TY - JOUR AU - Chapman, Henry N. AU - Li, Chufeng AU - Bajt, Sasa AU - Butola, Mansi AU - Dresselhaus, Jan Lukas AU - Egorov, Dmitry AU - Fleckenstein, Holger AU - Ivanov, Nikolay AU - Kiene, Antonia AU - Klopprogge, Bjarne AU - Kremling, Viviane AU - Middendorf, Philipp AU - Oberthür, Dominik AU - Prasciolu, Mauro AU - Scheer, Theresa Emilie Sophie AU - Sprenger, Janina AU - Wong, Jia Chyi AU - Yefanov, Oleksandr AU - Zakharova, Margarita AU - Zhang, Wenhui TI - Convergent-beam attosecond x-ray crystallography JO - Structural dynamics VL - 12 IS - 1 SN - 2329-7778 CY - Melville, NY PB - AIP Publishing LLC M1 - PUBDB-2024-05957 SP - 014301 PY - 2025 AB - Sub-ångström spatial resolution of electron density coupled with sub-femtosecond temporal resolution is required to directly observe the dynamics of the electronic structure of a molecule after photoinitiation or some other ultrafast perturbation. Meeting this challenge, pushing the field of quantum crystallography to attosecond timescales, would bring insights into how the electronic and nuclear degrees of freedom couple, enable the study of quantum coherences involved in molecular dynamics, and ultimately enable these dynamics to be controlled. Here we propose to reach this realm by employing convergent-beam X-ray crystallography with high- power attosecond pulses from a hard-X-ray free-electron laser. We show that with dispersive optics, such as multilayer Laue lenses of high numerical aperture, it becomes possible to encode time into the resulting diffraction pattern with deep sub-femtosecond precision. Each snapshot diffraction pattern consists of Bragg streaks that can be mapped back to arrival times and positions of X-rays on the face of a crystal. This can span tens of femtoseconds, and can be finely sampled as we demonstrate experimentally. The approach brings several other advantages, such as an increase of the number of observable reflections in a snapshot diffraction pattern, all fully integrated, to improve the speed and accuracy of serial crystallography—especially for crystals of small molecules. LB - PUB:(DE-HGF)16 C6 - 39816474 UR - <Go to ISI:>//WOS:001396299100001 DO - DOI:10.1063/4.0000275 UR - https://bib-pubdb1.desy.de/record/614737 ER -