The concept of laser-based conversion electron Mössbauer spectroscopy for a precise energy determination of 229mTh

Lars C. von der Wense, Benedict Seiferle, Christian Schneider, Justin Jeet, Ines Amersdorffer, Nicolas Arlt, Florian Zacherl, Raphael Haas, Dennis Renisch, Patrick Mosel, Philip Mosel, Milutin Kovacev, Uwe Morgner, Christoph E. Düllmann, Eric R. Hudson, Peter G. Thirolf


229Th is the only nucleus currently under investigation for the development of a nuclear optical clock (NOC) of ultra-high accuracy. The insufficient knowledge of the first nuclear excitation energy of 229Th has so far hindered direct nuclear laser spectroscopy of thorium ions and thus the development of a NOC. Here, a nuclear laser excitation scheme is detailed, which makes use of thorium atoms instead of ions. This concept, besides potentially leading to the first nuclear laser spectroscopy, would determine the isomeric energy to 40 μeV resolution, corresponding to 10 GHz, which is a 104 times improvement compared to the current best energy constraint. This would determine the nuclear isomeric energy to a sufficient accuracy to allow for nuclear laser spectroscopy of individual thorium ions in a Paul trap and thus the development of a single-ion nuclear optical clock.

Electronic level structure of Th+ in the range of the 229mTh isomer energy

David-Marcel Meier, Johannes Thielking, Przemysław Głowacki, Maksim V. Okhapkin, Robert A. Müller, Andrey Surzhykov, Ekkehard Peik


Using resonant two-step laser excitation of trapped 232Th+ ions, we observe 166 previously unknown energy levels of even parity within the energy range from 7.8 to 9.8 eV and angular momenta from J=1/2 to 7/2. We also classify the high-lying levels observed in our earlier experiments by the total angular momentum and perform ab-initio calculations to compare their results with the observed level density. The observed levels can be relevant for the excitation or decay of the 229mTh isomeric nuclear state which lies in this energy range. The high density of electronic levels promises a strongly enhanced electronic bridge excitation of the isomer in 229Th+.

All-solid-state VUV frequency comb at 160 nm using high-harmonic generation in nonlinear femtosecond enhancement cavity

J. Seres, E. Seres, C. Serrat, E. C. Young, J. S. Speck, T. Schumm


We realized a solid-state-based vacuum ultraviolet frequency comb by harmonics generation in an external enhancement cavity. Optical conversions were so far reported by only using gaseous media. We present a theory that allows the most suited solid generation medium to be selected for specific target harmonics by adapting the material’s bandgap. We experimentally use a thin AlN film grown on a sapphire substrate to realize a compact frequency comb high-harmonic source in the Deep Ultraviolet (DUV) / Vacuum Ultraviolet (VUV) spectral range. By extending our earlier VUV source [Opt. Express 26, 21900 (2018)] with the enhancement cavity, a sub-Watt level Ti:sapphire femtosecond frequency comb is enhanced to 24 W stored average power, its 3rd, 5th, and 7th harmonics are generated, and the targeted 5th harmonic’s power at 160 nm increased by two orders of magnitude. The emerging nonlinear effects in the solid medium, together with suitable intra-cavity dispersion management, support optimal enhancement and stable locking. To demonstrate the realized frequency comb’s spectroscopic ability, we report on the beat measurement between the 3rd harmonic beam and a 266 nm CW laser reaching about 1 MHz accuracy.

X-ray pumping of the Th-229 nuclear clock isomer

Takahiko Masuda, Akihiro Yoshimi, Akira Fujieda, Hiroyuki Fujimoto, Hiromitsu Haba, Hideaki Hara, Takahiro Hiraki, Hiroyuki Kaino, Yoshitaka Kasamatsu, Shinji Kitao, Kenji Konashi, Yuki Miyamoto, Koichi Okai, Sho Okubo, Noboru Sasao, Makoto Seto, Thorsten Schumm, Yudai Shigekawa, Kenta Suzuki, Simon Stellmer, Kenji Tamasaku, Satoshi Uetake, Makoto Watanabe, Tsukasa Watanabe, Yuki Yasuda, Atsushi Yamaguchi, Yoshitaka Yoda, Takuya Yokokita, Motohiko Yoshimura, Koji Yoshimura


Thorium-229 is a unique case in nuclear physics: it presents a metastable first excited state Th-229m, just a few electronvolts above the nuclear ground state. This so-called isomer is accessible by VUV lasers, which allows transferring the amazing precision of atomic laser spectroscopy to nuclear physics. Being able to manipulate the Th-229 nuclear states at will opens up a multitude of prospects, from studies of the fundamental interactions in physics to applications as a compact and robust nuclear clock. However, direct optical excitation of the isomer or its radiative decay back to the ground state has not yet been observed, and a series of key nuclear structure parameters such as the exact energies and half-lives of the low-lying nuclear levels of Th-229 are yet unknown. Here we present the first active optical pumping into Th-229m. Our scheme employs narrow-band 29 keV synchrotron radiation to resonantly excite the second excited state, which then predominantly decays into the isomer. We determine the resonance energy with 0.07 eV accuracy, measure a half-life of 82.2 ps, an excitation linewidth of 1.70 neV, and extract the branching ratio of the second excited state into the ground and isomeric state respectively. These measurements allow us to re-evaluate gamma spectroscopy data that have been collected over 40 years.

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.

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