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引用次数: 0
摘要
超快电子衍射(UED)仪器通常以千赫或更低的重复率运行,并依赖于电子的间接探测。然而,由于这些实验需要使用含有相对大量电子(≫100 个电子/脉冲)的电子束,因此会产生严重的空间电荷效应,从而使实验受到限制。因此,需要使用持续时间长、横向直径大的电子脉冲来检测样品。在这里,我们介绍了一种新型 UED 仪器,它以高重复率运行,并采用直接电子探测技术。通过使用每个脉冲包含 1-140 个电子、频率为 30 kHz 的电子束,我们的操作大大低于严重的空间电荷机制。我们展示了从薄膜固体样品中探测时间分辨信号的能力,其差分对比信号Δ I / I 0和仪器响应函数分别低至10-5和184-fs(FWHM),且无时间压缩。总之,我们的研究结果强调了提高 UED 实验重复率和采用直接电子探测方案的重要性,这对气相 UED 尤为重要。我们新开发的方案能够利用超短电子束更高效、更灵敏地研究光激发样品中的超快动力学。
High-repetition-rate ultrafast electron diffraction with direct electron detection.
Ultrafast electron diffraction (UED) instruments typically operate at kHz or lower repetition rates and rely on indirect detection of electrons. However, these experiments encounter limitations because they are required to use electron beams containing a relatively large number of electrons (≫100 electrons/pulse), leading to severe space-charge effects. Consequently, electron pulses with long durations and large transverse diameters are used to interrogate the sample. Here, we introduce a novel UED instrument operating at a high repetition rate and employing direct electron detection. We operate significantly below the severe space-charge regime by using electron beams containing 1-140 electrons per pulse at 30 kHz. We demonstrate the ability to detect time-resolved signals from thin film solid samples with a difference contrast signal, , and an instrument response function as low as 10-5 and 184-fs (FWHM), respectively, without temporal compression. Overall, our findings underscore the importance of increasing the repetition rate of UED experiments and adopting a direct electron detection scheme, which will be particularly impactful for gas-phase UED. Our newly developed scheme enables more efficient and sensitive investigations of ultrafast dynamics in photoexcited samples using ultrashort electron beams.
Structural Dynamics-UsCHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
CiteScore
5.50
自引率
3.60%
发文量
24
审稿时长
16 weeks
期刊介绍:
Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods.
The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as:
Time-resolved X-ray and electron diffraction and scattering,
Coherent diffractive imaging,
Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.),
Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy,
Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.),
Multidimensional spectroscopies in the infrared, the visible and the ultraviolet,
Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains,
Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals.
These new methods are enabled by new instrumentation, such as:
X-ray free electron lasers, which provide flux, coherence, and time resolution,
New sources of ultrashort electron pulses,
New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources,
New sources of ultrashort infrared and terahertz (THz) radiation,
New detectors for X-rays and electrons,
New sample handling and delivery schemes,
New computational capabilities.