Collective effects in 229Th-doped crystals

Brenden Nickerson, Wen-Te Liao, and Adriana Pálffy


Vacuum-ultraviolet-transparent crystals have been proposed as host lattice for the coherent driving of the unusually low-lying isomer excitation in 229Th for metrology and quantum optics applications. Here the possible collective effects occurring for the coherent pulse propagation in the crystal system are investigated theoretically. We consider the effect of possible doping sites, quantization axis orientation, and pulse configurations on the scattered light intensity and signatures of nuclear excitation. Our results show that for narrow-pulse driving, the rather complicated quadrupole splitting of the level scheme is significantly simplified. Furthermore, we investigate complex driving schemes with a combination of pulsed fields and investigate the occurring interference process. Our theoretical results support experimental attempts for first direct driving of the nuclear transition with coherent light.

Nuclear Charge Radii of 229Th from Isotope and Isomer Shifts

M. S. Safronova, S. G. Porsev, M. G. Kozlov, J. Thielking, M. V. Okhapkin, P. Głowacki, D. M. Meier, and E. Peik


The isotope 229Th is unique in that it possesses an isomeric state of only a few electron volts above the ground state, suitable for nuclear laser excitation. An optical clock based on this transition is expected to be a very sensitive probe for variations of fundamental constants, but the nuclear properties of both states have to be determined precisely to derive the actual sensitivity. We carry out isotope shift calculations in Th+ and Th2+ including the specific mass shift, using a combination of configuration interaction and all-order linearized coupled-cluster methods and estimate the uncertainty of this approach. We perform experimental measurements of the hyperfine structure of Th2+ and isotopic shift between 229Th2+ and 232Th2+ to extract the difference in root-mean-square radii as δr2232,229=0.299(15)fm2. Using the recently measured values of the isomer shift of lines of 229mTh, we derive the value for the mean-square radius change between 229Th and its low-lying isomer 229mTh to be δr2229m,229=0.0105(13)fm2.

Hyperfine interaction with the 229Th nucleus and its low lying isomeric state

Robert A. Müller, Anna V. Maiorova, Stephan Fritzsche, Andrey V. Volotka, Randolf Beerwerth, Przemyslaw Glowacki, Johannes Thielking, David-Marcel Meier, Maksim Okhapkin, Ekkehard Peik, Andrey Surzhykov


The thorium nucleus with mass number A=229 has attracted much interest because its extremely low lying first excited isomeric state at about 8eV opens the possibility for the development of a nuclear clock. However, neither the exact energy of this nuclear isomer nor properties, such as nuclear magnetic dipole and electric quadrupole moment are known to a high precision so far. The latter can be determined by investigating the hyperfine structure of thorium atoms or ions. Due to its electronic structure and the long lifetime of the nuclear isomeric state, Th2+ is especially suitable for such kind of studies. In this letter we present a combined experimental and theoretical investigation of the hyperfine structure of the 229Th2+ ion in the nuclear ground and isomeric state. A very good agreement between theory and experiment is found for the nuclear ground state. Moreover, we use our calculations to confirm the recently presented experimental value for the nuclear magnetic dipole moment of the thorium nuclear isomer, which was in contradiction to previous theoretical studies.

Non-perturbative generation of DUV/VUV harmonics from crystal surfaces at 108 MHz repetition rate

J. Seres, E. Seres, C. Serrat, and T. Schumm


We demonstrate non-perturbative 3rd (267 nm) and 5th (160 nm) harmonic generation in solids from a Ti:sapphire frequency comb (800 nm) at 108 MHz repetition rate. The experiments show that non-perturbative low harmonics are dominantly generated on the surface and on the interface between solids, and that they are not produced by bulk processes from the near-surface layer of the material. Measurements reveal that due to the lack of phase matching, the generated harmonics in bulk are suppressed by orders of magnitude compared to the signal generated on the surface. Our results pave the way for the development of all-solid-state high repetition rate harmonic sources for vacuum ultraviolet spectroscopy and high precision frequency comb metrology.

Toward an energy measurement of the internal conversion electron in the deexcitation of the 229Th isomer

Simon Stellmer, Yudai Shigekawa, Veronika Rosecker, Georgy A. Kazakov, Yoshitaka Kasamatsu, Yuki Yasuda, Atsushi Shinohara, and Thorsten Schumm


The first excited isomeric state of Th-229 has an exceptionally low energy of only a few eV and could form the gateway to high-precision laser spectroscopy of nuclei. The excitation energy of the isomeric state has been inferred from precision γ spectroscopy, but its uncertainty is still too large to commence laser spectroscopy. Reducing this uncertainty is one of the most pressing challenges in the field. Here we present an approach to infer the energy of the isomer from spectroscopy of the electron which is emitted when the isomer de-excites through internal conversion (IC). The experiment builds on U-233, which α-decays to Th-229 and populates the isomeric state with a 2% branching ratio. A film of U-233 is covered by a stopping layer of few-nm thickness and placed between an α detector and an electron detector, such that the α particle and the IC electron can be detected in coincidence. Retarding field electrodes allow for an energy measurement. In the present design, the signal of the Th-229m IC electrons is masked by low-energy electrons emitted from the surface of the metallic stopping layer. We perform reference measurements with U-232 and U-234 to study systematic effects, and we study various means to reduce the background of low-energy electrons. Our study gives guidelines to the design of an experiment that is capable of detecting the IC electrons and measuring the isomer energy.

On an attempt to optically excite the nuclear isomer in Th-229

Simon Stellmer, Georgy Kazakov, Matthias Schreitl, Hendrik Kaser, Michael Kolbe, and Thorsten Schumm


We aim to perform direct optical spectroscopy of the Th-229 nuclear isomer to measure its energy and lifetime, and to demonstrate optical coupling to the nucleus. To this end, we develop Th-doped CaF2 crystals, which are transparent at the anticipated isomer wavelength. Such crystals are illuminated by tunable VUV undulator radiation for direct excitation of the isomer. We scan a 5 sigma region around the assumed isomer energy of 7.8(5) eV and vary the excitation time in sequential scans between 30 and 600 seconds. Suffering from an unforeseen strong photoluminescence of the crystal, the experiment is sensitive only to radiative isomer lifetimes between 0.2 and 1.1 seconds. For this parameter range, and assuming radiative decay as the dominant de-excitation channel, we can exclude an isomer with energy between 7.5 and 10 eV at the 95% confidence level.

Towards a 229Th-Based Nuclear Clock

Lars von der Wense, Benedict Seiferle, and Peter G. Thirolf


An overview of the current status of the development of a nuclear clock based on the state of lowest known nuclear excitation energy in 229Th is presented. The text is especially written for the interested reader without any particular knowledge in this field of research. It is thus ideal as an introductory reading to get a broad overview of the various different aspects of the field; in addition, it can serve as a guideline for future research. An introductory part is provided, giving a historic context and explaining the fundamental concept of clocks. Finally, potential candidates for nuclear clocks other than 229Th are discussed.

Nuclear resonant scattering experiment with fast time response: Photonuclear excitation of 201Hg

A. Yoshimi, H. Hara, T. Hiraki, Y. Kasamatsu, S. Kitao, Y. Kobayashi, K. Konashi, R. Masuda, T. Masuda, Y. Miyamoto, K. Okai, S. Okubo, R. Ozaki, N. Sasao, O. Sato, M. Seto, T. Schumm, Y. Shigekawa, S. Stellmer, K. Suzuki, S. Uetake, M. Watanabe, A. Yamaguchi, Y. Yasuda, Y. Yoda, K. Yoshimura, M. Yoshimura


Nuclear resonant excitation and detection of its decay signal for the 26.27-keV level of 201Hg is demonstrated with high-brilliance synchrotron radiation (SR) and a fast x-ray detector system. This SR-based photonuclear excitation scheme, known as nuclear resonant scattering (NRS) in the field of materials science, is also useful for investigating nuclear properties, such as the half-lives and radiative widths of excited nuclear levels. To date, because of the limited time response of the x-ray detector, the nuclear levels to which this method could be applied have been limited to the one whose half-lives are longer than ∼1 ns. The faster time response of the NRS measurement makes possible NRS experiments on nuclear levels with much shorter half-lives. We have fabricated an x-ray detector system that has a time resolution of 56 ps and a shorter tail function than that reported previously. With the implemented detector system, the NRS signal of the 26.27-keV state of 201 Hg could be clearly discriminated from the electronic scattering signal at an elapsed time of 1 ns after the SR pulse. The half-life of the state was determined as 629 ± 18 ps, which has better precision by a factor of three compared with that reported to date obtained from nuclear decay spectroscopy.

Nonlinear Pulse Compression to Sub-40 fs at 4.5 μJ Pulse Energy by Multi-Pass-Cell Spectral Broadening

Johannes Weitenberg, Tobias Saule, Jan Schulte, and Peter Rußbüldt


We report on the pulse compression of an 18.5 MHz repetition rate pulse train from 230 fs to sub-40 fs by nonlinear spectral broadening in a multi-pass cell and subsequent chirp removal. The compressed pulse energy is 4.5 μJ, which corresponds to 84 W of average power, with a compression efficiency of 88%. This recently introduced compression scheme is suitable for a large pulse energy range and for high average power. In this paper, we show that it can achieve three times shorter pulses than previously demonstrated.

A Laser Excitation Scheme for 229mTh

Lars von der Wense, Benedict Seiferle, Simon Stellmer, Johannes Weitenberg, Georgy Kazakov, Adriana Pálffy, and Peter G. Thirolf


Direct laser excitation of the lowest known nuclear excited state in 229Th has been a long-standing objective. It is generally assumed that reaching this goal would require a considerably reduced uncertainty of the isomer’s excitation energy compared to the presently adopted value of (7.8±0.5)eV. Here we present a direct laser excitation scheme for 229mTh, which circumvents this requirement. The proposed excitation scheme makes use of already existing laser technology and therefore paves the way for nuclear laser spectroscopy. In this concept, the recently experimentally observed internal-conversion decay channel of the isomeric state is used for probing the isomeric population. A signal-to-background ratio of better than 104 and a total measurement time of less than three days for laser scanning appear to be achievable.

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