Abstract
Near-field interactions between metallic surfaces and single molecules play an essential role in the application of metamaterials. To reveal the near-field around a photo-irradiated single molecule on the metallic surface, high-resolution photo-assisted scanning microscopy is required. In this study, we theoretically propose photoinduced force microscopy (PiFM) measurements of single molecules at the atomic resolution. For experimental demonstration, we performed a numerical calculation of PiFM images of various transition states, including optical forbidden transitions, and interpreted them in terms of the interaction between the molecular internal polarization structures and localized plasmon. We also clarified the critical role of atomic-scale structures on the tip surface for high-resolution PiFM measurements.
Highlights
A fascinating feature of metamaterials is their ability to manipulate and enhance chiral fields, leading to peculiar interactions with chiral matter systems
In [5,6,7,8], the authors have shown that near-field interactions of metallic surfaces and molecules should play an essential role in the above-mentioned metamaterial effects, it is still challenging to reveal the spatial structures of the near-field around a single molecule because of the limited resolution of existing photo-assisted microscopic techniques
We demonstrate Photoinduced force microscopy (PiFM) measurements of a single molecule using a simplified model to understand the microscopic interaction between the molecule and the localized plasmon
Summary
A fascinating feature of metamaterials is their ability to manipulate and enhance chiral fields, leading to peculiar interactions with chiral matter systems. CD signals and enable highly sensitive enantioselective detection of chiral molecules [5,6,7,8] These results indicate that the elucidation of the interaction between metamaterials and molecular systems is an important factor for the future development of metamaterials for relevant applications. By utilizing such properties of PiFM, we can elucidate the near-field interaction between metamaterials and single molecules For this purpose, it is important to theoretically clarify how the intrinsic optical response of each molecule can be “seen” by PiFM. We investigated how atomic-scale structures on the tip surface, picocavity [22], play an important role in the atomic resolution measurement of PiFM, which detects the field gradient of localized plasmons
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