The effects of pressure on two prototypes of molecule-based magnets have been investigated through dc magnetic measurements in an attempt to realize these higher transition temperatures (T C 's). The target compounds are (1) a genuine organic radical weak-ferromagnet, p-NC-C 6 F 4 -CNSSN (T C = 35.5 K) with through-space intermolecular interaction and (2) a metal-complex ferrimagnet [Mn(en)] 3 [Cr(CN) 6 ] 2 •4H 2 O (T C = 69 K) with a cyanide bridge network between magnetic metal ions. In (1), T C is enhanced as dT C /dP = 22.0 K/GPa, and it exceeds 70 K at around 1.5 GPa. Exceeding a border of 70 K is worthy in the field of the genuine organic system. In (2), pressure dependences of T C and magnetic moment have been investigated over wider pressure region. The ideal material control for higher-T C was realized at around 5 GPa. Two types of pressure cells developed for these studies are also mentioned.KEYWORDS: molecule-based magnets, magnetic susceptibility, high pressure, pressure cell
IntroductionIn recent days, much attention of material scientists has been devoted to a molecule-based magnetic system, called as molecule-based magnet, from the interest of the magneto-structural correlation and the viewpoints of new functionality due to nano-size effect, giant molecules and the topology.1, 2) The studies of the above-mentioned moleculebased magnets are divided into two, below.The first category is a genuine organic system without magnetic metal ions. There are furthermore two strategies on constructing the magneto-structural correlation; through-space interaction in an organic radical system and through-bond one in an organic polymer one. These compounds belonging to the first category are commonly soft, flexible and brittle. In this sense, the structural control via applying pressure presents us wealthy information about the interaction mechanism.3) In the case of organic radical system, intermolecular SOMO (single-occupied molecular orbital)-SOMO overlap favors the antiferromagnetic spin configuration, while the overlappings such as SOMO-HOMO (highest occupied MO) and SOMO-LUMO (lowest unoccupied MO) encourage the ferromagnetic correlation. Under a forced shrinkage by applying pressure, the former is relatively easy to be enlarged, whereas the latter often weakens. 4,5) Thus, pressurization can work as a negative factor on enhancing the ferromagnetic transition temperature T C . If we hope to construct a higher-T C magnet by using a technique of pressurization, it is reasonable to seek after higher-T C in a weak-ferromagnetic system with antiferromagnetic frame and the slight magnetic anisotropy.