As described by Kutoglu (1976 [161), single crystals of As4S4 (II) phase have been grown using a new two-step synthesis that drastically increases the reproducibility that is attainable in synthetic experiments. First, through photo-induced phase transformation, pararealgar powder is prepared as a precursor instead of AsS melt. Then it is dissolved and recrystallized from CS2 solvent. Results show that single crystals of the As4S4 (II) phase were obtained reproducibly through the dissolution-recrystallization process. Single crystals of As4S4 (II) obtained using this method were translucent and showed a uniform yellow-orange color. The crystal exhibits a platelet-like shape as a thin film with well-developed faces (01 0) and (0 (1) over bar 0). The grown crystals are as large as 0.50 x 0.50 x 0.01 mm. They were characterized using powder and single crystal X-ray diffraction techniques to confirm the phase identification and the lattice parameters. The As4S4 (II) phase crystallizes in monoclinic system with cell parameters a=11.202(4) angstrom, b=9.954(4) angstrom, c=7.142(4) angstrom, beta=92.81(4)degrees, V=795.4(6) angstrom(3), which shows good agreement with the former value. Raman spectroscopic studies elucidated the behavior of the substance and the relation among phases of tetra-arsenic tetrasulfide. (C) 2010 Elsevier B.V. All rights reserved.