Electron dynamics in water are of fundamental importance for a broad range of phenomena [1-3], but their real-time study faces numerous conceptual and methodological challenges [4][5][6]. Here, we introduce attosecond size-resolved cluster spectroscopy and build up a molecular-level understanding of the attosecond electron dynamics in water. We measure the effect that the addition of single water molecules has on the photoionization time delays [7][8][9][10][11] of water clusters. We find a continuous increase of the delay for clusters containing up to 4-5 molecules and little change towards larger clusters. We show that these delays are proportional to the spatial extension of the created electron hole, which first increases with cluster size and then partially localizes through the onset of structural disorder that is characteristic of large clusters and bulk liquid water. These results establish a previously unknown sensitivity of photoionization delays to electron-hole delocalization and reveal a direct link between electronic structure and attosecond photoemission dynamics. Our results offer novel perspectives for studying electron/hole delocalization and its attosecond dynamics.Electronic dynamics in water play a central role in a broad range of scientific and technological research areas ranging from radiation chemistry to photocatalysis. The dynamics induced by ionization of water are of particular relevance since they initiate the processes underlying radiation damage [2,3,12]. The ionization of water is predicted to lead to the formation of a delocalized electron hole, followed by its localization on one water molecule and proton transfer to a neighboring molecule, forming H 3 O + and OH [13]. The latter step has been time-resolved only very recently using one-photon extreme-ultraviolet (XUV) photoionization of water clusters [4] 1
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