- Moradi, Mina;
- Opara, Nadia L;
- Tulli, Ludovico G;
- Wäckerlin, Christian;
- Dalgarno, Scott J;
- Teat, Simon J;
- Baljozovic, Milos;
- Popova, Olha;
- van Genderen, Eric;
- Kleibert, Armin;
- Stahlberg, Henning;
- Abrahams, Jan Pieter;
- Padeste, Celestino;
- Corvini, Philippe F-X;
- Jung, Thomas A;
- Shahgaldian, Patrick
Stable, single-nanometer thin, and free-standing two-dimensional layers with controlled molecular architectures are desired for several applications ranging from (opto-)electronic devices to nanoparticle and single-biomolecule characterization. It is, however, challenging to construct these stable single molecular layers via self-assembly, as the cohesion of those systems is ensured only by in-plane bonds. We herein demonstrate that relatively weak noncovalent bonds of limited directionality such as dipole-dipole (-CN⋅⋅⋅NC-) interactions act in a synergistic fashion to stabilize crystalline monomolecular layers of tetrafunctional calixarenes. The monolayers produced, demonstrated to be free-standing, display a well-defined atomic structure on the single-nanometer scale and are robust under a wide range of conditions including photon and electron radiation. This work opens up new avenues for the fabrication of robust, single-component, and free-standing layers via bottom-up self-assembly.