Quenching by Oxygen of the Lowest Singlet and Triplet States of Pyrene and the Efficiency of the Formation of Singlet Oxygen in Liquid Solution under High Pressure

Quenching by oxygen of the lowest singlet (S1) and triplet (T1) states of pyrene at pressures up to 400 MPa in liquid solution was investigated. The rate constant of the S1 state, k q S, decreased significantly with increasing pressure, while that of the T1 state, k q T, was nearly independent of pr...

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Published in:The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2002-04, Vol.106 (15), p.3982-3990
Main Authors: Okamoto, Masami, Tanaka, Fujio
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description Quenching by oxygen of the lowest singlet (S1) and triplet (T1) states of pyrene at pressures up to 400 MPa in liquid solution was investigated. The rate constant of the S1 state, k q S, decreased significantly with increasing pressure, while that of the T1 state, k q T, was nearly independent of pressure at the lower pressure region (
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The rate constant of the S1 state, k q S, decreased significantly with increasing pressure, while that of the T1 state, k q T, was nearly independent of pressure at the lower pressure region (&lt;100 MPa) and decreased monotonically with further increase in pressure. The activation volume for k q S, ΔV q S⧧, at 0.1 MPa fell in the range of 12−16 cm3/mol, depending on the solvents examined, whereas that for k q T, ΔV q T⧧, was nearly zero. It was found that both the activation volumes, ΔV q S⧧ and ΔV q T⧧, are significantly smaller than those determined from the pressure dependence of the solvent viscosity, η, ΔV η ⧧ (22−25 cm3/mol). For the quenching of the S1 state, the large difference between ΔV q S⧧ and ΔV η ⧧ was interpreted in terms of the competition of the quenching with diffusion, and k q S was separated into the contributions of the rate constants for diffusion, k diff, and for the bimolecular quenching in the solvent cage, k S,bim. For the quenching of the T1 state, it was found that k q T/k diff increases over 1/9 and approaches 4/9 with increasing pressure. The oxygen concentration dependence on the quantum yield for the formation of singlet oxygen, ΦΔ, in methylcylohexane (MCH) was measured at pressures up to 400 MPa in order to separate ΦΔ into the contributions of the S1 and T1 states. From the results, together with those of the pressure dependence of the quantum yield of T1 state, the branching ratio for the formation of singlet oxygen in the T1 state, f Δ T, was found to decrease with increasing pressure. 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A, Molecules, spectroscopy, kinetics, environment, &amp; general theory</title><addtitle>J. Phys. Chem. A</addtitle><description>Quenching by oxygen of the lowest singlet (S1) and triplet (T1) states of pyrene at pressures up to 400 MPa in liquid solution was investigated. The rate constant of the S1 state, k q S, decreased significantly with increasing pressure, while that of the T1 state, k q T, was nearly independent of pressure at the lower pressure region (&lt;100 MPa) and decreased monotonically with further increase in pressure. The activation volume for k q S, ΔV q S⧧, at 0.1 MPa fell in the range of 12−16 cm3/mol, depending on the solvents examined, whereas that for k q T, ΔV q T⧧, was nearly zero. It was found that both the activation volumes, ΔV q S⧧ and ΔV q T⧧, are significantly smaller than those determined from the pressure dependence of the solvent viscosity, η, ΔV η ⧧ (22−25 cm3/mol). For the quenching of the S1 state, the large difference between ΔV q S⧧ and ΔV η ⧧ was interpreted in terms of the competition of the quenching with diffusion, and k q S was separated into the contributions of the rate constants for diffusion, k diff, and for the bimolecular quenching in the solvent cage, k S,bim. For the quenching of the T1 state, it was found that k q T/k diff increases over 1/9 and approaches 4/9 with increasing pressure. The oxygen concentration dependence on the quantum yield for the formation of singlet oxygen, ΦΔ, in methylcylohexane (MCH) was measured at pressures up to 400 MPa in order to separate ΦΔ into the contributions of the S1 and T1 states. From the results, together with those of the pressure dependence of the quantum yield of T1 state, the branching ratio for the formation of singlet oxygen in the T1 state, f Δ T, was found to decrease with increasing pressure. The oxygen quenching of the T1 state from these results was discussed by using the mechanism that involves the encounter complex pairs with singlet, triplet, and quintet spin multiplicities.</description><issn>1089-5639</issn><issn>1520-5215</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2002</creationdate><recordtype>article</recordtype><recordid>eNptkMtOwzAQRSMEEqWw4A-8YcEi4EfsJEtU9YEUqUUpEjvLdSatS5sUOxHN9_CjJH2wYjVXmjNnNON59wQ_EUzJ83qHCRMh1xdej3CKfU4Jv2wzjmKfCxZfezfOrTFuMRr0vJ-3Ggq9MsUSLRo03TdLKFCZo2oFKCm_wVUobZsbqJAqMjS3ZtfltFIVuA6cNRYKODS7mWGeG21aZXO2jEq7VZUpD9qz67TIFCgxX7XJUFpu6gNUFxlYNDHLFZpZcK62cOtd5Wrj4O5U-977aDgfTPxkOn4dvCS-YoJUvuAkjsKI6kizQIWYckZETDjOApLjiNMMC8LyWOWxxhlnC0VBYBZGOgCqQbG-93j0als6ZyGXO2u2yjaSYNl9V_59t2X9I2tcBfs_UNlPKUIWcjmfpZKyyXgkog_JWv7hyCvt5LqsbdFe8o_3F-D_iT8</recordid><startdate>20020418</startdate><enddate>20020418</enddate><creator>Okamoto, Masami</creator><creator>Tanaka, Fujio</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20020418</creationdate><title>Quenching by Oxygen of the Lowest Singlet and Triplet States of Pyrene and the Efficiency of the Formation of Singlet Oxygen in Liquid Solution under High Pressure</title><author>Okamoto, Masami ; Tanaka, Fujio</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a361t-65198782c8c34a70253169150d41f0852d0613f9af9c0d53ba2e60378c4e2cea3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2002</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Okamoto, Masami</creatorcontrib><creatorcontrib>Tanaka, Fujio</creatorcontrib><collection>Istex</collection><collection>CrossRef</collection><jtitle>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, &amp; general theory</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Okamoto, Masami</au><au>Tanaka, Fujio</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Quenching by Oxygen of the Lowest Singlet and Triplet States of Pyrene and the Efficiency of the Formation of Singlet Oxygen in Liquid Solution under High Pressure</atitle><jtitle>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, &amp; general theory</jtitle><addtitle>J. Phys. Chem. A</addtitle><date>2002-04-18</date><risdate>2002</risdate><volume>106</volume><issue>15</issue><spage>3982</spage><epage>3990</epage><pages>3982-3990</pages><issn>1089-5639</issn><eissn>1520-5215</eissn><abstract>Quenching by oxygen of the lowest singlet (S1) and triplet (T1) states of pyrene at pressures up to 400 MPa in liquid solution was investigated. The rate constant of the S1 state, k q S, decreased significantly with increasing pressure, while that of the T1 state, k q T, was nearly independent of pressure at the lower pressure region (&lt;100 MPa) and decreased monotonically with further increase in pressure. The activation volume for k q S, ΔV q S⧧, at 0.1 MPa fell in the range of 12−16 cm3/mol, depending on the solvents examined, whereas that for k q T, ΔV q T⧧, was nearly zero. It was found that both the activation volumes, ΔV q S⧧ and ΔV q T⧧, are significantly smaller than those determined from the pressure dependence of the solvent viscosity, η, ΔV η ⧧ (22−25 cm3/mol). For the quenching of the S1 state, the large difference between ΔV q S⧧ and ΔV η ⧧ was interpreted in terms of the competition of the quenching with diffusion, and k q S was separated into the contributions of the rate constants for diffusion, k diff, and for the bimolecular quenching in the solvent cage, k S,bim. For the quenching of the T1 state, it was found that k q T/k diff increases over 1/9 and approaches 4/9 with increasing pressure. The oxygen concentration dependence on the quantum yield for the formation of singlet oxygen, ΦΔ, in methylcylohexane (MCH) was measured at pressures up to 400 MPa in order to separate ΦΔ into the contributions of the S1 and T1 states. From the results, together with those of the pressure dependence of the quantum yield of T1 state, the branching ratio for the formation of singlet oxygen in the T1 state, f Δ T, was found to decrease with increasing pressure. The oxygen quenching of the T1 state from these results was discussed by using the mechanism that involves the encounter complex pairs with singlet, triplet, and quintet spin multiplicities.</abstract><pub>American Chemical Society</pub><doi>10.1021/jp013675c</doi><tpages>9</tpages></addata></record>
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title Quenching by Oxygen of the Lowest Singlet and Triplet States of Pyrene and the Efficiency of the Formation of Singlet Oxygen in Liquid Solution under High Pressure
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