury--alkali-metal diatomics, that can be feasibly produced from ultracold atoms. We present calculations of the effective electric fields experienced by the electron in these molecules. The combination of reasonably large effective electric fields, and the possibility of obtaining trapped ultracold samples, leads us to identify these molecules as favorable candidates for eEDM search experiments.
We investigate Feshbach resonances in collisions of high-spin atoms such as Er and Dy with closed-shell atoms such as Sr and Yb, using coupled-channel scattering and bound-state calculations.We consider both low-anisotropy and high-anisotropy limits.In both regimes, we find many resonances with a wide variety of widths.The wider resonances are suitable for tuning interatomic interactions, while some of the narrower resonances are highly suitable for magnetoassociation to form high-spin molecules.These molecules might be transferred to short-range states, where they would have large magnetic moments and electric dipole moments that can be induced with very low electric fields.The results offer the opportunity to study mixed quantum gases where one species is dipolar and the other is not and open up important prospects for a new field of ultracold high-spin polar molecules.
The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3
That the universe contains a disproportionate amount of matter compared to antimatter cannot be explained by the standard model of particle physics; this is because it contains too little charge-parity (CP) symmetry violation. Low energy experiments with atoms and molecules can be extremely sensitive probes for many types of new physics. An active area of research is the search for electric dipole moments (EDMs) of fundamental particles or nuclei; a nonzero EDM would be evidence for new sources of CP violation. Ytterbium monofluoride (YbF) molecules in a supersonic beam are currently being used to measure the electric dipole moment of the electron (eEDM). This thesis presents progress towards a new, more sensitive eEDM experiment that will use a slower YbF beam source and transverse laser cooling to collimate this beam. We have demonstrated laser cooling of YbF in one transverse dimension to less than 100 μK, which is below the Doppler cooling limit. This was done using a Sisyphus-type mechanism called magnetic field induced laser cooling. We also demonstrate polarisation gradient cooling of YbF. After rebuilding and upgrading much of the experiment, we cooled the beam in both transverse dimensions. By scanning experimental parameters, we have gained insight into the cooling mechanisms, and the optimum conditions for laser cooling. We placed an upper limit of a few mK on the transverse temperature of the molecules, although I argue that the true temperature must be very much lower. The number of ultracold molecules was carefully quantified and found to be 2.0(4)x10^5 per pulse. These experiments lay the foundations for an eEDM sensitivity improvement by up to a factor of 100.