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

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) [1–4], significant progress has been made developing X-ray transient grating (XTG) spectroscopy[5, 6], aiming at the coherent control of elementary excitations with nanoscale X-ray standing waves. So far, XTGs have been probed only at optical wavelengths [5, 6], thus intrinsically limiting the achievable periodicities to several hundreds of nanometers. 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.