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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 demonstrate that the isotope shift in isotopomers of diatomic molecules, where the nucleus of one of its constituent atoms is replaced by another isotope, can be expressed as the sum of a field shift and a mass shift, similar to the atomic case. We show that a linear relation holds between atomic and molecular isotopes shifts, thus extending the King-plot analysis to molecular isotope shifts. Optical isotope shifts in YbF and ZrO and infrared isotope shifts in SnH are analyzed with a molecular King-plot approach, utilizing Yb$^{+}$ and Zr$^{+}$ ionic isotope shifts and charge radii of Sn obtained with non-optical methods. The changes in the mean-squared nuclear charge radii $\delta \langle r^2 \rangle$ of $^{170-174,176}$Yb and $^{90-92,94,96}$Zr extracted from the molecular transitions are found to be in excellent agreement with the values from the spectroscopy of Yb$^{+}$ and Zr$^{+}$, respectively. On the contrary, in the case of the vibrational-rotational transition in SnH, no sensitivity to the nuclear volume could be deduced within the experimental resolution, which makes it unsuitable for the extraction of nuclear charge radii but provides insights into the molecular electronic wave function not accessible via other methods. The new opportunities offered by the molecular King-plot analysis for research in nuclear structure and molecular physics are discussed., Comment: Accepted at Physical Review X. Link to abstract: https://journals.aps.org/prx/accepted/be075Kf7E0c16505459d9fa833408356a593fd904

Recently a breakthrough has been achieved in laser-spectroscopic studies of short-lived radioactive compounds with the first measurements of the radium monofluoride molecule (RaF) UV/vis spectra. We report results from high accuracy \emph{ab initio} calculations of the RaF electronic structure for ground and low-lying excited electronic states. Two different methods agree excellently with experimental excitation energies from the electronic ground state to the $^2\Pi_{1/2}$ and $^2\Pi_{3/2}$ states, but lead consistently and unambiguously to deviations from experimental-based adiabatic transition energy estimates for the $^2\Sigma_{1/2}$ excited electronic state and show that more measurements are needed to clarify spectroscopic assignment of the $^2\Delta$ states., Comment: 7 pages, 1 figure, 1 table

In this study, we present the ro-vibrationally resolved gas-phase spectrum of the diatomic molecule TiO around 1000\,cm$^{-1}$. Molecules were produced in a laser ablation source by vaporizing a pure titanium sample in the atmosphere of gaseous nitrous oxide. Adiabatically expanded gas, containing TiO, formed a supersonic jet and was probed perpendicularly to its propagation by infrared radiation from quantum cascade lasers. Fundamental bands of $^{46-50}$TiO and vibrational hotbands of $^{48}$TiO are identified and analyzed. In a mass-independent fitting procedure combining the new infrared data with pure rotational and electronic transitions from the literature, a Dunham-like parameterization is obtained. From the present data set, the multi-isotopic analysis allows to determine the spin-rotation coupling constant $\gamma$ and the Born-Oppenheimer correction coefficient $\Delta_{\rm U_{10}}^{\mathrm{Ti}}$ for the first time. The parameter set enables to calculate the Born-Oppenheimer correction coefficients $\Delta_{\rm U_{02}}^{\mathrm{Ti}}$ and $\Delta_{\rm U_{02}}^{\mathrm{O}}$. In addition, the vibrational transition moments for the observed vibrational transitions are reported., Comment: 2 figures

More than 130 pure rotational transitions of $^{46}$TiO, $^{47}$TiO, $^{48}$TiO, $^{49}$TiO, $^{50}$TiO, and $^{48}$Ti$^{18}$O are recorded using a high-resolution mm-wave supersonic jet spectrometer in combination with a laser ablation source. For the first time a mass-independent Dunham-like analysis is performed encompassing rare titanium monoxide isotopologues, and are compared to results from high-accuracy quantum-chemical calculations. The obtained parametrization reveals for titanium monoxide effects due to deviations from the Born-Oppenheimer approximation. Additionally, the dominant titanium properties enable an insight into the electronic structure of TiO by analyzing its hyperfine interactions. Further, based on the mass-independent analysis, the frequency positions of the pure rotational transitions of the short lived rare isotopologue $^{44}$TiO are predicted with high accuracy, i.e., on a sub-MHz uncertainty level. This allows for dedicated radio-astronomical searches of this species in core-collapse environments of supernovae., Comment: 29 pages, 3 figures

We report the first detection of the isotopologues 13CCC and C13CC. We used the heterodyne receivers GREAT and upGREAT on board SOFIA to search for the ro-vibrational transitions Q(2) and Q(4) of 13CCC and C13CC at 1.9 THz along the line of sight towards SgrB2(M). For both species the ro-vibrational absorption lines Q(2) and Q(4) have been identified, primarily arising from the warm gas physically associated with the strong continuum source SgrB2(M). In addition, to determine the local excitation temperature we analyzed data from nine ro-vibrational transitions of the main isotopologue CCC in the frequency range between 1.6-1.9 THz which were taken from the Herschel Science Data Archive, and derived a gas excitation temperature of Tex = 44.4(+4.7/-3.9) K and a total column density of N(CCC)=3.88(+0.39/-0.35)x10^15 cm^-2. Assuming the excitation temperatures of C13CC and 13CCC to be the same as for CCC, we obtained column densities of the 13C-isotopologues of N(C13CC) = 2.1(+0.9/-0.6)X10^14 cm^-2 and N(13CCC)=2.4(+1.2/-0.8)x10^14 cm^-2. The derived 12C/13C abundance ratio in the C3 molecules is 20.5(4.2), which is in agreement with the elemental ratio of 20, typically observed in SgrB2(M). However, we find the N(13CCC) / N(C13CC) ratio to be 1.2(0.1), which is shifted from the statistically expected value of 2. We propose that the discrepant abundance ratio arises due to the lower zero-point energy of C13CC which makes position exchange reaction converting 13CCC to C13CC energetically favorable., Comment: 7 pages, 4 figures, 5 tables

Decades ago, $\gamma$-ray observatories identified diffuse Galactic emission at 1.809 MeV originating from $\beta^+$ decays of an isotope of aluminium, $^{26}$Al, that has a mean-life time of 1.04 Myr. Objects responsible for the production of this radioactive isotope have never been directly identified, owing to insufficient angular resolutions and sensitivities of the $\gamma$-ray observatories. Here, we report observations of millimetre-wave rotational lines of the isotopologue of aluminium monofluoride that contains the radioactive isotope ($^{26}$AlF). The emission is observed toward CK Vul which is thought to be a remnant of a stellar merger. Our constraints on the production of $^{26}$Al combined with the estimates on the merger rate make it unlikely that objects similar to CK Vul are major producers of Galactic $^{26}$Al. However, the observation may be a stepping stone for unambiguous identification of other Galactic sources of $^{26}$Al. Moreover, a high content of $^{26}$Al in the remnant indicates that prior to the merger, the CK Vul system contained at least one solar-mass star that evolved to the red giant branch., Comment: 18 pages, accepted to Nature Astronomy