Single Molecules in Strong Optical Fields: A Variable-Temperature Molecular Junction Spectroscopy Setup

Autor: Hai Bi, Chao Jing, Daniel Gerster, Peter Hasch, Joachim Reichert, Johannes V. Barth, Yuxiang Gong
Rok vydání: 2021
Předmět:
Zdroj: Analytical Chemistry. 93:9853-9859
ISSN: 1520-6882
0003-2700
DOI: 10.1021/acs.analchem.1c01633
Popis: In order to advance the development of molecular electronic devices, it is mandatory to improve the understanding of electron transport and functionalities in single molecules, integrated in a well-defined environment. However, limited information can be obtained by solely analyzing I-V characteristics, whence multiparameter studies are required to obtain more information on such systems including chemical bonds, geometry, and intramolecular strain. Therefore, we developed an analytical method incorporating an optical near-field technique, which allows us to investigate single-molecule junctions at variable temperatures in strong optical fields. An apertureless near-field emitter acts as a counter electrode and a plasmonic waveguide to focus surface plasmon polaritons into the molecular junctions, where a strongly enhanced evanescent field is confined to only a few nanometers around the apex of the tip. The proof of concept, even at low temperatures, is demonstrated by simultaneously investigating electronic and optical features of the molecule p-terphenyl-4,4″-dithiol in dependence of its charge state. This multichannel method can be employed to analyze a variety of nearly unexplored properties in single-molecule junctions such as photoconductance and photocurrent generation and allows a characterization of the molecular junctions by spectroscopic means as well.
Databáze: OpenAIRE