Composite molecular assemblies: Nanoscale structural control and spectroelectrochemical diversity

Graham De Ruiter, Michal Lahav, Guennadi Evmenenko, Pulak Dutta, Domenico A. Cristaldi, Antonino Gulino, Milko E. Van Der Boom

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

The controlled deposition of metal complexes from solution on inorganic surfaces offers access to functional materials that otherwise would be elusive. For such surface-confined interfaces to form, specific assembly sequences are often used. We show here that varying the assembly sequence of two well-defined and iso-structural osmium and ruthenium polypyridyl complexes results in interfaces with strikingly different spectroelectrochemical properties. Successive deposition of redox-active layers of osmium and ruthenium polypyridyl complexes, leads to self-propagating molecular assemblies (SPMAs) with distinct internal interfaces and individually addressable components. In contrast, the clear separation of these interfaces upon sequential deposition of these two complexes, results in charge trapping or electrochemical communication between the metal centers, as a function of layer thickness and applied assembly sequence. The SPMAs were characterized using a variety of techniques, including: UV-vis spectroscopy, spectroscopic ellipsometry, electrochemistry, synchrotron X-ray reflectivity, angle-resolved X-ray photoelectron spectroscopy, and spectroelectrochemistry. The combined data demonstrate that the sequence-dependent assembly is a decisive factor that influences and provides the material properties that are difficult to obtain otherwise.

Original languageEnglish
Pages (from-to)16533-16544
Number of pages12
JournalJournal of the American Chemical Society
Volume135
Issue number44
DOIs
Publication statusPublished - Nov 6 2013

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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