Self-assembled monolayers (SAMs) present unique opportunities for controlling the precise position and orientation of individual molecules across nanometer-length scales. The major effort in this field has focused on redox-inactive monolayers formed from just 1-2 molecules that extend across surfaces in well-ordered arrays. Our group is pursuing a new approach to the formation of multicomponent, highly patterned SAMs using redox-active molecules of different structures and dimensions. We are initially targeting metal bis(terpyridine) complexes as modular building blocks capable of functionalization along their (distorted) x-, y-, and z-axis. We show that these can form sulfur-bound homo- and heterometallic SAMs on gold surfaces, which we characterize using surface electrochemistry, X-ray photoelectron spectroscopy, and electrochemical scanning tunneling microscope-based imaging experiments. Through the development of new strategies for molecular surface self-assembly, we aim to facilitate the rational design and construction of functional patterned SAMs that can be utilized in surface-based homogeneous catalysis or advanced nanotechnologies such as molecular electronics or machinery.

Redox-active self-assembled monolayers built from metal bis(terpyridine) complexes

ACS Spring 2022

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