Various regimes of quantum behavior in S = 1/2 Heisenberg antiferromagnetic chain with fourfold periodicity

We have succeeded in synthesizing single crystals of the verdazyl radical beta-2,6-Cl2-V [= beta-3-(2,6-dichlorophenyl)-1,5-diphenylverdazyl]. The ab initio MO calculation indicated the formation of an S = 1/2 Heisenberg antiferromagnetic chain with four-fold magnetic periodicity consisting of three types of exchange interactions.We have successfully explained the magnetic and thermodynamic properties based on the expected spin model by using the quantum Monte Carlo method. Furthermore, we revealed that the alternating and unique Ising ferromagnetic chains become effective in the specific field regions and observed a cooperative phenomenon caused by the magnetic order and quantum fluctuations. These results demonstrate that verdazyl radical could form unconventional spin model with interesting quantum behavior and provide a new way to study a variety of quantum spin systems.

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