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随着X射线光源品质的提升, X射线波段的量子调控成为了新兴的前沿领域, 基于薄膜平面腔的X射线腔量子光学是其中一个重要分支. X射线腔量子光学研究始于原子核跃迁体系, 近期兴起了调控原子内壳层跃迁的研究工作. 原子内壳层跃迁存在丰富的候选体系和退激通道, 极大地拓宽了X射线腔量子光学的研究范围. 此外, 内壳层激发及其退激通道对应着多种X射线谱学表征技术, 促进X射线腔量子光学和谱学技术的融合, 有望促成X射线谱学新技术的出现. 本文概述了基于原子内壳层跃迁的X射线腔量子光学, 介绍了基本的实验体系和实验方法、经典和量子理论模型以及已经实现的一些量子光学现象. 最后, 本文简要介绍了内壳层X射线腔量子光学仍需要解决的一些问题, 同时展望了未来的发展方向.
Over the past decade, X-ray quantum optics has emerged as a dynamic research field, driven by significant advancements in X-ray sources such as next-generation synchrotron radiation facilities and X-ray free-electron lasers, as well as improvements in X-ray methodologies and sample fabrication techniques. One of the most successful platforms in this field is the X-ray planar thin-film cavity, also known as the X-ray cavity QED setup. To date, most studies in X-ray cavity quantum optics have focused on Mössbauer nuclear resonances. However, this approach is constrained by the limited availability of suitable nuclear isotopes and the lack of universal applicability. Recently, experimental realizations of X-ray cavity quantum control in atomic inner-shell transitions have demonstrated that cavity effects can simultaneously modify transition energies and core-hole lifetimes. These pioneering studies suggest that X-ray cavity quantum optics based on inner-shell transitions will become a promising new platform. Notably, the core-hole state is a fundamental concept in various modern X-ray spectroscopic techniques. Therefore, integrating X-ray quantum optics with X-ray spectroscopy holds the potential to open new frontiers in the field of core-level spectroscopy. In this review, we introduce the experimental systems used in X-ray cavity quantum optics with inner-shell transitions, covering cavity structures, sample fabrications, and experimental methodologies. We explain that X-ray thin-film cavity experiments require high flux, high energy resolution, minimal beam divergence, and precise angular control, necessitating the use of synchrotron radiations. Grazing reflectivity and fluorescence measurements are described in detail, along with a brief introduction to resonant inelastic X-ray scattering techniques. The review also outlines simulation tools, including the classical Parratt algorithm, semi-classical matrix formalism, quantum optical theory based on the Jaynes-Cummings model, and the quantum Green’s function method. We discuss the similarities and unique features of electronic inner-shell transitions and highlight recent advancements, focusing on cavity-induced phenomena such as collective Lamb shift, Fano interference, core-hole lifetime control, etc. Observables such as reflectivity and fluorescence spectra play a central role in these studies. Finally, we review and discuss potential future directions for the field. Designing novel cavities is crucial for addressing current debates regarding cavity effects in inner-shell transitions and uncovering new quantum optical phenomena. Integrating modern X-ray spectroscopies with X-ray cavity quantum optics represents a promising research frontier with significant application potential. Furthermore, X-ray free-electron lasers, with much higher pulse intensity and shorter pulse duration, are expected to propel X-ray cavity quantum optics into the nonlinear and multiphoton regimes, opening new avenues for exploration. -
Keywords:
- X-ray quantum optics /
- X-ray planar thin-film cavity /
- synchrotron radiation /
- inner-shell transition
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图 4 Parratt迭代方法示意图. 其中$ n_i $为第i层介质对X射线的折射率, $ d_i $为第i层介质的厚度, $ r_{i-1,i} $和$ t_{i-1,i} $为X射线在介质($i-1 $)与i界面处的反射和透射系数
Fig. 4. Illustration of Parratt’s method. $ n_i $ and $ d_i $ are the refractive indices and thickness of the$ i\text{-}\mathrm{th} $ layer, $ r_{i-1,i} $ and $ t_{i-1,i} $ are the Fresnel coefficients for reflection and transmission at the interface between $ (i-1) $ and $ i\text{-}\mathrm{th} $ layers.
图 7 (a)结构Pt(2.0 nm)/C(18.0 nm)/WSi2(2.0 nm)/C(18.0 nm)/Pt(16.0 nm)/Si100(infinitely thick)的薄膜平面腔的X射线反射率曲线; (b)不同角度下腔内场强随着z方向深度的分布, 其中白色实线描绘了不同膜层的边界
Fig. 7. (a) Rocking curve of the cavity with the structure of Pt(2.0 nm)/C(18.0 nm)/WSi2(2.0 nm)/C(18.0 nm)/Pt(16.0 nm)/Si100(infinitely thick); (b) the field intensity distribution inside the cavity. The white solid lines dipict the boundaries of different layers.
图 12 实验测量与理论模拟的X射线反射二维谱 (a)实验测量结果; (b)实验数据扣除吸收边; (c)理论模拟结果; (d)理论模拟扣除吸收边
Fig. 12. X-ray reflection two-dimensional spectrum of experimental measurements and theoretical simulations: (a) Experimental reflectivity map; (b) experimental data by exclusion of the absorption edge; (c) simulated reflectivity map; (d) simulated map by exclusion of the absorption edge.
图 13 3种腔结构下实验测量的模式角度下的反射谱及拟合曲线, 其中数据点和红色虚线分别为实验测量结果与拟合结果, 绿色实线为实验数据去除拟合的吸收边得到的法诺线形, 数据引自文献[61]
Fig. 13. Measured reflectivity spectra at the first mode angle. The dots are experimental data, and the dashed lines are the fit to data according to the theoretical model. The solid lines present the Fano profiles in the reflectivity spectra by subtracting the fitted edge components from the experimental data. The squares of $ \mathrm{Im}(q) $ for each data set are also presented. Data are quoted from Ref. [61].
图 17 (a)一阶、(b)三阶、(c)五阶模式角以及(d)远离腔模式角度下的荧光谱及拟合曲线, 远离腔模式时, 洛伦兹响应的线宽为原子本身的线宽3.6 eV, 而在模式角度下, 辐射速率受到腔效应增强, 线宽显著增大, 数据引自[60]
Fig. 17. Selected fluorescence spectra at the (a) 1st, (b) 3rd, (c) 5th mode angles, and (d) offset angle far from the mode angles. The experimental spectra are fitted by the theoretical model, and the widths of the Lorentzian response are presented. Note that the response features as the natural linewidth of the atomic transition at off-resonant angles while the width is strongly altered by the cavity effect at mode angles. Data are quoted from Ref. [60].
图 18 远场下不同出射角度的Co Kα荧光辐射强度, 在第1阶和第3阶腔模式角度下观测到了明显的荧光强度增强. 黑色实线为基于互易定理的模拟结果, 蓝色点线是使用X射线激发空穴态, 红色点线是使用电子束激发空穴态, 数据引自[58]
Fig. 18. Far-field fluorescence intensities at different emission angles. The directional emission is observed at the first and third cavity modes. The blue and red dotted lines are experimental data resulted from X-ray excitation and electron beam excitation, respectively. The solid black line is the simulation based on the reciprocity theorem. Data are digitized from [58].
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