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arXiv:1210.3611 · Physical Review Letters

Coherence-Enhanced Optical Determination of the Th229 Isomeric Transition

Wen-Te Liao, Sumanta Das, Christoph H. Keitel, Adriana Pálffy

Published Dec 28, 2012• 34 citations
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Abstract

The impact of coherent light propagation on the excitation and fluorescence of thorium nuclei in a crystal lattice environment is investigated theoretically. We find that in the forward direction, the fluorescence signal exhibits characteristic intensity modulations dominated by a sped-up initial decay signal that is orders of magnitude faster. This feature can be exploited for the optical determination of the isomeric transition energy. In order to obtain a unmistakable signature of the isomeric nuclear fluorescence, we put forward a novel scheme for the direct measurement of the transition energy via electromagnetically modified nuclear forward scattering involving two fields that couple to three nuclear states.

DOI
10.1103/physrevlett.109.262502

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Quantum interference effects in an ensemble of 229 Th nuclei interacting with coherent light

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As a unique feature, the ${}^{229}$Th nucleus has an isomeric transition in the vacuum ultraviolet that can be accessed by optical lasers. The interference effects occurring in the interaction between coherent optical light and an ensemble of ${}^{229}$Th nuclei are investigated theoretically. We consider the scenario of nuclei doped in vacuum ultraviolet transparent crystals and take into account the effect of different doping sites and therefore different lattice fields that broaden the nuclear transition width. This effect is shown to come into interplay with interference effects due to the hyperfine splitting of the ground and isomeric nuclear states. We investigate possible experimentally available situations involving two-, three- and four-level schemes of quadrupole sublevels of the ground and isomeric nuclear states coupling to one or two coherent fields. Specific configurations which offer clear signatures of the isomer excitation advantageous for the more precise experimental determination of the transition energy are identified. Furthermore, it is shown that population trapping into the isomeric state can be achieved. This paves the way for further nuclear quantum optics applications with ${}^{229}$Th such as nuclear coherent control.

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We present a comprehensive theoretical investigation of hyperfine-resolved excitation and detection of the low-energy isomeric state of $^{229}$Th in trapped $^{229}\mathrm{Th}^{3+}$ ions. Using a quantum master equation approach, we quantitatively analyze the dependence of the isomeric population on laser linewidth, detuning, and irradiation time, showing that their proper matching is essential for efficient excitation. Going beyond earlier conceptual discussions of electronic-fluorescence-based nuclear-state detection, we propose two concrete nuclear-state detection schemes based on three hyperfine-resolved electronic fluorescence channels at 690, 984, and 1088 nm. Our quantitative analysis shows that, for 50 ions, the 690- and 984-nm scheme yields detectable photon count rates on the order of $10^3~\mathrm{s}^{-1}$ at 690 nm and $10^4~\mathrm{s}^{-1}$ at 984 nm, whereas the 1088-nm scheme achieves a detectable photon rate on the order of $10^3~\mathrm{s}^{-1}$. By quantifying the trade-off between irradiation time and scan-step size, we show that the nuclear transition can be located within one month for a 100-MHz uncertainty using currently available vacuum-ultraviolet laser technology. These results provide practical guidance for trapped-ion $^{229}\mathrm{Th}$ spectroscopy and the development of nuclear clocks.

physics.atom-phCross-listedarXiv:2604.27614•May 1, 2026
The impact of coherent light propagation on the excitation and fluorescence of thorium nuclei in a crystal lattice environment is investigated theoretically. We find that in the forward direction, the fluorescence signal exhibits characteristic intensity modulations dominated by a sped-up initial decay signal that is orders of magnitude faster. This feature can be exploited for the optical determination of the isomeric transition energy. In order to obtain a unmistakable signature of the isomeric nuclear fluorescence, we put forward a novel scheme for the direct measurement of the transition energy via electromagnetically modified nuclear forward scattering involving two fields that couple to three nuclear states.
As a unique feature, the 229{}^{229}229Th nucleus has an isomeric transition in the vacuum ultraviolet that can be accessed by optical lasers. The interference effects occurring in the interaction between coherent optical light and an ensemble of 229{}^{229}229Th nuclei are investigated theoretically. We consider the scenario of nuclei doped in vacuum ultraviolet transparent crystals and take into account the effect of different doping sites and therefore different lattice fields that broaden the nuclear transition width. This effect is shown to come into interplay with interference effects due to the hyperfine splitting of the ground and isomeric nuclear states. We investigate possible experimentally available situations involving two-, three- and four-level schemes of quadrupole sublevels of the ground and isomeric nuclear states coupling to one or two coherent fields. Specific configurations which offer clear signatures of the isomer excitation advantageous for the more precise experimental determination of the transition energy are identified. Furthermore, it is shown that population trapping into the isomeric state can be achieved. This paves the way for further nuclear quantum optics applications with 229{}^{229}229Th such as nuclear coherent control.
A possibility of the two-photon excitation of an isomeric state in a nucleus of thorium-229 has been discussed. The fluorescence intensity of the excitation is demonstrated to be identical for the irradiation of nuclei with either monochromatic light or polychromatic radiation consisting of a sequence of short lightpulses of the same intensity. The two-photon excitation of Th3+ ion in an electromagnetic trap with a focused laser beam with a wavelength of about 320 nm and power of 100 mW can lead to the absorption saturation, at which the fluorescence emission with the frequency of the transition in a nucleus is maximal. In crystals doped with Th4+ to a concentration of about 1018 cm-3 and irradiated with a laser radiation 10 W in power, the emission of several photons persecond with a wavelength of about 160 nm becomes possible.
A low-energy nuclear transition in the isotope thorium-229 has been excited in thorium-doped crystals with laser light. This opens the perspective towards a highly stable and robust solid-state optical nuclear clock. The required laser radiation at 148 nm wavelength has so far been produced using pulsed laser systems where only a small fraction of the incident photons has been resonant with the narrow nuclear transition. Here we show that the nuclear resonance can be excited with a continuous-wave narrow-bandwidth laser source with a power of less than 1 nW, and that the resonance signal can be detected in absorption rather than in fluorescence. This eliminates the slow nuclear fluorescence decay from the detection process and offers a considerable advantage for clock operation through fast signal acquisition. The VUV laser source is based on three sequential frequency doublings, starting from a diode laser at 1187 nm that is well suited for linewidth narrowing and for frequency comparisons with optical atomic clocks. We use absorption spectroscopy for the quantitative characterization of two different Th-centers in calcium fluoride crystal and measure the isomeric shift between them. One of the centers shows a very small static electric crystal field gradient 0.1 V/A˚2Å^2A˚2, to be compared to gradients in the range of 100 V/A˚2Å^2A˚2 observed earlier. This indicates a center with high symmetry of the ions surrounding the Th nucleus, promising nuclear resonance lines that are nearly independent of the lattice spacing.
The laser-accessible nuclear transition in the thorium-229 isotope has been identified as a promising candidate for the realization of an optical nuclear clock. Such a nuclear clock might rival or outperform current optical clocks based on electron-shell transitions in atoms or ions, is expected to be more robust against external perturbations, and provides enhanced sensitivity in clock-based tests of fundamental principles of physics. Here, we implement a thorium-229 nuclear clock by stabilizing a continuous-wave laser to the 148 nm nuclear transition with rapid feedback based on continuous absorption spectroscopy. The thorium-229 nuclei are embedded into a millimeter-sized, room temperature calcium fluoride crystal. A subharmonic of the 148 nm radiation is continuously compared to a Yb+ single-ion clock. The nuclear clock shows a simple shot-noise limited scaling of the fractional frequency instability of 3⋅10−12τ/s3\cdot 10^{-12} \sqrt{τ/\text{s}}3⋅10−12τ/s​ where τττ is the averaging time, approaching 10−1510^{-15}10−15 instabilities over 1 day of continuous operation. Improvements of the instability by several orders of magnitude can be projected for future solid-state nuclear clocks. We use the nuclear clock to constrain models of ultralight dark matter by searching for periodic fluctuations and slow drifts in the nuclear transition energy, on time scales between 20 s and 1 day. Drawing benefit from the enhanced sensitivity of the thorium-229 transition, these constraints compete with the best atomic clocks concerning dark matter coupling to photons and go beyond previous measurements regarding coupling to the strong force and quarks.
Vacuum-ultraviolet-transparent crystals have been proposed as host lattice for the coherent driving of the unusually low-lying isomer excitation in 229Th^{229}\mathrm{Th}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.
Hyperfine-resolved laser excitation and detection of nuclear isomer in trapped 229^{229}229Th3+^{3+}3+ ions
We present a comprehensive theoretical investigation of hyperfine-resolved excitation and detection of the low-energy isomeric state of 229^{229}229Th in trapped 229Th3+^{229}\mathrm{Th}^{3+}229Th3+ ions. Using a quantum master equation approach, we quantitatively analyze the dependence of the isomeric population on laser linewidth, detuning, and irradiation time, showing that their proper matching is essential for efficient excitation. Going beyond earlier conceptual discussions of electronic-fluorescence-based nuclear-state detection, we propose two concrete nuclear-state detection schemes based on three hyperfine-resolved electronic fluorescence channels at 690, 984, and 1088 nm. Our quantitative analysis shows that, for 50 ions, the 690- and 984-nm scheme yields detectable photon count rates on the order of 103 s−110^3~\mathrm{s}^{-1}103 s−1 at 690 nm and 104 s−110^4~\mathrm{s}^{-1}104 s−1 at 984 nm, whereas the 1088-nm scheme achieves a detectable photon rate on the order of 103 s−110^3~\mathrm{s}^{-1}103 s−1. By quantifying the trade-off between irradiation time and scan-step size, we show that the nuclear transition can be located within one month for a 100-MHz uncertainty using currently available vacuum-ultraviolet laser technology. These results provide practical guidance for trapped-ion 229Th^{229}\mathrm{Th}229Th spectroscopy and the development of nuclear clocks.