All-optical subcycle microscopy on atomic length scales

T. Siday, J. Hayes, F. Schiegl, F. Sandner, P. Menden, V. Bergbauer, M. Zizlsperger, S. Nerreter, S. Lingl, J. Repp, J. Wilhelm (), M. A. Huber (), Y. A. Gerasimenko () and R. Huber
Additional contact information
T. Siday: University of Regensburg
J. Hayes: University of Regensburg
F. Schiegl: University of Regensburg
F. Sandner: University of Regensburg
P. Menden: University of Regensburg
V. Bergbauer: University of Regensburg
M. Zizlsperger: University of Regensburg
S. Nerreter: University of Regensburg
S. Lingl: University of Regensburg
J. Repp: University of Regensburg
J. Wilhelm: University of Regensburg
M. A. Huber: University of Regensburg
Y. A. Gerasimenko: University of Regensburg
R. Huber: University of Regensburg

Nature, 2024, vol. 629, issue 8011, 329-334

Abstract: Abstract Bringing optical microscopy to the shortest possible length and time scales has been a long-sought goal, connecting nanoscopic elementary dynamics with the macroscopic functionalities of condensed matter. Super-resolution microscopy has circumvented the far-field diffraction limit by harnessing optical nonlinearities1. By exploiting linear interaction with tip-confined evanescent light fields2, near-field microscopy3,4 has reached even higher resolution, prompting a vibrant research field by exploring the nanocosm in motion5–19. Yet the finite radius of the nanometre-sized tip apex has prevented access to atomic resolution20. Here we leverage extreme atomic nonlinearities within tip-confined evanescent fields to push all-optical microscopy to picometric spatial and femtosecond temporal resolution. On these scales, we discover an unprecedented and efficient non-classical near-field response, in phase with the vector potential of light and strictly confined to atomic dimensions. This ultrafast signal is characterized by an optical phase delay of approximately π/2 and facilitates direct monitoring of tunnelling dynamics. We showcase the power of our optical concept by imaging nanometre-sized defects hidden to atomic force microscopy and by subcycle sampling of current transients on a semiconducting van der Waals material. Our results facilitate access to quantum light–matter interaction and electronic dynamics at ultimately short spatio-temporal scales in both conductive and insulating quantum materials.

Date: 2024
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DOI: 10.1038/s41586-024-07355-7

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