Showing 1–12 of 12 results for author: Au, M

Energies and lifetimes of the 9p and 10p excited states in atomic francium

Authors: P. Lassègues, A. Ajayakumar, M. Athanasakis-Kaklamanakis, O. Ahmad, M. Au, J. Berbalk, D. Bettaney, B. van den Borne, A. Chakraborty, T. E. Cocolios, M. Duggan, C. Fajardo, K. T. Flanagan, R. F. Garcia Ruiz, R. de Groote, D. Gonzalez-Acevedo, A. Kastberg, A. Koszorús, L. Lalanne, K. M. Lynch, D. T. McLeroy, A. McGlone, G. Neyens, L. Nies, L. Quanjel , et al. (7 additional authors not shown)

Abstract: We present the first measurement of 9p 2P1/2,3/2 and 10p 2P1/2,3/2 excited levels absolute wavenumbers and radiative lifetime in francium. We used the Collinear Resonance Ionization Spectroscopy (CRIS) technique, applied on a beam of 221Fr atoms. Prior to this work, no experimental data existed for francium p-states with n > 8. The results provide a precision experimental test of relativistic coup… ▽ More We present the first measurement of 9p 2P1/2,3/2 and 10p 2P1/2,3/2 excited levels absolute wavenumbers and radiative lifetime in francium. We used the Collinear Resonance Ionization Spectroscopy (CRIS) technique, applied on a beam of 221Fr atoms. Prior to this work, no experimental data existed for francium p-states with n > 8. The results provide a precision experimental test of relativistic coupled-cluster theory for the heaviest alkali, showing good agreement for lifetimes and relative excitation energies, despite a residual global offset in absolute energies. △ Less

Submitted 12 May, 2026; v1 submitted 14 April, 2026; originally announced April 2026.

Laser spectroscopy and CP-violation sensitivity of actinium monofluoride

Authors: M. Athanasakis-Kaklamanakis, M. Au, A. Kyuberis, C. Zülch, K. Gaul, H. Wibowo, L. Skripnikov, L. Lalanne, J. R. Reilly, A. Koszorús, S. Bara, J. Ballof, R. Berger, C. Bernerd, A. Borschevsky, A. A. Breier, K. Chrysalidis, T. E. Cocolios, R. P. de Groote, A. Dorne, J. Dobaczewski, C. M. Fajardo Zambrano, K. T. Flanagan, S. Franchoo, J. D. Johnson , et al. (17 additional authors not shown)

Abstract: 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 ha… ▽ More 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. △ Less

Submitted 7 July, 2025; originally announced July 2025.

Comments: Submitted

Journal ref: Nature 648 (2025) 562

Theoretical determination of the ionization potentials of ScF, YF, LaF and AcF

Authors: Aleksandra A. Kyuberis, Lukas F. Pasteka, Ephraim Eliav, Ayaki Sunaga, Mia Au, Shane G. Wilkins, Anastasia Borschevsky

Abstract: We present a comprehensive theoretical study of the ionization potentials of the MF (M = Sc, Y, La, Ac) molecules using the state-of-the-art relativistic coupled cluster approach with single, double, and perturbative triple excitations (CCSD(T)). We have further corrected our results for higherorder excitations (up to full triples), the QED self-energy and vacuum-polarization contributions. We hav… ▽ More We present a comprehensive theoretical study of the ionization potentials of the MF (M = Sc, Y, La, Ac) molecules using the state-of-the-art relativistic coupled cluster approach with single, double, and perturbative triple excitations (CCSD(T)). We have further corrected our results for higherorder excitations (up to full triples), the QED self-energy and vacuum-polarization contributions. We have extensively investigated the effect of the various computational parameters on the calculated ionization potentials, allowing us to assign realistic uncertainties to our predictions. △ Less

Submitted 7 February, 2025; originally announced February 2025.

Ionization potential of radium monofluoride

Authors: S. G. Wilkins, H. A. Perrett, S. M. Udrescu, A. A. Kyuberis, L. F. Pašteka, M. Au, I. Belošević, R. Berger, C. L. Binnersley, M. L. Bissell, A. Borschevsky, A. A. Breier, A. J. Brinson, K. Chrysalidis, T. E. Cocolios, B. S. Cooper, R. P. de Groote, A. Dorne, E. Eliav, R. W. Field, K. T. Flanagan, S. Franchoo, R. F. Garcia Ruiz, K. Gaul, S. Geldhof , et al. (21 additional authors not shown)

Abstract: 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 th… ▽ More 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. △ Less

Submitted 21 October, 2024; v1 submitted 26 August, 2024; originally announced August 2024.

Radiative lifetime of the A 2Π1/2 state in RaF with relevance to laser cooling

Authors: M. Athanasakis-Kaklamanakis, S. G. Wilkins, P. Lassègues, L. Lalanne, J. R. Reilly, O. Ahmad, M. Au, S. W. Bai, J. Berbalk, C. Bernerd, A. Borschevsky, A. A. Breier, K. Chrysalidis, T. E. Cocolios, R. P. de Groote, C. M. Fajardo-Zambrano, K. T. Flanagan, S. Franchoo, R. F. Garcia Ruiz, D. Hanstorp, R. Heinke, P. Imgram, A. Koszorús, A. A. Kyuberis, J. Lim , et al. (16 additional authors not shown)

Abstract: The radiative lifetime of the $A$ $^2 Π_{1/2}$ (v=0) state in radium monofluoride (RaF) is measured to be 35(1) ns. The lifetime of this state and the related decay rate $Γ= 2.86(8) \times 10^7$ $s^{-1}$ are of relevance to the laser cooling of RaF via the optically closed $A$ $^2 Π_{1/2} \leftarrow X$ $^2Σ_{1/2}$ transition, which makes the molecule a promising probe to search for new physics. Ra… ▽ More The radiative lifetime of the $A$ $^2 Π_{1/2}$ (v=0) state in radium monofluoride (RaF) is measured to be 35(1) ns. The lifetime of this state and the related decay rate $Γ= 2.86(8) \times 10^7$ $s^{-1}$ are of relevance to the laser cooling of RaF via the optically closed $A$ $^2 Π_{1/2} \leftarrow X$ $^2Σ_{1/2}$ 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. △ Less

Submitted 6 June, 2024; v1 submitted 14 March, 2024; originally announced March 2024.

Comments: Accepted as a Letter in Physical Review A; 8 pages of main text, 5 pages of supplemental material

Pre-Flight Calibration of PIXL for X-ray Fluorescence Elemental Quantification

Authors: Christopher M. Heirwegh, William Timothy Elam, Yang Liu, Anusheela Das, Christopher Hummel, Bret Naylor, Lawrence A. Wade, Abigail C. Allwood, Joel A. Hurowitz, Les G. Armstrong, Naomi Bacop, Lauren P. O'Neil, Kimberly P. Sinclair, Michael E. Sondheim, Robert W. Denise, Peter R. Lawson, Rogelio Rosas, Jonathan H. Kawamura, Mitchell H. Au, Amarit Kitiyakara, Marc C. Foote, Raul A. Romero, Mark S. Anderson, George R. Rossman, Benton C. Clark III

Abstract: The Planetary Instrument for X-ray Lithochemistry (PIXL) is a rasterable focused-beam X-ray fluorescence (XRF) spectrometer mounted on the arm of National Aeronautics and Space Administration's (NASA) Mars 2020 Perseverance rover. To ensure that PIXL would be capable of performing accurate in-flight compositional analysis of martian targets, in situ, an elemental calibration was performed pre-flig… ▽ More The Planetary Instrument for X-ray Lithochemistry (PIXL) is a rasterable focused-beam X-ray fluorescence (XRF) spectrometer mounted on the arm of National Aeronautics and Space Administration's (NASA) Mars 2020 Perseverance rover. To ensure that PIXL would be capable of performing accurate in-flight compositional analysis of martian targets, in situ, an elemental calibration was performed pre-flight on the PIXL flight instrument in a simulated martian environment. The details of this calibration, and implications for measuring unknown materials on Mars are the subjects of this paper. The major goals of this calibration were both to align the spectrometer to perform accurate elemental analysis and, to derive a matrix of uncertainties that are applied to XRF measurements of all elements in unknown materials. A small set of pure element and pure compound targets and geologically relevant reference materials were measured with the flight hardware in a simulated martian environment. Elemental calibration and quantifications were carried out using PIXL's XRF quantification software (PIQUANT). Uncertainties generated were implemented into the PIQUANT software version employed by the PIXL's data visualization software (PIXLISE). We outline in this work, a list of factors that impact micro-XRF accuracy, the methodology and steps involved in the calibration, details on the fabrication of the uncertainty matrix, instructions on the use and interpretations of the uncertainties applied to unknowns and an assessment on the limitations and areas open to future improvement as part of subsequent calibration efforts. △ Less

Submitted 2 February, 2024; originally announced February 2024.

Observation of the distribution of nuclear magnetization in a molecule

Authors: S. G. Wilkins, S. M. Udrescu, M. Athanasakis-Kaklamanakis, R. F. Garcia Ruiz, M. Au, I. Belošević, R. Berger, M. L. Bissell, A. A. Breier, A. J. Brinson, K. Chrysalidis, T. E. Cocolios, R. P. de Groote, A. Dorne, K. T. Flanagan, S. Franchoo, K. Gaul, S. Geldhof, T. F. Giesen, D. Hanstorp, R. Heinke, T. Isaev, Á. Koszorús, S. Kujanpää, L. Lalanne , et al. (11 additional authors not shown)

Abstract: 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 proper… ▽ More 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. △ Less

Submitted 23 October, 2025; v1 submitted 7 November, 2023; originally announced November 2023.

Journal ref: Science 390(6771):386-389 (2025)

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

Authors: M. Athanasakis-Kaklamanakis, S. G. Wilkins, L. V. Skripnikov, A. Koszorús, A. A. Breier, O. Ahmad, M. Au, S. W. Bai, I. Belošević, J. Berbalk, R. Berger, C. Bernerd, M. L. Bissell, A. Borschevsky, A. Brinson, K. Chrysalidis, T. E. Cocolios, R. P. de Groote, A. Dorne, C. M. Fajardo-Zambrano, R. W. Field, K. T. Flanagan, S. Franchoo, R. F. Garcia Ruiz, K. Gaul , et al. (31 additional authors not shown)

Abstract: 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… ▽ More 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. △ Less

Submitted 20 December, 2024; v1 submitted 28 August, 2023; originally announced August 2023.

Comments: Significant changes compared to previous version with additional experimental data. Accepted for publication under a different title

Ab initio study of electronic states and radiative properties of the AcF molecule

Authors: Leonid V. Skripnikov, Alexander V. Oleynichenko, Andréi Zaitsevskii, Nikolai S. Mosyagin, Michail Athanasakis-Kaklamanakis, Mia Au, Gerda Neyens

Abstract: Relativistic coupled-cluster calculations of the ionization potential, dissociation energy, and excited electronic states under 35,000 cm$^{-1}$ are presented for the actinium monofluoride (AcF) molecule. The ionization potential is calculated to be IP$_e=48,866$ cm$^{-1}$, and the ground state is confirmed to be a closed-shell singlet and thus strongly sensitive to the $\mathcal{T}$,… ▽ More Relativistic coupled-cluster calculations of the ionization potential, dissociation energy, and excited electronic states under 35,000 cm$^{-1}$ are presented for the actinium monofluoride (AcF) molecule. The ionization potential is calculated to be IP$_e=48,866$ cm$^{-1}$, and the ground state is confirmed to be a closed-shell singlet and thus strongly sensitive to the $\mathcal{T}$,$\mathcal{P}$-violating nuclear Schiff moment of the Ac nucleus. Radiative properties and transition dipole moments from the ground state are identified for several excited states, achieving an uncertainty of $\sim$450 cm$^{-1}$ for the excitation energies. For higher-lying states that are not directly accessible from the ground state, possible two-step excitation pathways are proposed. The calculated branching ratios and Franck-Condon factors are used to investigate the suitability of AcF for direct laser cooling. The lifetime of the metastable $(1)^3Δ_1$ state, which can be used in experimental searches of the electric dipole moment of the electron, is estimated to be of order 1 ms. △ Less

Submitted 11 May, 2023; originally announced May 2023.

Journal ref: J. Chem. Phys. 159, 124301 (2023)

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

Authors: M. Au, M. Athanasakis-Kaklamanakis, L. Nies, J. Ballof, R. Berger, K. Chrysalidis, P. Fischer, R. Heinke, J. Johnson, U. Köster, D. Leimbach, B. Marsh, M. Mougeot, J. Reilly, E. Reis, M. Schlaich, Ch. Schweiger, L. Schweikhard, S. Stegemann, J. Wessolek, F. Wienholtz, S. G. Wilkins, W. Wojtaczka, Ch. E. Düllmann, S. Rothe

Abstract: 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 s… ▽ More 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. △ Less

Submitted 21 March, 2023; originally announced March 2023.

Comments: 6 pages, 7 figures

Opportunities for Fundamental Physics Research with Radioactive Molecules

Authors: Gordon Arrowsmith-Kron, Michail Athanasakis-Kaklamanakis, Mia Au, Jochen Ballof, Robert Berger, Anastasia Borschevsky, Alexander A. Breier, Fritz Buchinger, Dmitry Budker, Luke Caldwell, Christopher Charles, Nike Dattani, Ruben P. de Groote, David DeMille, Timo Dickel, Jacek Dobaczewski, Christoph E. Düllmann, Ephraim Eliav, Jon Engel, Mingyu Fan, Victor Flambaum, Kieran T. Flanagan, Alyssa Gaiser, Ronald Garcia Ruiz, Konstantin Gaul , et al. (37 additional authors not shown)

Abstract: 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 seve… ▽ More 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. △ Less

Submitted 4 February, 2023; originally announced February 2023.

Journal ref: Rep. Prog. Phys. 87 084301 (2024)

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

Authors: J. Ballof, M. Au, E. Barbero, K. Chrysalidis, Ch. E. Düllmann, V. Fedosseev, E. Granados, R. Heinke, B. Marsh, M. Owen, S. Rothe, T. Stora, A. Yakushev

Abstract: 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 °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 availabl… ▽ More 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 °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. △ Less

Submitted 4 April, 2022; v1 submitted 1 October, 2021; originally announced October 2021.