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自由电子激光（Free Electron Laser, FEL）凭借高相干性、高亮度、覆盖远红外至X射线波段的连续可调性，在科学研究、材料科学、生物医学、环境监测等众多领域有着广泛的应用前景。特别是X射线自由电子激光（X-ray Free-Electron Laser, XFEL）以其独特的超高亮度、超短脉冲、极好相干性，强力地推动了超快X射线散射和超快光谱学领域的发展。基于XFEL的超快散射技术不仅实现了对晶格动力学、电荷和自旋序的超快时间和动量分辨研究，还能够测量大动量转移范围的声子色散。将基于XFEL的超快散射与光谱学手段相结合，有望同时测量元激发能态变化及其相关的原子或序结构变化。基于XFEL的光谱学正尝试充分利用自放大自发辐射模式（Self Amplified Spontaneous Emission，SASE）的全带宽，以减少脉冲延展，最终实现时间和能量分辨接近傅里叶变换极限的光谱测量。基于XFEL的非线性光学技术为探测元激发开辟了新途径，正在发展的新方法有望为探索表面和界面过程、手性、纳米尺度传输提供独特的机会，并实现多维度芯能级光谱学。In 2005, the FLASH soft X-ray free-electron laser (FEL) in Hamburg, Germany, achieved its first lasing, marking the beginning of an intensive phase of global FEL construction. Subsequently, the United States, Japan, South Korea, China, Italy, and Switzerland have all commenced building this type of photon facility. Recently, the new generation of FEL has started to utilize superconducting acceleration technology to achieve high-repetition-rate pulse output, thereby improving experimental efficiency. Currently completed facilities include the European XFEL, with ongoing constructions of the LCLS-II in the United States and the SHINE facility in Shanghai. The Shenzhen Superconducting soft X-ray Free-electron Laser (S3FEL) is also in preparation.
These FEL facilities generate coherent and tunable ultrashort pulses across the extreme ultraviolet to hard X-ray spectrum, advancing FEL-based scattering techniques such as ultrafast X-ray scattering, spectroscopy, and X-ray nonlinear optics, thereby transforming the way we study correlated quantum materials at ultrafast timescales.
The Self-Amplified Spontaneous Emission (SASE) process in FEL leads to timing jitter between FEL pulses and the synchronized pump laser, impacting the accuracy of ultrafast time-resolved measurements. To address this issue, timing tools have been developed to measure these jitters and reindex each pump-probe signal after measurement. This success enables ultrafast X-ray diffraction (UXRD) to be first realized, a systematic study of Peierls distorted materials is demonstrated. Furthermore, the high flux of FEL pulses enable Fourier Transform Inelastic X-ray Scattering (FT-IXS) method, which allows the extraction the phonon dispersion curves throughout the entire Brillouin zone by applying the Fourier transform to the measured momentum dependent coherent phonon scattering signals, even when the system is in a non-equilibrium state.
UXRD is typically employed to study ultrafast lattice dynamics, which requires hard X-ray wavelengths. In contrast, time resolved resonant elastic X-ray scattering (tr-REXS) in the soft X-ray regime has become a standard method for investigating nano-sized charge and spin orders in correlated quantum materials at ultrafast time scales.
In correlated quantum materials, the interplay between electron and lattice dynamics represents another important research direction. In addition to Zhi-Xun Shen's successful demonstration of the combined tr-ARPES and UXRD method at SLAC, this paper also reports attempts to integrate UXRD with Resonant X-ray Emission Spectroscopy (RXES) for the simultaneous measurement of electronic and lattice dynamics.
Resonant Inelastic X-ray Scattering (RIXS) is a powerful tool for studying elementary and collective excitations in correlated quantum materials. However, in FEL-based soft X-ray spectroscopy, the wavefront tilt introduced by the widely used grating monochromators inevitably stretches the FEL pulses, which degrades the time resolution. Therefore, the new design at FEL beamlines employs low line density gratings with long exit arms to reduce pulse stretch and achieve relatively high energy resolution. For example, the Heisenberg-RIXS instrument at the European XFEL achieves an energy resolution of 92 meV at the Cu L3 edge and approximately 150 fs time resolution.
In recent years, scientists at SwissFEL's Furka station have drawn inspiration from femtosecond optical covariance spectroscopy to propose a new method for generating two-dimensional time-resolved Resonant Inelastic X-ray Scattering (2D tr-RIXS) spectra. This method involves real-time detection of single-shot FEL incident and scattered spectra, followed by deconvolution calculation to avoid photon waste and wavefront tilt caused by monochromator slits. The SQS experimental station at European XFEL, in 2023, features a 1D-XUV spectrometer that utilizes subtle variations in photon energy absorption across the sample to induce spatial energy dispersion. Using Wolter mirrors, it directly images spatially resolved fluorescence emission from the sample onto the detector to generate 2D tr-RIXS spectra without the need for deconvolution. However, this design is limited to specific samples. Currently, the S3FEL is designing a novel 2D tr-RIXS instrument that uses an upstream low line density grating monochromator to generate spatial dispersion of the beam spot, allowing the full bandwidth of SASE to project spatially dispersed photon energy onto the sample. Subsequently, a similar optical design to the 1D-XUV spectrometer will be employed to achieve two-dimensional tr-RIXS spectra, thereby expanding the applicability beyond specific liquid samples. These new instruments are designed to minimize pulse elongation by fully utilizing SASE's full bandwidth, approaching Fourier-transform-limited RIXS spectra in both time and energy resolution.
Nonlinear X-ray optics techniques such as sum-frequency generation (SFG) and second-harmonic generation are being adapted for X-ray wavelengths, opening new avenues for probing elementary excitations. X-ray transient grating spectroscopy extends capabilities to study charge transport and spin dynamics on ultrafast timescales. The future developing of these scattering methods offer unique opportunities for probing dynamical events in a wide variety of systems, including surface and interface processes, chirality, nanoscale transport and the termed as multidimensional core-level spectroscopy.-
Keywords:
- Free Electron Laser /
- Ultrafast X-ray Scattering /
- Ultrafast X-ray Spectroscopy /
- X-ray Nonlinear Optics
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