Spin state energies were calculated for an antiferromagnetic linear chain composed of a doublet (S ) 1 / 2 ) radical and a biradical with a triplet (S ) 1) ground state by numerical diagonalization of a finite-size Heisenberg-Dirac spin Hamiltonian. A ferrimagnetic-like ground state with a spin value of S ) N/2 (N stands for the number of repeating units) appears if the intermolecular antiferromagnetic exchange interactions are uniform between all the S ) 1 / 2 sites. This finding is consistent with a simple picture of differing and neighboring spin angular moments S's ordered in sublattices in an antiparallel manner. On the other hand, quasi-degenerate low-lying states appear as the spatial symmetry of the intermolecular antiferromagnetic interactions is lowered. The quasi-degeneracy destabilizes the ferrimagnetic-like ground state. This instability is inherent in multicentered antiferromagnetic interactions between open-shell organic molecular systems, suggesting a prerequisite for long-range magnetic order in purely organic molecule-based ferrimagnetics. Such prerequisite has never been reported until now. The results of the calculations are invoked to explain the susceptibility and the spin-spin relaxation time measured for the first model system for purely organic ferrimagnetics, a nitronyl nitroxide-based molecular crystal composed of an S ) 1 / 2 and S ) 1 molecules (
N4-Aminocytidine is a potent mutagen toward Escherichia coli and Salmonella typhimurium. It induced reversion of an amber mutant of phi X174 phage (am3) to the wild type. This reversion was shown to be exclusively due to the AT to GC transition. It is likely that N4-aminocytidine is metabolized within the bacterial cells into N4-aminodeoxycytidine 5'-triphosphate and this nucleotide is incorporated into DNA during the multiplication of the cells and the phages, thereby causing base-pair transitions. The molecular basis for this erroneous replication was obtained in studies of in vitro incorporation of N4-aminodeoxycytidine 5'-triphosphate into polynucleotides catalyzed by the E. coli DNA polymerase I large fragment. The results have shown that this cytosine analogue can be efficiently incorporated as a substitute of cytosine and that it can also be incorporated as a substitute of thymine. The ratio in the rate of the N4-aminocytosine nucleotide incorporation to that of natural nucleotide incorporation was 1/2 to cytosine and 1/30 to thymine. Furthermore, the N4-aminocytosine residues in the polynucleotide templates can be read by the enzyme as efficiently as cytosines, and guanines were incorporated opposite to them.
A model compound for purely organic ferrimagnets has been studied by single-crystal cw-ESR spectroscopy. A heterospin system under study is composed of two kinds of nitronylnitroxide molecules with the ground states of S ) 1 / 2 and S ) 1. These molecules are stacked in an alternating chain in the crystal. The cw-ESR signal of the compound was found to split into two signals below 10 K, which were reproduced by the superposition of two Lorentzian signals. The X-ray measurements at 9.6 K disclosed that the crystal structure remained unchanged at low temperatures, indicating that the origin of the ESR line splitting is not attributable to symmetry reduction associated with structural change but to some change in the spin state: Two distinguishable paramagnetic species are found from the ESR spectra. The appearance of two kinds of paramagnetic species in the alternating chain at finite temperature is expected as a primitive model of thermal excitation in the ferrimagnetic chain which is based on a theoretical calculation. The present experimental results demonstrate that the classical picture of ferrimagnetic spin state (antiparallel alignment of adjacent spins with different spin quantum numbers) is invalidated to describe organic molecule-based exchangecoupled spin systems and overlooks an essential part of the nature of ferrimagnetics.
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