open access

https://hdl.handle.net/2115/95119

Generalized Transition Moment and Oscillator Strength for Optimal Control of Excited States Using Near-Field Light

英語

2024-05-09

American Chemical Society

Journal of physical chemistry letters

15(18)

4775-4781

The near field is a highly localized light field that is present in the vicinity of materials. It holds considerable potential for manipulating molecular excitation through the design of nanostructures. To that end, a simple yet applicable computational method is required. This letter presents an optimization strategy to achieve targeted electronic excitation in molecules using near-field light. The generalized transition moment and oscillator strength based on the multipolar Hamiltonian can incorporate key parameters affecting the near field, including shape, size, and material composition. This calculation helps optimize electronic transitions through manipulation of the aforementioned parameters. The feasibility of the proposed scheme was demonstrated using a scanning tunneling microscopic setup with light, wherein the near field is controlled by varying the tip position in two dimensions. This approach paves the way for further innovations, which may ultimately enable precise control of molecular behavior by using tailored near-field interactions.

学術雑誌論文

Accepted Manuscript

This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/articlesonrequest/AOR-33YYWKRRYUHVPZ8CNQSW

1948-7185