All-optical subcycle microscopy on atomic length scales
成果类型：
Article
署名作者：
Siday, T.; Hayes, J.; Schiegl, F.; Sandner, F.; Menden, P.; Bergbauer, V.; Zizlsperger, M.; Nerreter, S.; Lingl, S.; Repp, J.; Wilhelm, J.; Huber, M. A.; Gerasimenko, Y. A.; Huber, R.
署名单位：
University of Regensburg; University of Regensburg
刊物名称：
Nature
ISSN/ISSBN：
0028-5919
DOI：
10.1038/s41586-024-07355-7
发表日期：
2024-05-09
关键词：
single-molecule
tunneling-microscopy
terahertz control
fizeau drag
field
polaritons
light
time
spectroscopy
electrons
摘要：
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 pi/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. All-optical subcycle microscopy is achieved on atomic length scales, with picometric spatial and femtosecond temporal resolution.