skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.
Attention:The NSF Public Access Repository (NSF-PAR) system and access will be unavailable from 7:00 AM ET to 7:30 AM ET on Friday, April 24 due to maintenance. We apologize for the inconvenience.


Title: Laser-based conversion electron Mössbauer spectroscopy of 229ThO2
Abstract The exceptionally low-energy229Th nuclear isomeric state is expected to provide several new and powerful applications1,2, including the construction of a robust and portable solid-state nuclear clock3, perhaps contributing to a redefinition of the second4, exploration of nuclear superradiance5,6and tests of fundamental physics7–10. Further, analogous to the capabilities of traditional Mössbauer spectroscopy, the sensitivity of the nucleus to its environment can be used to realize laser Mössbauer spectroscopy and, with it, new types of strain and temperature sensors3,11and a new probe of the solid-state environment12,13, all with excellent sensitivity. However, current models for examining the nuclear transition in a solid require the use of a high-bandgap, vacuum ultraviolet (VUV) transmissive host, severely limiting the applicability of these techniques. Here we report the first, to the authors’ knowledge, demonstration of laser-induced conversion electron Mössbauer spectroscopy (CEMS) of the229Th isomer in a thin ThO2sample whose bandgap (approximately 6 eV) is considerably smaller than the nuclear isomeric state energy (8.4 eV). Unlike fluorescence spectroscopy of the229Th isomeric transition, this technique is compatible with materials whose bandgap is less than the nuclear transition energy, opening a wider class of systems to study and the potential of a conversion-electron-based nuclear clock.  more » « less
Award ID(s):
2016245
PAR ID:
10678881
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Nature
Date Published:
Journal Name:
Nature
Volume:
648
Issue:
8093
ISSN:
0028-0836
Page Range / eLocation ID:
300 to 305
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. The population dynamics of the Th 229 isomeric state is studied in a solid-state host under laser illumination. A photoquenching process is observed, where off-resonant vacuum-ultraviolet (VUV) radiation leads to relaxation of the isomeric state. The cross-section for this photoquenching process is measured, and a model for the decay process, where photoexcitation of electronic states within the material band gap opens an internal conversion decay channel, is presented and appears to reproduce the measured cross-section. By engineering defects into Th 229 -doped solid-state hosts, this previously unrecognized photoquenching process may be used to reduce the clock transition readout time and thereby increase the stability of the nuclear clock. Published by the American Physical Society2025 
    more » « less
  2. Abstract Resonant oscillators with stable frequencies and large quality factors help us to keep track of time with high precision. Examples range from quartz crystal oscillators in wristwatches to atomic oscillators in atomic clocks, which are, at present, our most precise time measurement devices1. The search for more stable and convenient reference oscillators is continuing2–6. Nuclear oscillators are better than atomic oscillators because of their naturally higher quality factors and higher resilience against external perturbations7–9. One of the most promising cases is an ultra-narrow nuclear resonance transition in45Sc between the ground state and the 12.4-keV isomeric state with a long lifetime of 0.47 s (ref. 10). The scientific potential of45Sc was realized long ago, but applications require45Sc resonant excitation, which in turn requires accelerator-driven, high-brightness X-ray sources11that have become available only recently. Here we report on resonant X-ray excitation of the45Sc isomeric state by irradiation of Sc-metal foil with 12.4-keV photon pulses from a state-of-the-art X-ray free-electron laser and subsequent detection of nuclear decay products. Simultaneously, the transition energy was determined as$${\mathrm{12,389.59}}_{+0.12\left({\rm{syst}}\right)}^{\pm 0.15\left({\rm{stat}}\right)}\,{\rm{eV}}$$ 12,389.59 + 0.12 syst ± 0.15 stat eV with an uncertainty that is two orders of magnitude smaller than the previously known values. These advancements enable the application of this isomer in extreme metrology, nuclear clock technology, ultra-high-precision spectroscopy and similar applications. 
    more » « less
  3. Laser spectroscopy of the 229m Th nuclear clock transition is necessary for the future construction of a nuclear-based optical clock. Precision laser sources with broad spectral coverage in the vacuum ultraviolet are needed for this task. Here, we present a tunable vacuum-ultraviolet frequency comb based on cavity-enhanced seventh-harmonic generation. Its tunable spectrum covers the current uncertainty range of the 229m Th nuclear clock transition. 
    more » « less
  4. The recent laser excitation of the 229Th isomeric transition in a solid-state host opens the door for a portable solid-state nuclear optical clock. However, at present, the vacuum-ultraviolet laser systems required for clock operation are not conducive to a fieldable form factor. Here, we propose a possible solution to this problem by using 229Th-doped nonlinear optical crystals, which would allow clock operation without a vacuum-ultraviolet laser system and without the need of maintaining the crystal under vacuum. We investigate electronic properties and thorium doping in BaMgF4 and BaZnF4 with density functional theory, predicting BaMgF4 to be the superior material, and evaluate the performance of a Th:BaMgF4 clock. 
    more » « less
  5. Wide-bandgap semiconductors have unique electron emission properties by virtue of having high-lying conduction bands. Among these, diamond stands out because of its chemical stability, allowing it to serve as a solid-state electron source in vacuum and non-vacuum environments, including water. However, the underlying mechanisms of electron emission are not well understood. Here, we report investigations of the mechanisms of electron emission from H-terminated and oxidized surfaces of single-crystal boron-doped diamond(111) in vacuum and in water using both sub-bandgap (4.75 eV and 3.05 eV) and above-bandgap (21.2 eV) excitation. Energy-resolved photoemission spectra in vacuum using different incident photon energies reveal two distinct energy distributions, reflecting different emission pathways. While oxidation greatly reduces electron emission into vacuum using both sub-bandgap and above-bandgap sources, facile electron emission into water persists on the oxidized samples using sub-bandgap excitation and is directly observed through transient optical absorption measurements using sub-bandgap excitation. Low-energy inverse photoemission spectroscopy shows that oxidation leads to broad distribution of surface states throughout the diamond bandgap. Our studies highlight 
    more » « less