Control of Oxidation and Spin State in a Single-Molecule Junction

Abstract

The oxidation and spin state of a metal-organic molecule determine its chemical reactivity and magnetic properties. Here, we demonstrate the reversible control of the oxidation and spin state in a single Fe porphyrin molecule in the force field of the tip of a scanning tunneling microscope. Within the regimes of half-integer and integer spin state, we can further track the evolution of the magnetocrystalline anisotropy. Our experimental results are corroborated by density functional theory and wave function theory. This combined analysis allows us to draw a complete picture of the molecular states over a large range of intramolecular deformations.

Designing a mechanically driven spin-crossover molecular switch via organic embedding

“…We exploit the magneto-structural relationship of the encapsulated FeP molecule [26][27][28][29] as the basis for the device functionality. FeP has been demonstrated to realize a spincrossover (SCO) under various conditions, e.g., through surface adsorption, [29][30][31][32] in molecular assembly, 33 or in singlemolecule junctions by approaching an STM tip, 34,35 all of which create internal strains in the embedded molecule. However, depending on the surface topology and surfacemolecule interactions, outer ligand groups, metal atom coordination and oxidation state, and the nature of external stimuli, the type of magnetic transition, i.e., low-spin (LS) to high-spin (HS) or vice versa, as well as the amount of required strain, vary substantially, oen diminishing the propensity for a SCO.…”

“…FeP has been demonstrated to realize a spin-crossover (SCO) under various conditions, e.g. , through surface adsorption, 29–32 in molecular assembly, 33 or in single-molecule junctions by approaching an STM tip, 34,35 all of which create internal strains in the embedded molecule. However, depending on the surface topology and surface–molecule interactions, outer ligand groups, metal atom coordination and oxidation state, and the nature of external stimuli, the type of magnetic transition, i.e.…”

Co(CO)n/Cu(001): Towards understanding chemical control of the Kondo effect

“…In this work, we would like to focus on the effect molecular ligands on the Kondo effect [17][18][19][20] .…”

Iron doped gold cluster nanomagnets: ab initio determination of barriers for demagnetization

“…On the other hand, several studies examined magnetic properties of transition metal complexes, i.e., a transition metal ion surrounded by a primarily organic framework, with wave function based, multireference perturbation theory methods. [23][24][25] In addition, Aravena et al studied transition metal ions in an inorganic polyoxometalate environment. 26 To our present knowledge, our study is the rst to report calculations of magnetic properties of transition metal doped gold clusters at the level of multireference perturbation theory.…”