Abstract
Detailed degenerate four wave mixing (DFWM) studies of four molybdenum complexes, cis-Mo(CO) 4(PPh 3) 2, cis-Mo(CO) 4(AsPh 3) 2, cis-Mo(CO) 4(PPh 2Np) 2 and cis-Mo(CO) 4(P(OPh) 3) 2 are reported in this paper. Upon exposure to air/oxygen, the χ (3) values of solutions of the first three complexes increase dramatically with time. However, when excess free ligand is added to any of the solutions, no additional increase in the χ (3) value is observed. Hence, it is possible to obtain solutions with high χ (3) values by first oxidizing the solution and then adding excess ligand to stabilize the solution. Further, the increase in the χ (3) values of the solutions parallels the increase in the linear absorption, but it is unclear whether the increased linear absorption plays any role in the increase in the χ (3) values of the solutions. This study also shows how degenerate four wave mixing can be used as a very sensitive technique to detect the chemical change in a solution when the third order optical nonlinearities of the reactant and product are very different.
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