Spin-1/2 Quantum Antiferromagnet on a Three-Dimensional Honeycomb Lattice Formed by a New Organic Biradical F4BIPBNN

We have succeeded in synthesizing a new organic biradical F4BIPBNN [= 2,2'-(3,3',5,5'-tetrafluorobiphenyl-4,4'-diyl)bis(4,4,5,5-tetramethylimidazolin-1-oxyl 3-oxide)] which forms an S = 1/2 Heisenberg three-dimensional honeycomb antiferromagnet. Each site of a honeycomb layer alternately couples with upper or lower layers, which results in the unique three-dimensional honeycomb network with four nearest neighbors. At zero magnetic field, antiferromagnetic long-range order has been observed below TN = 2.7 K. Magnetic susceptibility in both paramagnetic and antiferromagnetic states and the magnetization curves are well reproduced by quantum Monte Carlo calculations with three antiferromagnetic interactions in the range of 4.3 to 6.6 K. From the concave shape of the magnetization curve, the shrinkage of spin due to spin fluctuations is evaluated to approximately 30% with respect to its classical value. The phase diagram of magnetic field versus temperature was determined by heat capacity and magnetization. In the field region below 3 T, a slight increase of TN was observed, which reflects the effect of spin fluctuations.