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<p>Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. These results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.</p>

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Nanoscale ultrafast lattice modulation with a free-electron laser

  • 期刊论文

  • 发表日期：

    2026年1月27日

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  • 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 R. 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

摘要

Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. These results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.