metallic molecules


and charged molecular monolayers

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charged and metallic molecular monolayers through surface-induced aromatic stabilization

As predicted by quantum-mechanics, electrons in individual molecules can only have certain discrete energies with notable gaps in between. In extended metallic solids, on the other hand, these discrete levels are so close to each other that they can be regarded as a continuum of energies. Electrons can then easily move though the material, which is why metals conduct electricity so well. If molecules are brought into contact with a metal surface, they usually retain a finite electronic gap and, in this sense, stay molecules. In some cases, however, the first layer of molecules turns metallic itself and thus becomes part of the underlying metal. In this research paper, we develop a chemical rationale for this intriguing phenomenon. In many reported instances, we find that the molecular structure changes significantly through the bonding of specific chemical side-groups to the metal surface. The molecules at the interface are thus converted into different chemical species, one with a strongly reduced electronic gap. This mechanism of surface-induced aromatic stabilization helps molecules to overcome competing effects that tend to keep their energy levels well separated from where the conducting electrons reside in the metal. Our findings aid in the chemical design of stable precursors for metallic molecular monolayers, and thus enable new routes for the chemical engineering of metal surfaces. In particular, we envision a seamless integration of inorganic and organic components in hybrid (opto-)electronic devices.

This work was published in:
G. Heimel, S. Duhm, I. Salzmann, A. Gerlach, A. Strozecka, J. Niederhausen, C. Bürker, T. Hosokai, I. Fernandez-Torrente, G. Schulze, S. Winkler, A. Wilke, R. Schlesinger, J. Frisch, B. Bröker, A. Vollmer, B. Detlefs, J. Pflaum, S. Kera, K. J. Franke, N. Ueno, J. I. Pascual, F. Schreiber, N. Koch
Charged and metallic molecular monolayers through surface-induced aromatic stabilization
Nature Chemistry 5, 187 (2013). full-text
 

  further reading

G. M. Rangger, L. Romaner, O. T. Hofmann, G. Heimel, M. G. Ramsey, E. Zojer
Analyzing the Bonding between Conjugated Organic Molecules and Noble Metal Surfaces using Overlap Populations
J. Chem. Theory Comput. 6, 3481-3489 (2010). link

G. M. Rangger, O. T. Hofmann, L. Romaner, G. Heimel, B. Bröker, R.-P. Blum, R. L. Johnson, N. Koch, E. Zojer
F4TCNQ on Cu, Ag, and Au as prototypical example for a strong organic acceptor on coinage metals
Phys. Rev. B 79, 165306 (2009). link

L. Romaner, G. Heimel, J.-L. Brédas, A. Gerlach, F. Schreiber, R. L. Johnson, S. Duhm, N. Koch, J. Zegenhagen, E. Zojer
Impact of bi-directional charge transfer and molecular distortions on the electronic structure of a metal-organic interface
Phys. Rev. Lett. 99, 256801 (2007). link

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