pH-Dependent cis-trans isomerization rates for azo dyes in aqueous solution

ORGN 79

Nicholas J. Dunn, n-dunn@onu.edu, Tevye C. Celius, t-celius@onu.edu, and Jeffrey A. Gray, j-gray@onu.edu. Department of Chemistry, Ohio Northern University, 525 S. Main St., Ada, OH 45810
Azobenzene derivatives have unusual photo-isomerization properties that may lead to novel molecular switching applications. Photo-initiated cis-trans isomerization rates are known to depend on solvent environment, but kinetic studies in aqueous media have not been previously reported. We use nanosecond UV laser flash photolysis-transient absorption spectroscopy to measure relaxation rates for mono- and di-substituted p-aminoazobenzenes and p-hydroxyazobenzenes in water over the pH range of 11 to 4. Our observed absorption transients fit to simple first-order relaxation rate constants between 101 and 105 s-1, which are generally much larger values than in non-polar solvents, and the nearly linear relationship between rate constant and pH for neutral and acidic solutions suggests that the isomerization mechanism involves an acid-catalyzed pathway. Structural calculations to predict relative energy barriers for neutral and ionic transition states are in progress. Isomerization kinetics for hydroxyazobenzenes in high-pH solution may also involve an ionic pathway but the mechanism is apparently more complex.