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arXiv 2506.03428physics.optics
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利用硬X射线自由电子激光实现纳米尺度超快晶格调制

Nanoscale Ultrafast Lattice Modulation with Hard X-ray Free Electron Laser

Haoyuan Li, Nan Wang, Leon Zhang, Sanghoon Song, Yanwen Sun, May-Ling Ng, Takahiro Sato, Dillon Hanlon, Sajal Dahal, Mario D. Balcazar, Vincent Esposito, Selene… 展开作者

Haoyuan Li, Nan Wang, Leon Zhang, Sanghoon Song, Yanwen Sun, May-Ling Ng, Takahiro Sato, Dillon Hanlon, Sajal Dahal, Mario D. Balcazar, Vincent Esposito, Selene She, Chance Caleb Ornelas-Skarin, Joan Vila-Comamala, Christian David, Nadia Berndt, Peter Richard Miedaner, Zhuquan Zhang, Matthias Ihme, Mariano Trigo, Keith A. Nelson, Jerome B. Hastings, Alexei A. Maznev, Laura Foglia, Samuel Teitelbaum, David A. Reis, Diling Zhu

AI总结:

本文利用硬X射线自由电子激光实现亚飞秒同步双脉冲,首次生成10 nm周期的X射线瞬态光栅,并在SrTiO3中观测到纳米尺度弹道热输运,为纳米动力学相干控制提供了新平台。

摘要:

在过去几十年中,对跨空间和时间尺度的微观动力学的理解与控制推动了科学和技术的重大进步。虽然基于超快激光的技术已经能够在飞秒和阿秒级别的本征时间尺度上探测纳米尺度动力学,但光学激光的长波长阻碍了以纳米尺度空间特异性对这些动力学进行询问和操控。随着硬X射线自由电子激光(FEL)的发展,在开发X射线瞬态光栅(XTG)光谱学方面取得了显著进展,旨在利用纳米尺度X射线驻波实现对基本激发的相干控制。迄今为止,XTG仅在光学波长下被探测,因此其可实现的周期性本质上被限制在数百纳米。通过实现两个硬X射线脉冲在受控交叉角下的亚飞秒同步,我们展示了空间周期为10 nm的XTG的产生。XTG激发驱动一个热光栅,该热光栅在立方钙钛矿SrTiO3(STO)中驱动相干的单色纵向声学声子。利用具有相同光子能量的第三个X射线脉冲,对XTG诱导的散射强度调制进行时间与动量分辨测量,为STO中纳米尺度的弹道热输运提供了证据。这些结果凸显了XTG在研究凝聚态物质中高波矢激发和纳米尺度输运方面的巨大潜力,并将XTG确立为对纳米尺度动力学进行相干控制与研究的强大平台。

英文摘要:

Understanding and controlling microscopic dynamics across spatial and temporal scales has driven major progress in science and technology over the past several decades. While ultrafast laser-based techniques have enabled probing nanoscale dynamics at their intrinsic temporal scales down to femto- and attoseconds, the long wavelengths of optical lasers have prevented the interrogation and manipulation of such dynamics with nanoscale spatial specificity. With advances in hard X-ray free electron lasers (FELs), significant progress has been made developing X-ray transient grating (XTG) spectroscopy, aiming at the coherent control of elementary excitations with nanoscale X-ray standing waves. So far, XTGs have been probed only at optical wavelengths, thus intrinsically limiting the achievable periodicities to several hundreds of nm. By achieving sub-femtosecond synchronization of two hard X-ray pulses at a controlled crossing angle, we demonstrate the generation of an XTG with spatial periods of 10 nm. The XTG excitation drives a thermal grating that drives coherent monochromatic longitudinal acoustic phonons in the cubic perovskite, SrTiO3 (STO). With a third X-ray pulse with the same photon energy, time-and-momentum resolved measurement of the XTG-induced scattering intensity modulation provides evidence of ballistic thermal transport at nanometer scale in STO. These results highlight the great potential of XTG for studying high-wave-vector excitations and nanoscale transport in condensed matter, and establish XTG as a powerful platform for the coherent control and study of nanoscale dynamics.

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