Application of Smoluchowski's generalized theory to the kinetics of triplet-triplet annihilation of anthracene in viscous solution after long-pulse excitation

Typeset version

 

TY  - JOUR
  - Nickel, B.,Borowicz, P.,Ruth*, A. A.,Troe, J.
  - 2004
  - July
  - Physical Chemistry Chemical Physics
  - Application of Smoluchowski's generalized theory to the kinetics of triplet-triplet annihilation of anthracene in viscous solution after long-pulse excitation
  - Validated
  - ()
  - 6
  - 13
  - 3350
  - 3363
  - The validity of Smoluchowski's theory is demonstrated by its application to the bimolecular triplet-triplet annihilation (TTA) T-1 + T-1 --> S-0+ S-1 in viscous solution. For that purpose the delayed S-1 --> S-0 fluorescence of anthracene in cis-1,3-dimethylcyclohexane/trans-1,4-dimethylcyclohexane (1:1) was measured after UV excitation with long laser pulses (similar to30 mus) in a temperature range where TTA is completely diffusion controlled. Through the adequate treatment of the kinetics of TTA upon spatially homogeneous and spatially periodic excitation (which is partially based on the results of previous publications) absolute values for the diffusion coefficients D of triplet molecules, for the effective annihilation distance R-A and for the Forster radius R-ST of heterogeneous annihilation S-1 + T-1 --> S-0 + T-n were determined. The temperature dependence of all three parameters (D, R-A and R-ST) is discussed. From the decrease of R-A with increasing temperature, the parameters A and L can be determined, which define the exponential distance dependence of the annihilation of a triplet pair in the kinetic model of Butler and Pilling (1977). Differences of the two models and applicability criteria are discussed.The validity of Smoluchowski's theory is demonstrated by its application to the bimolecular triplet-triplet annihilation (TTA) T-1 + T-1 --> S-0+ S-1 in viscous solution. For that purpose the delayed S-1 --> S-0 fluorescence of anthracene in cis-1,3-dimethylcyclohexane/trans-1,4-dimethylcyclohexane (1:1) was measured after UV excitation with long laser pulses (similar to30 mus) in a temperature range where TTA is completely diffusion controlled. Through the adequate treatment of the kinetics of TTA upon spatially homogeneous and spatially periodic excitation (which is partially based on the results of previous publications) absolute values for the diffusion coefficients D of triplet molecules, for the effective annihilation distance R-A and for the Forster radius R-ST of heterogeneous annihilation S-1 + T-1 --> S-0 + T-n were determined. The temperature dependence of all three parameters (D, R-A and R-ST) is discussed. From the decrease of R-A with increasing temperature, the parameters A and L can be determined, which define the exponential distance dependence of the annihilation of a triplet pair in the kinetic model of Butler and Pilling (1977). Differences of the two models and applicability criteria are discussed.
  - 1463-90761463-9076
  - ://000223041400021 ://000223041400021
DA  - 2004/07
ER  - 
@article{V67924374,
   = {Nickel,  B. and Borowicz,  P. and Ruth*,  A. A. and Troe,  J. },
   = {2004},
   = {July},
   = {Physical Chemistry Chemical Physics},
   = {Application of Smoluchowski's generalized theory to the kinetics of triplet-triplet annihilation of anthracene in viscous solution after long-pulse excitation},
   = {Validated},
   = {()},
   = {6},
   = {13},
  pages = {3350--3363},
   = {{The validity of Smoluchowski's theory is demonstrated by its application to the bimolecular triplet-triplet annihilation (TTA) T-1 + T-1 --> S-0+ S-1 in viscous solution. For that purpose the delayed S-1 --> S-0 fluorescence of anthracene in cis-1,3-dimethylcyclohexane/trans-1,4-dimethylcyclohexane (1:1) was measured after UV excitation with long laser pulses (similar to30 mus) in a temperature range where TTA is completely diffusion controlled. Through the adequate treatment of the kinetics of TTA upon spatially homogeneous and spatially periodic excitation (which is partially based on the results of previous publications) absolute values for the diffusion coefficients D of triplet molecules, for the effective annihilation distance R-A and for the Forster radius R-ST of heterogeneous annihilation S-1 + T-1 --> S-0 + T-n were determined. The temperature dependence of all three parameters (D, R-A and R-ST) is discussed. From the decrease of R-A with increasing temperature, the parameters A and L can be determined, which define the exponential distance dependence of the annihilation of a triplet pair in the kinetic model of Butler and Pilling (1977). Differences of the two models and applicability criteria are discussed.The validity of Smoluchowski's theory is demonstrated by its application to the bimolecular triplet-triplet annihilation (TTA) T-1 + T-1 --> S-0+ S-1 in viscous solution. For that purpose the delayed S-1 --> S-0 fluorescence of anthracene in cis-1,3-dimethylcyclohexane/trans-1,4-dimethylcyclohexane (1:1) was measured after UV excitation with long laser pulses (similar to30 mus) in a temperature range where TTA is completely diffusion controlled. Through the adequate treatment of the kinetics of TTA upon spatially homogeneous and spatially periodic excitation (which is partially based on the results of previous publications) absolute values for the diffusion coefficients D of triplet molecules, for the effective annihilation distance R-A and for the Forster radius R-ST of heterogeneous annihilation S-1 + T-1 --> S-0 + T-n were determined. The temperature dependence of all three parameters (D, R-A and R-ST) is discussed. From the decrease of R-A with increasing temperature, the parameters A and L can be determined, which define the exponential distance dependence of the annihilation of a triplet pair in the kinetic model of Butler and Pilling (1977). Differences of the two models and applicability criteria are discussed.}},
  issn = {1463-90761463-9076},
   = {://000223041400021 ://000223041400021},
  source = {IRIS}
}
AUTHORSNickel, B.,Borowicz, P.,Ruth*, A. A.,Troe, J.
YEAR2004
MONTHJuly
JOURNAL_CODEPhysical Chemistry Chemical Physics
TITLEApplication of Smoluchowski's generalized theory to the kinetics of triplet-triplet annihilation of anthracene in viscous solution after long-pulse excitation
STATUSValidated
TIMES_CITED()
SEARCH_KEYWORD
VOLUME6
ISSUE13
START_PAGE3350
END_PAGE3363
ABSTRACTThe validity of Smoluchowski's theory is demonstrated by its application to the bimolecular triplet-triplet annihilation (TTA) T-1 + T-1 --> S-0+ S-1 in viscous solution. For that purpose the delayed S-1 --> S-0 fluorescence of anthracene in cis-1,3-dimethylcyclohexane/trans-1,4-dimethylcyclohexane (1:1) was measured after UV excitation with long laser pulses (similar to30 mus) in a temperature range where TTA is completely diffusion controlled. Through the adequate treatment of the kinetics of TTA upon spatially homogeneous and spatially periodic excitation (which is partially based on the results of previous publications) absolute values for the diffusion coefficients D of triplet molecules, for the effective annihilation distance R-A and for the Forster radius R-ST of heterogeneous annihilation S-1 + T-1 --> S-0 + T-n were determined. The temperature dependence of all three parameters (D, R-A and R-ST) is discussed. From the decrease of R-A with increasing temperature, the parameters A and L can be determined, which define the exponential distance dependence of the annihilation of a triplet pair in the kinetic model of Butler and Pilling (1977). Differences of the two models and applicability criteria are discussed.The validity of Smoluchowski's theory is demonstrated by its application to the bimolecular triplet-triplet annihilation (TTA) T-1 + T-1 --> S-0+ S-1 in viscous solution. For that purpose the delayed S-1 --> S-0 fluorescence of anthracene in cis-1,3-dimethylcyclohexane/trans-1,4-dimethylcyclohexane (1:1) was measured after UV excitation with long laser pulses (similar to30 mus) in a temperature range where TTA is completely diffusion controlled. Through the adequate treatment of the kinetics of TTA upon spatially homogeneous and spatially periodic excitation (which is partially based on the results of previous publications) absolute values for the diffusion coefficients D of triplet molecules, for the effective annihilation distance R-A and for the Forster radius R-ST of heterogeneous annihilation S-1 + T-1 --> S-0 + T-n were determined. The temperature dependence of all three parameters (D, R-A and R-ST) is discussed. From the decrease of R-A with increasing temperature, the parameters A and L can be determined, which define the exponential distance dependence of the annihilation of a triplet pair in the kinetic model of Butler and Pilling (1977). Differences of the two models and applicability criteria are discussed.
PUBLISHER_LOCATION
ISBN_ISSN1463-90761463-9076
EDITION
URL://000223041400021 ://000223041400021
DOI_LINK
FUNDING_BODY
GRANT_DETAILS