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Precision spectroscopy of few-electron atoms and molecules

       量子电动力学(QED)作为原子分子精密谱的理论基础, 为理解微观物理世界提供了坚实的框架. 少电子原子分子体系由于其相对简单的电子结构, 成为高精度计算与测量的理想对象, 是检验束缚态QED理论的独特平台. 随着冷原子物理和激光技术的迅猛发展, 原子分子光谱的精密测量也不断取得突破. 精度的提升使得能级的位移揭示出越来越多的物理效应, 为检验QED理论、测量基本物理常数、揭示原子核结构以及探索新物理开辟了重要的科学路径. 可以说, 历经一个多世纪的发展, 少电子原子分子精密谱研究仍然在推动着物理学的前沿进展. 

       当前, 少电子原子分子精密谱面临着诸多挑战和未解难题. 例如: 质子半径之谜依然困扰着科学界——不同实验、不同方法得到的μ氢及氢原子体系质子半径存在一定偏差; 从同位素位移导出的氘核的电荷半径在不同谱线中的结果存在明显差异. 此外, 氦原子2S—2P态跃迁频率的测量在不同实验组之间存在显著偏差, 且在2S—3D和2P—3D跃迁中, 理论与实验结果间也有不小的分歧. 锂原子及其离子的精密光谱研究也揭示出锂–6的核电磁半径与核物理定出的结果之间有相当的偏离. 少体束缚态QED理论中, 能级展开为精细结构常数的幂级数, 目前实验精度已敏感的第七阶修正的理论数据来源十分有限, 第八阶修正仍然不完善. 这些问题表明, 少电子原子分子精密谱的研究不仅充满挑战, 更充满着解决新问题的希望. 

       本专题汇聚了活跃在少电子原子分子精密谱研究前沿的中青年科学家, 展示这一领域的最新研究进展和未来发展趋势. 通过结合各自的研究工作, 从不同视角为读者呈现该领域的前沿进展, 旨在促进学术交流并激发新的研究思路. 专题内容涵盖多个重要议题, 包括: 氢分子离子超精细结构的理论研究; 原子兰姆位移与超精细结构中核结构效应的探讨; 锂离子精密光谱与核结构信息的挖掘; 少电子原子在极紫外波段的精密光谱测量; 基于协同冷却技术的HD+振转光谱精密测量; 高电荷态类硼离子$^{ {\mathrm{2}}} {\mathrm{P}}_{ {\mathrm{3/2}}} {\mathrm{—}}^{ {\mathrm{2}}} {\mathrm{P}}_{ {\mathrm{1/2}}} $跃迁的实验与理论研究进展; 自由电子激光在氦原子高强度亚稳态的制备中的前景展望; 以及基于潘宁离子阱的少电子离子g因子的精密测量. 

     我们希望本专题不仅能为相关领域的研究者提供有价值的参考, 也能吸引更多的学者, 特别是青年科学家, 加入到少电子原子分子精密谱的研究中来, 为我国在该领域的蓬勃发展注入新鲜活力.

客座编辑:高克林 中国科学院精密测量科学与技术创新研究院
Acta Physica Sinica. 2024, 73(20).
Nuclear structure effects to atomic Lamb shift and hyperfine splitting
Ji Chen
2024, 73 (20): 202101. doi: 10.7498/aps.73.20241063
Abstract +
The development of precision atomic spectroscopy experiments and theoretical advancements plays a crucial role in measuring fundamental physical constants and testing quantum electrodynamics (QED) theories. It also provides a significant platform for studying the internal structure of atomic nuclei and developing high-precision nuclear structure theories. Nuclear structure effects such as charge distribution, magnetic moment distribution, and nuclear polarizability have been accurately determined in many atomic spectroscopy experiments, significantly enhancing the precision of nuclear structure detection.This paper systematically reviews the theoretical research and developments on the corrections of two-photon exchange (TPE) effects on the Lamb shift and hyperfine structure (HFS) in light ordinary and muonic atoms. Advanced nuclear force models and ab initio methods are employed to analyze the TPE nuclear structure corrections to the Lamb shift in a series of light muonic atoms. The paper compares the calculation of TPE effects from various nuclear models and evaluates the model dependencies and theoretical uncertainties of TPE effect predictions.Furthermore, the paper discusses the significant impact of TPE theory on explaining the discrepancies between experimental measurements and QED theoretical predictions in atomic hyperfine structures, resolving the accuracy difficulties in traditional theories. Detailed analyses of TPE effects on HFS in electronic and muonic deuterium using pionless effective field theory show good agreement with experimental measurements, validating the accuracy of theoretical predictions.The theoretical studies of TPE effects in light atoms are instrumental for determining nuclear charge radii and Zemach radii from spectroscopy measurements. These results not only enhance the understanding of nuclear structure and nuclear interactions but also offer crucial theoretical guidance for future experiments, thereby advancing the understanding of the proton radius puzzle and related studies.
Precise measurements of electron g factors in bound states of few-electron ions
Tu Bing-Sheng
2024, 73 (20): 203103. doi: 10.7498/aps.73.20240683
Abstract +
The electron g factor is an important fundamental structural parameter in atomic physics, as it reveals various mechanisms of interactions between electrons and external fields. Precise measurements of g factors of bound electrons in simple atomic and molecular systems provide an effective method for investigating the bound-state quantum electrodynamics (QED) theory. Especially in highly-charged heavy ions (HCIs), the strong electromagnetic interactions between the nuclei and inner-shell electrons provide unique opportunities to test QED under extremely strong fields. Accurate measurements of the g factors of the bound-state electrons are also important for determining nuclear effects, nuclear parameters and fundamental constants. The research on g factors of the bound-state electrons has become a frontier topic in fundamental physics. A Penning trap, which uses steady-state electromagnetic fields to confine charged particles, is utilized to precisely measure the g factor. This paper presents a comprehensive review of the experiments on g factors for few-electron simple systems in Penning traps, including experimental principles, experimental setups, measurement methods, and a summary of important research findings. The physical concept of the electron g factor and its historical research background are introduced. The electron g factor is considered as an effective probe to study higher-order QED effects. Through high-precision measurements of the free electron g factor, discrepancies between the fine-structure constants and other experimental results in atomic physics are identified. Notably, the g factor of the 1s electron in HCIs deviates significantly from the value for free electrons as the atomic number increases. Experimental principles, including the principle of the Penning trap and the principle of measuring the bound-state electron g factors are discussed. A double-trap experiment setup and related precision measurement techniques are also introduced.This paper reviews several milestone experiments including (1) the stringent test of bound-state QED by precise measurement of bound-state electron g factor of a 118Sn49+ ion, (2) measurement of the g factors of lithium-like and boron-like ions and their applications, and (3) measurement of the g-factor isotope shift by using an advanced two-ion balance technique in the Penning trap, providing an insight into the QED effects in nuclear recoil. Finally, this paper summarizes the challenges currently faced in measuring the g factors of bound-state electrons in few-electron ion systems and provides the prospects for the future developments of this field.
Precision measurement based on rovibrational spectrum of cold molecular hydrogen ion
Zhang Qian-Yu, Bai Wen-Li, Ao Zhi-Yuan, Ding Yan-Hao, Peng Wen-Cui, He Sheng-Guo, Tong Xin
2024, 73 (20): 203301. doi: 10.7498/aps.73.20241064
Abstract +
A molecular hydrogen ion HD+, composed of a proton, a deuteron, and an electron, has a rich set of rovibrational transitions that can be theoretically calculated and experimentally measured precisely. Currently, the relative accuracy of the rovibrational transition frequencies of the HD+ molecular ions has reached 10–12. By comparing experimental measurements with theoretical calculations of the HD+ rovibrational spectrum, the precise determination of the proton-electron mass ratio, the testing of quantum electrodynamics(QED) theory, and the exploration of new physics beyond the standard model can be achieved. The experiment on HD+ rovibrational spectrum has achieved the highest accuracy (20 ppt, 1 ppt = 10–12) in measuring proton-electron mass ratio. This ppaper comprehensively introduces the research status of HD+ rovibrational spectroscopy, and details the experimental method of the high-precision rovibrational spectroscopic measurement based on the sympathetic cooling of HD+ ions by laser-cooled Be+ ions. In Section 2, the technologies of generating and trapping both Be+ ions and HD+ ions are introduced. Three methods of generating ions, including electron impact, laser ablation and photoionization, are also compared. In Section 3, we show the successful control of the kinetic energy of HD+ molecular ions through the sympathetic cooling, and the importance of laser frequency stabilization for sympathetic cooling of HD+ molecular ions. In Section 4, two methods of preparing internal states of HD+ molecular ions, optical pumping and resonance enhanced threshold photoionization, are introduced. Both methods show the significant increase of population in the ground rovibrational state. In Section 5, we introduce two methods of determining the change in the number of HD+ molecular ions, i.e. secular excitation and molecular dynamic simulation. Both methods combined with resonance enhanced multiphoton dissociation can detect the rovibrational transitions of HD+ molecular ions. In Section 6, the experimental setup and process for the rovibrational spectrum of HD+ molecular ions are given and the up-to-date results are shown. Finally, this paper summarizes the techniques used in HD+ rovibrational spectroscopic measurements, and presents the prospects of potential spectroscopic technologies for further improving frequency measurement precision and developing the spectroscopic methods of different isotopic hydrogen molecular ions.
Review of the hyperfine structure theory of hydrogen molecular ions
Zhong Zhen-Xiang
2024, 73 (20): 203104. doi: 10.7498/aps.73.20241101
Abstract +
The study of high-precision spectroscopy for hydrogen molecular ions enables the determination of fundamental constants, such as the proton-to-electron mass ratio, the deuteron-to-electron mass ratio, the Rydberg constant, and the charge radii of proton and deuteron. This can be accomplished through a combination of high precision experimental measurements and theoretical calculations. The spectroscopy of hydrogen molecular ions reveals abundant hyperfine splittings, necessitating not only an understanding of rovibrational transition frequencies but also a thorough grasp of hyperfine structure theory to extract meaningful physical information from the spectra. This article reviews the history of experiments and theories related to the spectroscopy of hydrogen molecular ions, with a particular focus on the theory of hyperfine structure. As far back as the second half of the last century, the hyperfine structure of hydrogen molecular ions was described by a comprehensive theory based on its leading-order term, known as the Breit-Pauli Hamiltonian. Thanks to the advancements in non-relativistic quantum electrodynamics (NRQED) at the beginning of this century, a systematic development of next-to-leading-order theory for hyperfine structure has been achieved and applied to $\text{H}_2^+$ and $\text{HD}^+$ in recent years, including the establishment of the $m\alpha^7\ln(\alpha)$ order correction. For the hyperfine structure of $\text{H}_2^+$, theoretical calculations show good agreement with experimental measurements after decades of work. However, for HD+, discrepancies have been observed between measurements and theoretical predictions that cannot be accounted for by the theoretical uncertainty in the non-logarithmic term of the $m\alpha^7$ order correction. To address this issue, additional experimental measurements are needed for mutual validation, as well as independent tests of the theory, particularly regarding the non-logarithmic term of the $m\alpha^7$ order correction.
Precision spectroscopic measurements of few-electron atomic systems in extreme ultraviolet region
Xiao Zheng-Rong, Zhang Heng-Zhi, Hua Lin-Qiang, Tang Li-Yan, Liu Xiao-Jun
2024, 73 (20): 204205. doi: 10.7498/aps.73.20241231
Abstract +
Precision spectroscopic measurements on the few-electron atomic systems have attracted much attention because they shed light on important topics such as the “proton radius puzzle” and testing quantum electrodynamics (QED). However, many important transitions of few-electron atomic systems are located in the vacuum/extreme ultraviolet region. Lack of a suitable narrow linewidth light source is one of the main reasons that hinder the further improvement of the spectral resolution.Recently, narrow linewidth extreme ultraviolet (XUV) light sources based on high harmonic processes in rare gases have opened up new opportunities for precision measurements of these transitions. The recently implemented XUV comb has a shortest wavelength of about 12 nm, a maximum power of milliwatts, and a linewidth of about 0.3 MHz, making it an ideal tool for precision measurements in the XUV band. At the same time, the Ramsey comb in the XUV band can achieve a spectral resolution of the kHz range, and may operate throughout the entire XUV band.With these useful tools, direct frequency spectroscopy and Ramsey comb spectroscopy in the XUV region are developed, and precision spectroscopic measurements of few-electron atomic systems with these methods are becoming a hot topic in cutting-edge science. In this paper, we provide an overview of the current status and the progress of relevant researches, both experimentally and theoretically, and discuss the opportunities for relevant important transitions in the extreme ultraviolet band.
Experimental and theoretical research progress of 2P1/2 2P3/2 transitions of highly charged boron-like ions
Liu Xin, Wen Wei-Qiang, Li Ji-Guang, Wei Bao-Ren, Xiao Jun
2024, 73 (20): 203102. doi: 10.7498/aps.73.20241190
Abstract +
The precise measurement of the fine structure and radiative transition properties of highly charged ions (HCI) is essential for testing fundamental physical models, including strong-field quantum electrodynamics (QED) effects, electron correlation effects, relativistic effects, and nuclear effects. These measurements also provide critical atomic physics parameters for astrophysics and fusion plasma physics. Compared with the extensively studied hydrogen-like and lithium-like ion systems, boron-like ions exhibit significant contributions in terms of relativistic and QED effects in their fine structure forbidden transitions. High-precision experimental measurements and theoretical calculations of these systems provide important avenues for further testing fundamental physical models in multi-electron systems. Additionally, boron-like ions are considered promising candidates for HCI optical clocks. This paper presents the latest advancements in experimental and theoretical research on the ground state 2P3/22P1/2 transition in boron-like ions, and summarizes the current understanding of their fine and hyperfine structures. It also discusses a proposed experimental setup for measuring the hyperfine splitting of boron-like ions by using an electron beam ion trap combined with high-resolution spectroscopy. This proposal aims to provide a reference for future experimental research on the hyperfine splitting of boron-like ions, to test the QED effects with higher precision, extract the radius of nuclear magnetization distribution, and validate relevant nuclear structure models.
Precision spectroscopy and nuclear structure information of Li+ ions
Guan Hua, Qi Xiao-Qiu, Chen Shao-Long, Shi Ting-Yun, Gao Ke-Lin
2024, 73 (20): 204203. doi: 10.7498/aps.73.20241128
Abstract +
Precision spectroscopy of lithium ions offers a unique research platform for exploring bound state quantum electrodynamics and investigating the structure of atomic nuclei. This paper overviews our recent efforts dedicated to the precision theoretical calculations and experimental measurements of the hyperfine splittings of 6,7Li+ ions in the $\,^3{\rm{S}}_1$ and $\,^3{\rm{P}}_J$ states. In our theoretical research, we utilize bound state quantum electrodynamics to calculate the hyperfine splitting of the $\,^3{\rm{S}}_1$ and $\,^3{\rm{P}}_J$ states with remarkable precision, achieving an accuracy on the order of $m\alpha^6$. Using Hylleraas basis sets, we first solve the non-relativistic Hamiltonian of the three-body system to derive high-precision energy and wave functions. Subsequently, we consider various orders of relativity and quantum electrodynamics corrections by using the perturbation method, with accuracy of the calculated hyperfine splitting reaching tens of kHz. In our experimental efforts, we developed a low-energy metastable lithium-ion source that provides a stable and continuous ion beam in the $\,^3{\rm{S}}_1$ state. Using this ion beam, we utilize the saturated fluorescence spectroscopy to enhance the precision of hyperfine structure splittings of 7Li+ in the $\,^3{\rm{S}}_1$ and $\,^3{\rm{P}}_J$ states to about 100 kHz. Furthermore, by utilizing the optical Ramsey method, we obtain the most precise values of the hyperfine splittings of 6Li+, with the smallest uncertainty of about 10 kHz. By combining theoretical calculations and experimental measurements, our team have derived the Zemach radii of the 6,7Li nuclei, revealing a significant discrepancy between the Zemach radius of 6Li and the values predicted by the nuclear model. These findings elucidate the distinctive properties of the 6Li nucleus, promote further investigations of atomic nuclei, and advance the precise spectroscopy of few-electron atoms and molecules.
Free electron laser prepared high-intensity metastable helium and helium-like ions
Du Xiao-Jiao, Wei Long, Sun Yu, Hu Shui-Ming
2024, 73 (15): 150201. doi: 10.7498/aps.73.20240554
Abstract +
In the precision spectroscopy of few-electron atoms, the generation of high-intensity metastable helium atoms and helium-like ions is crucial for implementing experimental studies as well as a critical factor for improving the signal-to-noise ratio of experimental measurements. With the rapid development of free-electron laser (FEL) and technology, FEL wavelengths extend from hard X-rays to soft X-rays and even vacuum ultraviolet bands. Meanwhile, laser pulses with ultra-fast, ultra-intense and high repetition frequencies are realized, thus making it possible for FEL to prepare single-quantum state atoms/ions with high efficiency. In this work, we propose an experimental method for obtaining high-intensity single-quantum state helium atoms and helium-like ions by using FEL. The preparation efficiency can be calculated by solving the master equation of light-atom interaction. Considering the experimental parameters involved in this work, we predict that the efficiencies of preparing metastable 23S He, Li+ and Be2+ are about 3%, 6% and 2%, respectively. Compared with the common preparation methods such as gas discharge and electron bombardment, a state-of-the-art laser excitation method can not only increase the preparation efficiency, but also reduce the effects of high-energy stray particles such as electrons, ions, and photons generated during discharge. Furthermore, combined with the laser preparation technique, the sophisticated ion confinement technique, which can ensure a long interaction time between the ions and laser, increases the efficiency of metastable Li+ and Be2+ by several orders of magnitude. Therefore, the preparation of high-intensity metastable helium and helium-like ions can improve the measurement accuracy of precision spectroscopy of atoms and ions. A new experimental method, based on FEL, to study the fine structure energy levels 23P of helium, has the potential to obtain the results with an accuracy exceeding the sub-kHz level. Thus, the high-precision fine structure constants can be determined with the development of high-order quantum electrodynamics theory. In order to measure energy levels with higher accuracy, a new detection technique, which can reduce or even avoid more systematic effects, must be developed. For example, the quantum interference effect, which has been proposed in recent years, seriously affects the accuracy of fine-structure energy levels. If the interference phenomenon of spontaneous radiation between different excited states can be avoided in the detection process, the measurement accuracy will not be affected by this quantum interference effect. High-intensity metastable atoms or ions in chemical reaction dynamics studies also have better chances to investigate reaction mechanisms. In summary, the FEL preparation of high-intensity metastable helium atoms and helium-like ions proposed in this work will lay an important foundation for developing cold atom physics and chemical reaction dynamics.
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