arXiv subjects

S. Rothe

Publications and source records attributed to S. Rothe.

At least 19 recordsLinked to original sources

arXiv2026

Exploring $\alpha$- and $\beta$-decay-induced quenching of the $^{229}$Th nuclear-clock isomer in solid-state hosts

The radiative decay dynamics of an ensemble of $^{229\mathrm{m}}$Th nuclei embedded in CaF$_2$ and MgF$_2$ is investigated. The isomer is populated through $\beta$ decay of $^{229}$Ac following ion implantation, and its radiative decay is detected using vacuum-ultraviolet spectroscopy and measured as a function of time. This allows to identify and quantify the quenching of the radiative-decay signal induced by $\alpha$ or $\beta$ radiation. The quenching probability density is determined in different CaF$_2$ crystals and in a MgF$_2$ crystal, revealing differences up to two orders of magnitude between the investigated samples and a strong dependence on the host material and defect densities. The results support a microscopic mechanism mediated by charge carriers in which electronic excitations created by the decay radiation are captured near Th defects, thereby favoring non-radiative decay channels.

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arXiv2025

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↗

arXiv2025

Reduction in nuclear size and quadrupole deformation of high-spin isomers of 127,129In

We employed laser spectroscopy of atomic transitions to measure the nuclear charge radii and electromagnetic properties of the high-spin isomeric states in neutron-rich indium isotopes (Z = 49) near the closed proton and neutron shells at Z = 50 and N = 82. Our data reveal a reduction in the nuclear charge radius and intrinsic quadrupole moment when protons and neutrons are fully aligned in 129In(N = 80), to form the high spin isomer. Such a reduction is not observed in 127In(N = 78), where more complex configurations can be formed by the existence of four neutron-holes. These observations are not consistently described by nuclear theory.

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arXiv2024

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↗

arXiv2024

Radiative Decay of the $^{229m}$Th Nuclear Clock Isomer in Different Host Materials

A comparative vacuum ultraviolet spectroscopy study conducted at ISOLDE-CERN of the radiative decay of the $^{229m}$Th nuclear clock isomer embedded in different host materials is reported. The ratio of the number of radiative decay photons and the number of $^{229m}$Th embedded are determined for single crystalline CaF$_2$, MgF$_2$, LiSrAlF$_6$, AlN, and amorphous SiO$_2$. For the latter two materials, no radiative decay signal was observed and an upper limit of the ratio is reported. The radiative decay wavelength was determined in LiSrAlF$_6$ and CaF$_2$, reducing its uncertainty by a factor of 2.5 relative to our previous measurement. This value is in agreement with the recently reported improved values from laser excitation.

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arXiv2024

Radiative lifetime of the A 2{\Pi}1/2 state in RaF with relevance to laser cooling

The radiative lifetime of the $A$ $^2 \Pi_{1/2}$ (v=0) state in radium monofluoride (RaF) is measured to be 35(1) ns. The lifetime of this state and the related decay rate $\Gamma = 2.86(8) \times 10^7$ $s^{-1}$ are of relevance to the laser cooling of RaF via the optically closed $A$ $^2 \Pi_{1/2} \leftarrow X$ $^2\Sigma_{1/2}$ transition, which makes the molecule a promising probe to search for new physics. RaF is found to have a comparable photon-scattering rate to homoelectronic laser-coolable molecules. Thanks to its highly diagonal Franck-Condon matrix, it is expected to scatter an order of magnitude more photons than other molecules when using just 3 cooling lasers, before it decays to a dark state. The lifetime measurement in RaF is benchmarked by measuring the lifetime of the $8P_{3/2}$ state in Fr to be 83(3) ns, in agreement with literature.

physics.atom-ph↗

arXiv2023

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↗

arXiv2023

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↗

arXiv2023

In-source and in-trap formation of molecular ions in the actinide mass range at CERN-ISOLDE

The use of radioactive molecules for fundamental physics research is a developing interdisciplinary field limited dominantly by their scarce availability. In this work, radioactive molecular ion beams containing actinide nuclei extracted from uranium carbide targets are produced via the Isotope Separation On-Line technique at the CERN-ISOLDE facility. Two methods of molecular beam production are studied: extraction of molecular ion beams from the ion source, and formation of molecular ions from the mass-separated ion beam in a gas-filled radio-frequency quadrupole ion trap. Ion currents of U$^+$, UO$_{1-3}^+$, UC$_{1-3}^+$, UF$_{1-4}^+$, UF$_{1,2}$O$_{1,2}^+$ are reported. Metastable tantalum and uranium fluoride molecular ions are identified. Formation of UO$_{1-3}^+$, U(OH)$_{1-3}^+$, UC$_{1-3}^+$, UF$_{1,2}$O$_{1,2}^+$ from mass-separated beams of U$^+$, UF$_{1,2}^+$ with residual gas is observed in the ion trap. The effect of trapping time on molecular formation is presented.

physics.ins-det↗

arXiv2023

Production of neptunium and plutonium nuclides from uranium carbide using 1.4-GeV protons

Accelerator-based techniques are one of the leading ways to produce radioactive nuclei. In this work, the Isotope Separation On-Line method was employed at the CERN-ISOLDE facility to produce neptunium and plutonium from a uranium carbide target material using 1.4-GeV protons. Neptunium and plutonium were laser-ionized and extracted as 30-keV ion beams. A Multi-Reflection Time-of-Flight mass spectrometer was used for ion identification by means of time-of-flight measurements as well as for isobaric separation. Isotope shifts were investigated for the 395.6-nm ground state transition in $^{236,237,239}$Np and the 413.4-nm ground state transition in $^{236,239,240}$Pu. Rates of $^{235-241}$Np and $^{234-241}$Pu ions were measured and compared with predictions of in-target production mechanisms simulated with GEANT4 and FLUKA to elucidate the processes by which these nuclei, which contain more protons than the target nucleus, are formed. $^{241}$Pu is the heaviest nuclide produced and identified at a proton-accelerator-driven facility to date. We report the availability of neptunium and plutonium as two additional elements at CERN-ISOLDE and discuss the limit of accelerator-based isotope production at high-energy proton accelerator facilities for nuclides in the actinide region.

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arXiv2021

Charge radii, moments and masses of mercury isotopes across the N = 126 shell closure

Combining laser spectroscopy in a Versatile Arc Discharge and Laser Ion Source, with Penning-trap mass spectrometry at the CERN-ISOLDE facility, this work reports on mean-square charge radii of neutron-rich mercury isotopes across the $N = 126$ shell closure, the electromagnetic moments of $^{207}$Hg and more precise mass values of $^{206-208}$Hg. The odd-even staggering (OES) of the mean square charge radii and the kink at $N = 126$ are analyzed within the framework of covariant density functional theory (CDFT), with comparisons between different functionals to investigate the dependence of the results on the underlying single-particle structure. The observed features are defined predominantly in the particle-hole channel in CDFT, since both are present in the calculations without pairing. However, the magnitude of the kink is still affected by the occupation of the $1i_{11/2}$ and $2g_{9/2}$ orbitals with a dependence on the relative energies as well as pairing.

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arXiv2021

A cold electron-impact ion source driven by a photo-cathode -- New opportunities for the delivery of radioactive molecular beams?

The thick-target ISOL (Isotope mass Separation OnLine) method provides beams of more than 1000 radionuclides of 74 elements. The method is well established for elements with sufficiently high volatility at ca. 2000 {\deg}C. To extract non-volatile elements the formation of a volatile molecule is required. While successful in some cases (e.g. carbon or boron), most of these elements are not yet available as ISOL beam. A variety of volatile carrier molecules has been proposed for all elements produced in the target material, but their probability of survival during the extraction and ionization process is often limited by the high temperatures required for isotope diffusion in the thick targets and for ion source operation. While cold target concepts have already been proposed, the normal mode of operation of the typically used Versatile Arc Discharge Ion Source (VADIS) with a hot cathode is not well suited. Here, we report about first measurements with an electron-impact ion source operated at ambient temperature using electrons that were liberated via the photo-electric effect from a copper cathode.

physics.ins-det↗

arXiv2021

A concept for the extraction of the most refractory elements at CERN-ISOLDE as carbonyl complex ions

We introduce a novel thick-target concept tailored to the extraction of refractory 4d and 5d transition metal radionuclides of molybdenum, technetium, ruthenium and tungsten for radioactive ion beam production. Despite the more than 60-year old history of thick-target ISOL mass-separation facilities like ISOLDE, the extraction of the most refractory elements as radioactive ion beam has so far not been successful. In ordinary thick ISOL targets, their radioisotopes produced in the target are stopped within the condensed target material and have to diffuse through a solid material. Here, we present a concept which overcomes limitations associated with this method. We exploit the recoil momentum of nuclear reaction products for their release from the solid target material. They are thermalized in a carbon monoxide-containing atmosphere, in which volatile carbonyl complexes form readily at ambient temperature and pressure. This compound serves as volatile carrier for transport to the ion source. Excess carbon monoxide is removed by cryogenic gas separation to enable low pressures in the source region, in which the species are ionized and hence made available for radioactive ion beam formation. The setup is operated in batch mode, with the aim to extract isotopes having half-lives of at least several seconds. We report parameter studies of the key processes of the method, which validate this concept and which define the parameters for the setup. This would allow for the first time the extraction of radioactive molybdenum, tungsten and several other transition metals at thick-target ISOL facilities.

physics.ins-det↗

arXiv2021

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 $A^{2}{}{\Pi}_{1/2}\leftarrow X^{2}{}{\Sigma}^{+}$. 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↗

arXiv2020

Laser spectroscopy of neutron-rich $^{207,208}$Hg isotopes: Illuminating the kink and odd-even staggering in charge radii across the $N=126$ shell closure

The mean-square charge radii of $^{207,208}$Hg ($Z=80, N=127,128$) have been studied for the first time and those of $^{202,203,206}$Hg ($N=122,123,126$) remeasured by the application of in-source resonance-ionization laser spectroscopy at ISOLDE (CERN). The characteristic \textit{kink} in the charge radii at the $N=126$ neutron shell closure has been revealed, providing the first information on its behavior below the $Z=82$ proton shell closure. A theoretical analysis has been performed within relativistic Hartree-Bogoliubov and non-relativistic Hartree-Fock-Bogoliubov approaches, considering both the new mercury results and existing lead data. Contrary to previous interpretations, it is demonstrated that both the kink at $N=126$ and the odd-even staggering (OES) in its vicinity can be described predominately at the mean-field level, and that pairing does not need to play a crucial role in their origin. A new OES mechanism is suggested, related to the staggering in the occupation of the different neutron orbitals in odd- and even-$A$ nuclei, facilitated by particle-vibration coupling for odd-$A$ nuclei.

nucl-ex↗

arXiv2020

Detailed spectroscopy of doubly magic $^{132}$Sn

The structure of the doubly magic $^{132}_{50}$Sn$_{82}$ has been investigated at the ISOLDE facility at CERN, populated both by the $\beta^-$decay of $^{132}$In and $\beta^-$-delayed neutron emission of $^{133}$In. The level scheme of $^{132}$Sn is greatly expanded with the addition of 68 $\gamma$-transitions and 17 levels observed for the first time in the $\beta$ decay. The information on the excited structure is completed by new $\gamma$-transitions and states populated in the $\beta$-n decay of $^{133}$In. Improved delayed neutron emission probabilities are obtained both for $^{132}$In and $^{133}$In. Level lifetimes are measured via the Advanced Time-Delayed $\beta\gamma\gamma$(t) fast-timing method. An interpretation of the level structure is given based on the experimental findings and the particle-hole configurations arising from core excitations both from the \textit{N} = 82 and \textit{Z} = 50 shells, leading to positive and negative parity particle-hole multiplets. The experimental information provides new data to challenge the theoretical description of $^{132}$Sn.

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arXiv2020

The observation of vibrating pear shapes in radon nuclei: update

There is a large body of evidence that atomic nuclei can undergo octupole distortion and assume the shape of a pear. This phenomenon is important for measurements of electric-dipole moments of atoms, which would indicate CP violation and hence probe physics beyond the standard model of particle physics. Isotopes of both radon and radium have been identified as candidates for such measurements. Here, we have observed the low-lying quantum states in $^{224}$Rn and $^{226}$Rn by accelerating beams of these radioactive nuclei. We report here additional states not assigned in our 2019 publication. We show that radon isotopes undergo octupole vibrations but do not possess static pear-shapes in their ground states. We conclude that radon atoms provide less favourable conditions for the enhancement of a measurable atomic electric-dipole moment.

nucl-ex↗

arXiv2020

Evolution of Octupole Deformation in Radium Nuclei from Coulomb Excitation of Radioactive $^{222}$Ra and $^{228}$Ra Beams

There is sparse direct experimental evidence that atomic nuclei can exhibit stable pear shapes arising from strong octupole correlations. In order to investigate the nature of octupole collectivity in radium isotopes, electric octupole ($E3$) matrix elements have been determined for transitions in $^{222,228}$Ra nuclei using the method of sub-barrier, multi-step Coulomb excitation. Beams of the radioactive radium isotopes were provided by the HIE-ISOLDE facility at CERN. The observed pattern of $E$3 matrix elements for different nuclear transitions is explained by describing $^{222}$Ra as pear-shaped with stable octupole deformation, while $^{228}$Ra behaves like an octupole vibrator.

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