arXiv subjects

Peter G. Thirolf

Publications and source records attributed to Peter G. Thirolf.

At least 19 recordsLinked to original sources

arXiv2025

A cryogenic Paul trap for probing the nuclear isomeric excited state $^{229\text{m}}$Th$^{3+}$

While laser excitation of the nuclear isomeric transition in $^{229}$Th has been recently achieved for thorium atoms embedded in large-bandgap crystals, laser excitation and characterization of the nuclear transition in trapped $^{229}$Th$^{3+}$ ions has not yet been accomplished. To address these experiments, a cryogenic Paul trap setup has been designed, built, and commissioned at LMU Munich. Here, we present the specifications of the new experimental platform and demonstrate its successful operation, showing the extraction, subsequent ion-guiding, mass-purification, and trapping of $^{229}$Th$^{3+}$ and $^{229\text{m}}$Th$^{3+}$ ions from a newly designed buffer-gas stopping cell as well as of $^{88}$Sr$^{+}$ ions from laser ablation of a solid target. Further, we show sympathetic laser cooling of $^{229\text{(m)}}$Th$^{3+}$ by Doppler-cooled $^{88}$Sr$^{+}$ ions and the formation of mixed-species Coulomb crystals.

physics.atom-ph↗

arXiv2025

$^{229}$Th Nuclear Spectroscopy in an Opaque Material: Laser-Based Conversion Electron Mössbauer Spectroscopy of $^{229}$ThO$_2$

Here, we report the first demonstration of laser-induced conversion electron Mössbauer spectroscopy of the $^{229}$Th nuclear isomeric state, which provides the ability to probe the nuclear transition in a material that is opaque to light resonant with the nuclear transition. Specifically, we excite the nuclear transition in a thin ThO$_2$ sample whose band gap ($\sim$ 6 eV) is considerably smaller than the nuclear isomeric state energy (8.4 eV). As a result, the excited nucleus can quickly decay by internal conversion, resulting in the ejection of electrons from the surface. By collecting these conversion electrons, nuclear spectroscopy can be recorded. Unlike fluorescence spectroscopy, this technique is compatible with materials whose work function is less than the nuclear transition energy, opening a wider class of systems to study. Further, because ThO$_2$ can be made from spinless isotopes and the internal conversion decay process reduces the isomeric state lifetime to only $\sim$10 $μ$s, allowing $\sim$10$^8$ relative reduction in clock interrogation time, a conversion-electron-based nuclear clock could lead to a $\sim$10$^4$ reduction in clock instability.

physics.atom-ph↗

arXiv2025

First image-guided treatment of a mouse tumor with radioactive ion beams

Radioactive ion beams (RIB) are a key focus of current research in nuclear physics. Already long ago it was proposed that they could have applications in cancer therapy. In fact, while charged particle therapy is potentially the most effective radiotherapy technique available, it is highly susceptible to uncertainties in the beam range. RIB are well-suited for image-guided particle therapy, as isotopes that undergo \b{eta}+-decay can be precisely visualized using positron emission tomography (PET), enabling accurate real-time monitoring of the beam range. We successfully treated a mouse osteosarcoma using a radioactive 11C-ion beam. The tumor was located in the neck, in close proximity to the spinal cord, increasing the risk of radiation-induced myelopathy from even slight variations in the beam range caused by anatomical changes or incorrect calibration of the planning CT. We managed to completely control the tumor with the highest dose while minimizing toxicity. Low-grade neurological side effects were correlated to the positron activity measured in the spine. The biological washout of the activity from the tumor volume was dependent on the dose, indicating a potential component of vascular damage at high doses. This experiment marks the first instance of tumor treatment using RIB and paves the way for future clinical applications.

physics.med-ph↗

arXiv2024

Frequency ratio of the $^{229\mathrm{m}}$Th nuclear isomeric transition and the $^{87}$Sr atomic clock

Optical atomic clocks$^{1,2}$ use electronic energy levels to precisely keep track of time. A clock based on nuclear energy levels promises a next-generation platform for precision metrology and fundamental physics studies. Thorium-229 nuclei exhibit a uniquely low energy nuclear transition within reach of state-of-the-art vacuum ultraviolet (VUV) laser light sources and have therefore been proposed for construction of the first nuclear clock$^{3,4}$. However, quantum state-resolved spectroscopy of the $^{229m}$Th isomer to determine the underlying nuclear structure and establish a direct frequency connection with existing atomic clocks has yet to be performed. Here, we use a VUV frequency comb to directly excite the narrow $^{229}$Th nuclear clock transition in a solid-state CaF$_2$ host material and determine the absolute transition frequency. We stabilize the fundamental frequency comb to the JILA $^{87}$Sr clock$^2$ and coherently upconvert the fundamental to its 7th harmonic in the VUV range using a femtosecond enhancement cavity. This VUV comb establishes a frequency link between nuclear and electronic energy levels and allows us to directly measure the frequency ratio of the $^{229}$Th nuclear clock transition and the $^{87}$Sr atomic clock. We also precisely measure the nuclear quadrupole splittings and extract intrinsic properties of the isomer. These results mark the start of nuclear-based solid-state optical clock and demonstrate the first comparison of nuclear and atomic clocks for fundamental physics studies. This work represents a confluence of precision metrology, ultrafast strong field physics, nuclear physics, and fundamental physics.

physics.atom-ph↗

arXiv2023

Excitation and probing of low-energy nuclear states at high-energy storage rings

$^{229}$Th with a low-lying nuclear isomeric state is an essential candidate for a nuclear clock as well as many other applications. Laser excitation of the isomeric state has been a long-standing goal. With relativistic $^{229}$Th ions in storage rings, high-power lasers with wavelengths in the visible range or longer can be used to achieve high excitation rates of $^{229}$Th isomers. This can be realized through direct resonant excitation, or excitation via an intermediate nuclear or electronic state, facilitated by the tunability of both the laser-beam and ion-bunch parameters. Unique opportunities are offered by highly charged $^{229}$Th ions due to the nuclear-state mixing. The significantly reduced isomeric-state lifetime corresponds to a much higher excitation rate for direct resonant excitation. Importantly, we propose electric dipole transitions changing both the electronic and nuclear states that are opened by the nuclear hyperfine mixing. We suggest using them for efficient isomer excitation in Li-like $^{229}$Th ions, via stimulated Raman adiabatic passage or single-laser excitation. We also propose schemes for probing the isomers, utilizing nuclear radiative decay or laser spectroscopy on electronic transitions, through which the isomeric-state energy can be determined with an orders-of-magnitude higher precision than the current value. The schemes proposed here for $^{229}$Th could also be adapted to low-energy nuclear states in other nuclei, such as $^{229}$Pa.

nucl-ex↗

arXiv2022

Observation of the radiative decay of the ${}^{229}\mathrm{Th}$ nuclear clock isomer

The nucleus of the radioisotope thorium-229 (${}^{229}$Th) features an isomer with an exceptionally low excitation energy that enables direct laser manipulation of nuclear states. For this reason, it is a leading candidate for use in next-generation optical clocks. This nuclear clock will be a unique tool, amongst others, for tests of fundamental physics. While first indirect experimental evidence for the existence of such an extraordinary nuclear state is significantly older, the proof of existence has been delivered only recently by observing the isomer's electron conversion decay and its hyperfine structure in a laser spectroscopy study, revealing information on the isomer's excitation energy, nuclear spin and electromagnetic moments. Further studies reported the electron conversion lifetime and refined the isomer's energy. In spite of recent progress, the isomer's radiative decay, a key ingredient for the development of a nuclear clock, remained unobserved. In this Letter, we report the detection of the radiative decay of this low-energy isomer in thorium-229 (${}^{229\mathrm{m}}$Th). By performing vacuum-ultraviolet spectroscopy of ${}^{229\mathrm{m}}$Th incorporated into large-bandgap CaF${}_2$ and MgF${}_2$ crystals at the ISOLDE facility at CERN, the photon vacuum wavelength of the isomer's decay is measured as 148.71(42) nm, corresponding to an excitation energy of 8.338(24) eV. This value is in agreement with recent measurements, and decreases the uncertainty by a factor of seven. The half-life of ${}^{229\mathrm{m}}$Th embedded in MgF${}_2$ is determined to be 670(102) s. The observation of the radiative decay in a large-bandgap crystal has important consequences for the design of a future nuclear clock and the improved uncertainty of the energy eases the search for direct laser excitation of the atomic nucleus.

nucl-ex↗

arXiv2021

Expanding Nuclear Physics Horizons with the Gamma Factory

The Gamma Factory (GF) is an ambitious proposal, currently explored within the CERN Physics Beyond Colliders program, for a source of photons with energies up to $\approx 400\,$MeV and photon fluxes (up to $\approx 10^{17}$ photons per second) exceeding those of the currently available gamma sources by orders of magnitude. The high-energy (secondary) photons are produced via resonant scattering of the primary laser photons by highly relativistic partially-stripped ions circulating in the accelerator. The secondary photons are emitted in a narrow cone and the energy of the beam can be monochromatized, eventually down to the $\approx1$ ppm level, via collimation, at the expense of the photon flux. This paper surveys the new opportunities that may be afforded by the GF in nuclear physics and related fields.

nucl-ex↗

arXiv2020

The theory of direct laser excitation of nuclear transitions

A comprehensive theoretical study of direct laser excitation of a nuclear state based on the density matrix formalism is presented. The nuclear clock isomer $^{229\text{m}}$Th is discussed in detail, as it could allow for direct laser excitation using existing technology and provides the motivation for this work. The optical Bloch equations are derived for the simplest case of a pure nuclear two-level system and for the more complex cases taking into account the presence of magnetic sub-states, hyperfine-structure and Zeeman splitting in external fields. Nuclear level splitting for free atoms and ions as well as for nuclei in a solid-state environment is discussed individually. Based on the obtained equations, nuclear population transfer in the low-saturation limit is reviewed. Further, nuclear Rabi oscillations, power broadening and nuclear two-photon excitation are considered. Finally, the theory is applied to the special cases of $^{229\text{m}}$Th and $^{235\text{m}}$U, being the nuclear excited states of lowest known excitation energies. The paper aims to be a didactic review with many calculations given explicitly.

nucl-th↗

arXiv2020

Electronic bridge excitation in highly charged Th-229 ions

The excitation of the 8 eV $^{229m}$Th isomer through the electronic bridge mechanism in highly charged ions is investigated theoretically. By exploiting the rich level scheme of open $4f$ orbitals and the robustness of highly charged ions against photoionization, a pulsed high-intensity optical laser can be used to efficiently drive the nuclear transition by coupling it to the electronic shell. We show how to implement a promising electronic bridge scheme in an electron beam ion trap starting from a metastable electronic state. This setup would avoid the need for a tunable vacuum ultraviolet laser. Based on our theoretical predictions, determining the isomer energy with an uncertainty of $10^{-5}$ eV could be achieved in one day of measurement time using realistic laser parameters.

physics.atom-ph↗

arXiv2019

Energy of the $^{229}$Th nuclear clock transition

The first nuclear excited state of $^{229}$Th offers the unique opportunity for laser-based optical control of a nucleus. Its exceptional properties allow for the development of a nuclear optical clock which offers a complementary technology and is expected to outperform current electronic-shell based atomic clocks. The development of a nuclear clock was so far impeded by an imprecise knowledge of the energy of the $^{229}$Th nuclear excited state. In this letter we report a direct excitation energy measurement of this elusive state and constrain this to 8.28$\pm$0.17 eV. The energy is determined by spectroscopy of the internal conversion electrons emitted in-flight during the decay of the excited nucleus in neutral $^{229}$Th atoms. The nuclear excitation energy is measured via the valence electronic shell, thereby merging the fields of nuclear- and atomic physics to advance precision metrology. The transition energy between ground and excited state corresponds to a wavelength of 149.7$\pm$3.1 nm. These findings set the starting point for high-resolution nuclear laser spectroscopy and thus the development of a nuclear optical clock of unprecedented accuracy. A nuclear clock is expected to have a large variety of applications, ranging from relativistic geodesy over dark matter research to the observation of potential temporal variation of fundamental constants.

nucl-ex↗

arXiv2019

The concept of laser-based conversion electron Mössbauer spectroscopy for a precise energy determination of $^{229m}$Th

$^{229}$Th 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 $^{229}$Th 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 $μ$eV resolution, corresponding to 10 GHz, which is a $10^4$ 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.

nucl-ex↗

arXiv2018

Towards a precise determination of the excitation energy of the Thorium nuclear isomer using a magnetic bottle spectrometer

$^{229}$Th is the only known nucleus with an excited state that offers the possibility for a direct laser excitation using existing laser technology. Its excitation energy has been measured indirectly to be 7.8(5) eV ($\approx$160 nm). The energy and lifetime of the isomeric state make it the presently only suitable candidate for a nuclear optical clock, the uncertainty of the excitation energy is, however, still too large to allow for a direct laser excitation in a Paul trap. Therefore, a major goal during the past years has been an improved energy determination. One possible approach is to measure the kinetic energy of electrons which are emitted in the internal conversion decay of the first isomeric state in $^{229}$Th. For this reason an electron spectrometer based on a magnetic bottle combined with electrical retarding fields has been built. Its design, as well as first test measurements are presented, which reveal a relative energy resolution of 3 % and thus enable to measure the electrons' expected kinetic energy to better than 0.1 eV. This is sufficiently precise to specify a laser system able to drive the nuclear clock transition in $^{229}$Th.

physics.ins-det↗

arXiv2018

Towards a 229Th-based nuclear clock

An overview over the current status of the development of a nuclear clock based on the state of lowest known nuclear excitation energy in $^{229}$Th 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 over 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 $^{229}$Th are discussed.

nucl-ex↗

arXiv2018

Laser spectroscopic characterization of the nuclear clock isomer $^{229m}$Th

The isotope $^{229}$Th is the only nucleus known to possess an excited state $^{229m}$Th in the energy range of a few electron volts, a transition energy typical for electrons in the valence shell of atoms, but about four orders of magnitude lower than common nuclear excitation energies. A number of applications of this unique nuclear system, which is accessible by optical methods, have been proposed. Most promising among them appears a highly precise nuclear clock that outperforms existing atomic timekeepers. Here we present the laser spectroscopic investigation of the hyperfine structure of $^{229m}$Th$^{2+}$, yielding values of fundamental nuclear properties, namely the magnetic dipole and electric quadrupole moments as well as the nuclear charge radius. After the recent direct detection of this long-searched-for isomer, our results now provide detailed insight into its nuclear structure and present a method for its non-destructive optical detection.

nucl-ex↗

arXiv2018

Lifetime measurement of the $^{229}$Th nuclear isomer

The first excited isomeric state of $^{229}$Th possesses the lowest energy among all known excited nuclear states. The expected energy is accessible with today's laser technology and in principle allows for a direct optical laser excitation of the nucleus. The isomer decays via three channels to its ground-state (internal conversion, $γ$ decay and bound internal conversion), whose strengths depend on the charge state of $^{229m}$Th. We report on the measurement of the internal-conversion decay half-life of neutral $^{229m}$Th. A half-life of 7 $\pm$ 1 $μ$s has been measured, which is in the range of theoretical predictions and, based on the theoretically expected lifetime of $\approx10^4$ s of the photonic decay channel, gives further support for an internal conversion coefficient of $\approx10^9$, thus constraining the strength of a radiative branch in the presence of IC.

nucl-ex↗

arXiv2017

Direct detection of the 229Th nuclear clock transition

Today's most precise time and frequency measurements are performed with optical atomic clocks. However, it has been proposed that they could potentially be outperformed by a nuclear clock, which employs a nuclear transition instead of the atomic shell transitions used so far. By today there is only one nuclear state known which could serve for a nuclear clock using currently available technology, which is the isomeric first excited state in $^{229}$Th. Here we report the direct detection of this nuclear state, which is a further confirmation of the isomer's existence and lays the foundation for precise studies of the isomer's decay parameters. Based on this direct detection the isomeric energy is constrained to lie between 6.3 and 18.3 eV, and the half-life is found to be longer than 60 s for $^{229\mathrm{m}}$Th$^{2+}$. More precise determinations appear in reach and will pave the way for the development of a nuclear frequency standard.

nucl-ex↗

arXiv2017

The extraction of 229Th3+ from a buffer-gas stopping cell

In the whole landscape of atomic nuclei, $^{229}$Th is currently the only known nucleus which could allow for the development of a nuclear-based frequency standard, as it possesses an isomeric state of just 7.6 eV energy above the ground state. The 3+ charge state is of special importance in this context, as Th$^{3+}$ allows for a simple laser-cooling scheme. Here we emphasize the direct extraction of triply-charged $^{229}$Th from a buffer-gas stopping cell. This finding will not only simplify any future approach of $^{229}$Th ion cooling, but is also used for thorium-beam purification and in this way provides a powerful tool for the direct identification of the $^{229}$Th isomer to ground state nuclear transition.

physics.ins-det↗

arXiv2017

A laser excitation scheme for $^{229\text{m}}$Th

Direct laser excitation of the lowest known nuclear excited state in $^{229}$Th has been a longstanding 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 $(7.8\pm 0.5)$ eV. Here we present a direct laser excitation scheme for $^{229\text{m}}$Th, 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 $10^4$ and a total measurement time of less than three days for laser scanning appear to be achievable.

nucl-ex↗