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Picosecond excited state dynamics and excitation transport in solution and on surfaces

Technical Report ·
OSTI ID:5259101
Time correlated single photon counting was employed in studies of excitation transport (ET) depolarization in 2- and 3-dimensional disordered systems. Reduced concnetrations ranged up to )approximately)3 in ethylene glycol solutions of DODCI (3-dimensioanal system) and )approximately)5 in Langmuir-Blodgett monolayers containing octadecyl rhodamine B (2-dimensional system). Discrepencies between experiment and current ET theories (3-body Gochanour-Andersen-Fayer andor 2-particle Huber) are small when artifacts due to reabsorption, dimerization (and concomitant trapping), solvent reorganization, and molecular reorientation are minimized or correctly modeled. Discrepancies persist in glycerol solutions of DODCI; they are attributed to orientational correlation between chromophores. The orientational correlation apparently arises from 3-dimensional liquid glycerol structure and extends to )approximately)R/sub O/. An optical shot noise limites detection scheme was developed which enabled pump-probe transient absorption studies of submonolayer rhodamine 640 adsorbed on fused silica and ZnO. The ground state recovery dynamics on silica are coverage dependent due to excitation trapping by dye aggregates. In contrast, the recovery on ZnO is significantly faster and essentially coverage independent. This provides strong evidence for efficient dye )yield) semiconductor nonradiative excitation decay
Research Organization:
Ames Lab., IA (USA)
DOE Contract Number:
W-7405-ENG-82
OSTI ID:
5259101
Report Number(s):
IS-T-1291; ON: DE88007621
Country of Publication:
United States
Language:
English