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Using phase-matched third-harmonic generation we determine the effective nonlinear susceptibilities in [Hg.sub.2][Cl.sub.2] (Calomel) to [MATHEMATICAL EXPRESSION NOT REPRODUCIBLE IN ASCII] and [MATHEMATICAL EXPRESSION NOT REPRODUCIBLE IN ASCII] for type I and type II phase matching, respectively. The type III phase matching uses the same tensor components as type I and is deduced to be [MATHEMATICAL EXPRESSION NOT REPRODUCIBLE IN ASCII]. The effective third-order susceptibilities of [Hg.sub.2][Cl.sub.2] are two orders of magnitude higher than those of CaC[O.sub.3], and the tensor components [[chi].sub.11] - 3[[chi].sub.18] exceed the components of ADP by a factor of 5. These measurements demonstrate that Calomel might be a promising material to be used for nonlinear optical devices. OCIS codes: 160.4330, 260.1440, 190.4160, 190.4720, 190.4400, 190.2620.