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K. Gaul

Publications and source records attributed to K. Gaul.

6 recordsLinked to original sources

Cold Hypersonic Gas Jets for Precision Laser Spectroscopy of Radioactive Molecules

The sensitivity to possible beyond standard model physics via a study of the nuclear Schiff moment (NSM) has since recently been driving laser spectroscopy of short-lived radioactive molecules. These experiments have in part been hindered by inefficient cooling of the molecular degrees of freedom, resulting in complex, difficult to interpret molecular spectra. Hypersonic (de Laval) nozzles have been shown to provide ideal environments to study cold short-lived actinides by means of in-gas-jet laser ionization spectroscopy. We present here the first application of this technique on molecules using $^{229,230,232}$ThO laser ablation targets. Translational and rotational temperatures were characterized via laser spectroscopy and found to be $12.5(25)\,\mathrm{K}$ and $7.2(6)\,\mathrm{K}$, respectively, along the nozzle-collimated $60\,\mathrm{mm}$-long, $5\,\mathrm{mm}$-diameter gas jet. An upper bound of the vibrational temperature was estimated as no transitions from $v''=1$ were observed. Molecular King-plot analysis shows a large field shift of $-4.0(13)\,\mathrm{cm}^{-1}/\mathrm{fm}^2$, indicating enhanced sensitivity to the differential nuclear charge radii. Relativistic FSCCSD calculations reproduce the measured molecular field-shift factor, providing a benchmark between state-of-the-art molecular and atomic calculations.

physics.atom-ph↗

Observation of the distribution of nuclear magnetization in a molecule

Rapid progress in the experimental control and interrogation of molecules, combined with developments in precise calculations of their structure, are enabling new opportunities in the investigation of nuclear and particle physics phenomena. Molecules containing heavy, octupole-deformed nuclei such as radium are of particular interest for such studies, offering an enhanced sensitivity to the properties of fundamental particles and interactions. Here, we report precision laser spectroscopy measurements and theoretical calculations of the structure of the radioactive radium monofluoride molecule, $^{225}$Ra$^{19}$F. Our results allow fine details of the short-range electron-nucleus interaction to be revealed, indicating the high sensitivity of this molecule to the distribution of magnetization, currently a poorly constrained nuclear property, within the radium nucleus. These results provide a direct and stringent test of the description of the electronic wavefunction inside the nuclear volume, highlighting the suitability of these molecules to investigate subatomic phenomena.

nucl-ex↗

Laser spectroscopy and CP-violation sensitivity of actinium monofluoride

The apparent invariance of the strong nuclear force under combined charge conjugation and parity (CP) remains an open question in modern physics. Precision experiments with heavy atoms and molecules can provide stringent constraints on CP violation via searches for effects due to permanent electric dipole moments and other CP-odd properties in leptons, hadrons, and nuclei. Radioactive molecules have been proposed as highly sensitive probes for such searches, but experiments with most such molecules have so far been beyond technical reach. Here we report the first production and spectroscopic study of a gas-phase actinium molecule, $^{227}$AcF. We observe the predicted strongest electronic transition from the ground state, which is necessary for efficient readout in searches of symmetry-violating interactions. Furthermore, we perform electronic- and nuclear-structure calculations for $^{227}$AcF to determine its sensitivity to various CP-violating parameters, and find that a realistic, near-term experiment with a precision of 1 mHz would improve current constraints on the CP-violating parameter hyperspace by three orders of magnitude. Our results thus highlight the potential of $^{227}$AcF for exceptionally sensitive searches of CP violation.

physics.atom-ph↗

Pinning down electron correlations in RaF via spectroscopy of excited states and high-accuracy relativistic quantum chemistry

We report the spectroscopy of the 14 lowest excited electronic states in the radioactive molecule radium monofluoride (RaF). The observed excitation energies are compared with fully relativistic state-of-the-art Fock-space coupled cluster (FS-RCC) calculations, which achieve an agreement of >=99.64% (within ~12 meV) with experiment for all states. Guided by theory, a firm assignment of the angular momentum and term symbol is made for 10 states and a tentative assignment for 4 states. The role of high-order electron correlation and quantum electrodynamics effects in the excitation energy of excited states is studied, found to be important for all states. Establishing the simultaneous accuracy and precision of calculations is an important step for research at the intersection of particle, nuclear, and chemical physics, including searches of physics beyond the Standard Model, for which RaF is a promising probe.

physics.atom-ph↗

Ionization potential of radium monofluoride

The ionization potential (IP) of radium monofluoride (RaF) was measured to be 4.969(2)[10] eV, revealing a relativistic enhancement in the series of alkaline earth monofluorides. The results are in agreement with a relativistic coupled-cluster prediction of 4.969[7] eV, incorporating up to quantum electrodynamics corrections. Using the same computational methodology, an improved calculation for the dissociation energy ($D_{0}$) of 5.54[5] eV is presented. This confirms that radium monofluoride joins the small group of diatomic molecules for which $D_{0}>\mathrm{IP}$, paving the way for precision control and interrogation of its Rydberg states.

physics.atom-ph↗

Isotope Shifts of Radium Monofluoride Molecules

Isotope shifts of $^{223-226,228}$Ra$^{19}$F were measured for different vibrational levels in the electronic transition $A^{2}{}Π_{1/2}\leftarrow X^{2}{}Σ^{+}$. The observed isotope shifts demonstrate the particularly high sensitivity of radium monofluoride to nuclear size effects, offering a stringent test of models describing the electronic density within the radium nucleus. Ab initio quantum chemical calculations are in excellent agreement with experimental observations. These results highlight some of the unique opportunities that short-lived molecules could offer in nuclear structure and in fundamental symmetry studies.

nucl-ex↗