Journal
SCIENCE
Volume 376, Issue 6591, Pages 401-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abn9220
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Funding
- US Department of Energy, Office of Basic Energy Sciences [DE-SC0019448]
- U.S. Department of Energy (DOE) [DE-SC0019448] Funding Source: U.S. Department of Energy (DOE)
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This article reports on a method for THz pump-probe measurements based on single molecule quantum sensing, achieved by combining STM and THz laser and using H-2 as a two-level system. Atomic-scale and femtosecond-scale spatial and temporal resolutions were obtained, allowing visualization of heterogeneity in the chemical environment at sub-angstrom scale.
A scanning tunneling microscope (STM) combined with a pump-probe femtosecond terahertz (THz) laser can enable coherence measurements of single molecules. We report THz pump-probe measurements that demonstrate quantum sensing based on a hydrogen (H-2) molecule in the cavity created with an STM tip near a surface. Atomic-scale spatial and femtosecond temporal resolutions were obtained from this quantum coherence. The H-2 acts as a two-level system, with its coherent superposition exhibiting extreme sensitivity to the applied electric field and the underlying atomic composition of the copper nitride (Cu2N) monolayer islands grown on a Cu(100) surface. We acquired time-resolved images of THz rectification of H-2 over Cu2N islands for variable pump-probe delay times to visualize the heterogeneity of the chemical environment at sub-angstrom scale.
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