Magnetic transitions and spin-glass reentrance in two-dimensional [MnII(TCNE)(NCMe)2]X (X = PF6,AsF6,SbF6) molecular magnets.

The structural, spectroscopic and magnetic properties of the two-dimensional (2D) molecule-based magnets of [Mn(II)(TCNE)(NCMe)2]X (X = PF6, AsF6, SbF6; TCNE = tetracyanoethylene, NCMe = acetonitrile) composition are reported. It is shown that the alteration of the interlayer distance by increasing the anion size has little effect on the critical magnetic ordering temperature, Tc, suggesting that it depends predominantly on the intra-plane magnetic exchange. The observed field-induced irreversibility in static magnetization, a slow decay of isothermal remanence below Tc, and the dynamic susceptibility data are in accord with a re-entrant spin-glass nature of the ground state of all materials. In contrast to the isostructural Fe-based magnets, in which strong magnetocrystalline anisotropy facilitates the finite temperature magnetic ordering with the magnetization easy axis perpendicular to the µ4-TCNE(•-) plane, in the studied Mn-based magnets the easy axis is canted away from the normal direction, due to a small magnetocrystalline anisotropy. The two magnetic transitions observed on cooling are assigned to the ferrimagnetic long-range ordering of the normal magnetization component followed by the re-entrant spin-glass type transition resulting from a random freezing of the in-plane magnetization component.

Magnetic bistability and nucleation of magnetic bubbles in a layered 2D organic-based magnet [Fe(TCNE)(NCMe)2][FeCl4].

The 2D layered organic-based magnet [Fe(TCNE)(NCMe)2][FeCl4] (TCNE=tetracyanoethylene) exhibits a unique macroscopic magnetic bistability between the field-cooled and zero-field-cooled states, which cannot be explained by either superparamagnetic behavior or spin freezing due to spin glass order. This magnetic bistability is described through consideration of the ensemble of uncoupled 2D Ising layers and their magnetization reversal initiated by a field-induced nucleation of magnetic bubbles in individual layers. The bubble nucleation rate strongly depends on the external field and temperature resulting in anomalous magnetic relaxation.

Multiple photonic responses in films of organic-based magnetic semiconductor V(TCNE)x, x approximately 2.

Concomitant photoinduced magnetic and electrical phenomena are reported for the organic-based magnetic semiconductor V(TCNE)x (x approximately 2; TCNE=tetracyanoethylene; magnetic ordering temperature Tc approximately 400 K). Upon optical excitation (457.9 nm), the system can be trapped in a thermally reversible photoexcited state, which exhibits reduced magnetic susceptibility and increased conductivity with a simultaneous change in IR absorption spectrum. The multiple photonic effects in V(TCNE)x are proposed to originate from structural changes induced by internal excitation in (TCNE)- anions, which lead to relaxation to a long-lived metastable state.