In a recent paper published in Phys. Rev. Lett. 133, 152503 (2024), H. Zhang, T. Li, and X. Wang predicted that modern intense lasers can induce highly nonlinear responses in the 229Th nucleus for the first time, which is an astonishing effect of light-nucleus interactions. This phenomenon is underpinned by two key factors: (1) the presence of a very low-lying nuclear excited state and (2) a nuclear hyperfine mixing effect that significantly enhances light-nucleus coupling. The resulting highly nonlinear responses facilitate efficient nuclear excitation and enable coherent light emission from the nucleus, resulting in high harmonic generation. 229Th presents a promising platform for advancements in both laser-nuclear physics and nuclear clock development. The pioneering work by Zhang et al. marks a new frontier in light-matter interactions.
Lasers with intensities exceeding 1013 W/cm2 can induce highly nonlinear responses in atoms and molecules, resulting in novel phenomena, such as multiphoton and above-threshold ionization [1, 2], nonsequential double ionization [3-5], high harmonic generation [6, 7], and laser-induced electron diffraction [8-10]. A particularly significant outcome of intense laser-atom interactions is the generation of attosecond (1 as = 10-18 s) pulses [11, 12], which is a breakthrough that achieved the 2023 Nobel Prize.
The ability to induce highly nonlinear responses in atoms arises when the laser-atom interaction energy EI becomes a non-negligible fraction of the atomic transition energy ΔE. The former is the product of the atomic transition moment D and laser field amplitude
The induction of highly nonlinear responses in atomic nuclei presents a significant challenge. First, a nucleus is approximately five orders of magnitude smaller than an atom, resulting in correspondingly smaller transition moment values D. Second, the nuclear transition energy ΔE is typically five orders of magnitude greater than that of atoms. Consequently, to achieve a similar η value for nuclei, the laser field amplitude
However, this estimation applies to “typical” nuclei, whereas Nature provides certain exceptional cases. One such nucleus is thorium-229 (229Th), which features an extremely low-lying excited state just 8.4 eV above the nuclear ground state. The minimized transition energy of the 229Th nucleus is
The second key element is the nuclear hyperfine mixing (NHM) effect. An inner-orbital electron generates a strong electromagnetic field at the nucleus site, causing mixing between nuclear states. This effect has significant implications for the 229Th nucleus. The lifetime of the isomeric state for the bare nucleus is of the order of 103 s. In contrast, this lifetime significantly decreases by five orders of magnitude to 10-2 s for the hydrogenlike ionic state, where the 1s electron contributes to the NHM effect. This reduction occurs because the NHM effect enhances the coupling between the nucleus and light field, effectively modifying the transition moment from D to
As the transition moment increases to
Figure 1(a) illustrates the nuclear excitation probability as a function of laser intensity for both the bare nucleus (Th90+) and hydrogenlike ion (Th89+). In the case of Th89+, the nuclear excited state splits into two levels due to hyperfine splitting, and the excitation probabilities for both levels (with total angular momentum F=1 and 2) are displayed. For Th89+, the excitation probabilities deviate from linearity at intensities above 1017 W/cm2, exhibiting highly nonlinear characteristics and rapidly climbing to the 10% level at an intensity of 1021 W/cm2. In contrast, for the bare nucleus Th90+, the excitation probability remains linearly dependent on laser intensity all the way up to 1023 W/cm2, indicating that the response is still linear and fails to evoke nonlinear effects. Moreover, the absolute value of the excitation probability remains relatively small.
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With highly nonlinear responses triggered in Th89+, radiation is emitted at multiple frequencies, which are the high-order harmonics of the laser frequency, as illustrated in Fig. 1(b) for four different laser intensities. The third and fifth harmonics appear at intensity 1018 W/cm2. As the intensity increases, higher-order harmonics become evident, with the 31st harmonic observable at 1021 W/cm2.
The potential for inducing highly nonlinear responses in nuclei presents several important applications: (1) Efficient excitation and manipulation of nuclei — an excitation probability of 10% per nucleus per laser pulse is remarkable, paving the way for further quantum-state manipulation. (2) High harmonic generation as a novel mechanism for nucleus-based coherent light emission, which is distinct from the long-sought nuclear laser concept based on population inversion [15]. (3) High harmonic spectra as a new spectroscopic technique for extracting nuclear information — these spectra encode valuable nuclear data, such as the nuclear transition moment, which can be decoded through detailed analysis.
Beyond serving as a valuable platform for studying laser-nucleus interactions, the 229Th nucleus holds immense promise for the construction of nuclear clocks. A peculiar low-energy nuclear transition in 229Th has been proposed as the basis for nuclear clocks [16], offering distinct advantages over atomic clocks. Substantial progress has been made in recent years [17-24].
Here, I highlight the recent advancements in China: (1) Vacuum Ultraviolet (VUV) Light Sources: Our group in Wuhan has developed a VUV frequency comb that provides narrowband (< 30 MHz) VUV light centered at 148 nm [25]. Additionally, Xiao et al. at Tsinghua University proposed a VUV laser scheme based on four-wave mixing in cadmium vapor [26]. (2) Th-Doped Crystals: Gong et al. investigated various Th-doped wide-bandgap crystals as potential materials for building solid-state nuclear clocks [27, 28]. (3) 229Th Production: Ma et al. proposed generating 229Th through accelerated 232Th and neutron knocking-out reactions [29], while Wu et al. suggested using γ rays to remove three neutrons from 232Th [30]. (4) Isomeric Excitation Methods: A variety of theoretical methods for isomeric excitation have been explored, including laser-driven electron recollision [31], electron bridge mechanisms [32, 33], inelastic electron scattering [34], laser-cluster interactions [35], proton Coulomb excitation [36], and electron capture [37].
In conclusion, 229Th stands out as a promising platform for both laser-nuclear physics and nuclear clock development, with substantial advancements already achieved and further progress anticipated.
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