Quantum-Enhanced Metrology for Molecular Symmetry Violation Using Decoherence-Free Subspaces.

We propose a method to measure time-reversal symmetry violation in molecules that overcomes the standard quantum limit while leveraging decoherence-free subspaces to mitigate sensitivity to classical noise. The protocol does not require an external electric field, and the entangled states have no first-order sensitivity to static electromagnetic fields as they involve superpositions with zero average lab-frame projection of spins and dipoles. This protocol can be applied with trapped neutral or ionic species, and can be implemented using methods that have been demonstrated experimentally.

Engineering Field-Insensitive Molecular Clock Transitions for Symmetry Violation Searches.

Molecules are a powerful platform to probe fundamental symmetry violations beyond the standard model, as they offer both large amplification factors and robustness against systematic errors. As experimental sensitivities improve, it is important to develop new methods to suppress sensitivity to external electromagnetic fields, as limits on the ability to control these fields are a major experimental concern. Here we show that sensitivity to both external magnetic and electric fields can be simultaneously suppressed using engineered radio frequency, microwave, or two-photon transitions that maintain large amplification of CP-violating effects. By performing a clock measurement on these transitions, CP-violating observables including the electron electric dipole moment, nuclear Schiff moment, and magnetic quadrupole moment can be measured with suppression of external field sensitivity of ≳100 generically, and even more in many cases. Furthermore, the method is compatible with traditional Ramsey measurements, offers internal co-magnetometry, and is useful for systems with large angular momentum commonly present in molecular searches for nuclear CP violation.

Fine and hyperfine interactions in 171YbOH and 173YbOH.

The odd isotopologues of ytterbium monohydroxide, 171,173YbOH, have been identified as promising molecules to measure parity (P) and time reversal (T) violating physics. Here, we characterize the Ã2Π1/2(0,0,0)-X̃2Σ+(0,0,0) band near 577 nm for these odd isotopologues. Both laser-induced fluorescence excitation spectra of a supersonic molecular beam sample and absorption spectra of a cryogenic buffer-gas cooled sample were recorded. In addition, a novel spectroscopic technique based on laser-enhanced chemical reactions is demonstrated and used in 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 Ã2Π1/2(0,0,0) and X̃2Σ+(0,0,0) states. A comparison of the determined X̃2Σ+(0,0,0) hyperfine parameters with recently predicted values [Denis et al., J. Chem. Phys. 152, 084303 (2020); K. Gaul and R. Berger, Phys. Rev. A 101, 012508 (2020); and Liu et al., J. Chem. Phys. 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 Wd and WM, 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 Ã2Π1/2(0,0,0) and X̃2Σ+(0,0,0) states for all isotopologues of YbOH are discussed, and a comparison to isoelectronic YbF is made.

Quantum control of trapped polyatomic molecules for eEDM searches.

Ultracold polyatomic molecules are promising candidates for experiments in quantum science and precision searches for physics beyond the Standard Model. A key requirement is the ability to achieve full quantum control over the internal structure of the molecules. In this work, we established coherent control of individual quantum states in calcium monohydroxide (CaOH) and demonstrated a method for searching for the electron electric dipole moment (eEDM). Optically trapped, ultracold CaOH molecules were prepared in a single quantum state, polarized in an electric field, and coherently transferred into an eEDM-sensitive state where an electron spin precession measurement was performed. To extend the coherence time, we used eEDM-sensitive states with tunable, near-zero magnetic field sensitivity. Our results establish a path for eEDM searches with trapped polyatomic molecules.