We have shown that the intense concentration of light in plasmonic nanogaps can pull single Au atoms out of the metal facet. The light is further concentrated around such atomically-sharp features, allowing optical probing of single molecules and atoms.
Current work:
Picocavity subatomic light
Enhanced optical field around a single gold atom pulled by light from the upper crystal facet. This trapped optical field is concentrated to <0.2nm, massively enhancing the optical response within its subatomic volume. We are now tracking the picocavity resonances in time. [1,2]
Reconstructing single molecule videos
Using systematic quantum theory, the transient vibrational spectra can be used to construct a video of single molecules near the picocavity atom. We are trying to understand better how these coordination bonds to metal atoms work. [3]
Massive forces from light-induced attraction
The nN forces required to pull out a metal atom are far more than conventional optical tweezing. At the atomic scale, we find the tightly-confined light can shift electron clouds on the tip of the nearby molecules, producing huge dipole-dipole attractions. [2]
Room light driven Au atoms
We recently discovered a class of molecules that bind to Au or Ag, and under even very weak illumination can move atoms by fractions of a mm. The secret appears to be a cooperative binding site between pairs of molecules which hand over the metal atoms rapidly. [5]
Flares: cooperative picocavities
Brief broadband flashes of light emitted by these plasmonic nanocavities are now shown by full quantum theory to come from entire atomic monolayers being lifted. Surprisingly, light can be trapped in the 0.2nm gap between metal atoms. [4]
Key papers:
- Single-molecule optomechanics in picocavities, Science 354, 726 (2016); DOI: 10.1126/science.aah5243
- Picocavities: a primer, Nano Letters 22, 5859 (2022); DOI: 10.1021/acs.nanolett.2c01695
- Resolving Sub-Å Ambient Motion through Reconstructions from Vibrational Spectra, Nature Comm (2021); DOI: 10.1038/s41467-021-26898-1
- Quantum plasmonics in sub-atom-thick optical slots, Nano Letters (2023); DOI: 10.1021/acs.nanolett.3c02537
- Extensive photochemical restructuring of molecule-metal surfaces under room light, Nature Comm. (2024); DOI: 10.1038/s41467-024-46125-x
Current people involved:
JJB, Bart deNijs, Paul Kerner, Chenyang Guo,