Estimation of the Fraction of Spin-Correlated Radical Ion Pairs in Irradiated Alkanes using Magnetosensitive Recombination Luminescence from Exciplexes Generated upon Recombination of a Probe Pair

被引:8
作者
Melnikov, Anatoly R. [1 ,2 ]
Verkhovlyuk, Vladimir N. [1 ]
Kalneus, Evgeny V. [1 ]
Korolev, Valeri V. [1 ]
Borovkov, Vsevolod I. [1 ,2 ]
Sherin, Peter S. [2 ,3 ]
Davydova, Maria P. [1 ,2 ]
Vasilevsky, Sergei F. [1 ,2 ]
Stass, Dmitri V. [1 ,2 ]
机构
[1] Voevodsky Inst Chem Kinet & Combust SB RAS, 3 Inst Skaya Str, Novosibirsk 630090, Russia
[2] Novosibirsk State Univ, 2 Pirogova Str, Novosibirsk 630090, Russia
[3] Int Tomog Ctr SB RAS, 3a Inst Skaya Str, Novosibirsk 630090, Russia
来源
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS | 2017年 / 231卷 / 02期
基金
俄罗斯科学基金会;
关键词
diphenylacetylene; exciplex luminescence; magnetic field effect; radical ion pair; spin correlation; X-ray irradiation; MOLECULAR CHARGE-TRANSFER; EXCITED SINGLET-STATE; MAGNETIC-FIELD MODULATION; OD-ESR; DELAYED FLUORESCENCE; OPTICAL-DETECTION; ELECTRON-TRANSFER; LIQUID ALKANES; RATE CONSTANTS; QUANTUM BEATS;
D O I
10.1515/zpch-2016-0819
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We suggest a convenient probe exciplex system for studies in radiation spin chemistry based on a novel acceptor-substituted diphenylacetylene, 1-(phenylethynyl)-4-(trifluoromethyl) benzene that has a very short fluorescence lifetime (<200 ps) and low quantum yield (0.01) of intrinsic emission, provides efficient electron capture in alkanes and efficient exciplex formation upon recombination in pair with DMA radical cation, while exhibiting a shifted to red exciplex emission band as compared to the parent system DMA-diphenylacetylene. After chemical, luminescent, radiation and spin-chemical characterization of the new system we used the magnitude of magnetic field effect in its exciplex emission band for experimental estimation of the fraction of spin-correlated radical ion pairs under X-irradiation with upper energy cutoff 40 keV in a set of 11 alkanes. For linear and branched alkanes magnetic field effects and the corresponding fractions are approximately 19-20% and 0.28, while for cyclic alkanes they are lower at 16-17% and 0.22, respectively.
引用
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页码:239 / 267
页数:29
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