Design Principles for Metastable Standing Molecules

The Journal of Physical Chemistry C, vol. 126, pp. 6880–6891

Abstract

Molecular nanofabrication with a scanning probe microscope (SPM) is a promising route toward the prototyping of metastable functional molecular structures and devices which do not form spontaneously. The aspect of mechanical stability is crucial for such structures, especially if they extend into the third dimension vertical to the surface. A prominent example is freestanding molecules fabricated on a metal which can function as field emitters or electric field sensors. Improving the stability of such molecular configurations is an optimization task involving many degrees of freedom and therefore best tackled by computational nanostructure design. Here, we use density functional theory to study 3,4,9,10-perylene-tetracarboxylic dianhydride (PTCDA) standing on the Ag(111) surface as well as on the tip of a scanning probe microscope. We cast our results into a simple set of design principles for such metastable structures, the validity of which we subsequently demonstrate in two computational case studies. Our work proves the capabilities of computational nanostructure design in the field of metastable molecular structures and offers the intuition needed to fabricate new devices without tedious trial and error.

Authors 5

1. Hadi H. Arefi

   Forschungszentrum Jülich · Helmholtz-Zentrum Berlin für Materialien und Energie · Jülich Aachen Research Alliance

   Affiliation as printed

   Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, 14109 Berlin, Germany

   Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, Jülich, 52425 Jülich, Germany

   Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425 Jülich, Germany

2. Daniel Corken

   University of Warwick

   Affiliation as printed

   Department of Chemistry, University of Warwick, Gibbet Hill Road, CV4 7AL Coventry, U.K

3. Frank Stefan Tautz Aachen Experimentalphysik IV A

   Forschungszentrum Jülich · Jülich Aachen Research Alliance · RWTH Aachen University

   Affiliation as printed

   Experimentalphysik IV A, RWTH Aachen University, Otto-Blumenthal-Straße, 52074 Aachen, Germany

   Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, Jülich, 52425 Jülich, Germany

   Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425 Jülich, Germany

4. Reinhard J. Maurer

   University of Warwick

   Affiliation as printed

   Department of Chemistry, University of Warwick, Gibbet Hill Road, CV4 7AL Coventry, U.K

5. Christian Wagner corresponding

   Forschungszentrum Jülich · Jülich Aachen Research Alliance

   Affiliation as printed

   Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, Jülich, 52425 Jülich, Germany

   Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425 Jülich, Germany