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Abstract Polyatomic molecules have been identified as sensitive probes of charge-parity violating and parity violating physics beyond the Standard Model (BSM). For example, many linear triatomic molecules are both laser-coolable and have parity doublets in the ground electronic $\tilde{X}{}^2{\mathrm{\Sigma }}^{+}\left(010\right)$state arising from the bending vibration, both features that can greatly aid BSM searches. Understanding the $\tilde{X}{}^2{\mathrm{\Sigma }}^{+}\left(010\right)$state is a crucial prerequisite to precision measurements with linear polyatomic molecules. Here, we characterize the fundamental bending vibration of ${}^{174}$YbOH using high-resolution optical spectroscopy on the nominally forbidden $\tilde{X}{}^2{\mathrm{\Sigma }}^{+}\left(010\right)$ $\to \tilde{A}{}^2{\mathrm{\Pi }}_{1/2}\left(000\right)$transition at 588 nm. We assign 39 transitions originating from the lowest rotational levels of the $\tilde{X}{}^2{\mathrm{\Sigma }}^{+}\left(010\right)$state, and accurately model the state’s structure with an effective Hamiltonian using best-fit parameters. Additionally, we perform Stark and Zeeman spectroscopy on the $\tilde{X}{}^2{\mathrm{\Sigma }}^{+}\left(010\right)$state and fit the molecule-frame dipole moment to $D_{\mathrm{m}\mathrm{o}\mathrm{l}}=2.16\left(1\right)$Dand the effective electrong-factor to $g_S=2.07\left(2\right)$. Further, we use an empirical model to explain observed anomalous line intensities in terms of interference from spin–orbit and vibronic perturbations in the excited $\tilde{A}{}^2{\mathrm{\Pi }}_{1/2}\left(000\right)$state. Our work is an essential step toward searches for BSM physics in YbOH and other linear polyatomic molecules. 

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this manuscript, we review the scientific case for studying radioactive molecules, discuss recent atomic, molecular, nuclear, astrophysical, and chemical advances which provide the foundation for their study, describe the facilities where these species are and will be produced, and provide an outlook for the future of this nascent field. 

We propose to use atoms and molecules as quantum sensors of axion-mediated monopole-dipole forces. We show that electron spin precession experiments using atomic and molecular beams are well-suited for axion searches thanks to the presence of co-magnetometer states and single-shot temporal resolution. Experimental strategies to detect axion gradients from localised sources and the earth are presented, taking ACME III as a prototype example. Other possibilities including atomic beams, and laser-cooled atoms and molecules are discussed. 

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.