Полный текст,
Полный текст на сайте правообладателя
Доп.точки доступа:
Lukzen, N.N.; Ivanov, K.L.; Sadovsky, V.M.; Садовский, Владимир Михайлович; Kaptein, R.; Sagdeev, R.Z.
Труды сотрудников ИВМ СО РАН
w10=
Найдено документов в текущей БД: 3
Magnetic field and spin effects on the recombination of radicals on two-dimensional surfaces
/ N. N. Lukzen [et al.] // Dokl. Phys. Chem. - 2013. - Vol. 449. - P44-47, DOI 10.1134/S0012501613030056. - Cited References: 15. - This work was supported by the Russian Foundation for Basic Research (project nos. 11-03-00356 and 11-03-00296), the Siberian Branch of the RAS (interdisciplinary project no. 71), the Division of Chemistry and Materials Science, RAS (project no. 5.1.1), and program P-220 of the Government of the Russian Federation (grant no. 11.G34.31.0045).
. - 4. - ISSN 0012-5016
РУБ Chemistry, Physical
Полный текст,
Полный текст на сайте правообладателя
Доп.точки доступа:
Lukzen, N.N.; Ivanov, K.L.; Sadovsky, V.M.; Садовский, Владимир Михайлович; Kaptein, R.; Sagdeev, R.Z.
Полный текст,
Полный текст на сайте правообладателя
Доп.точки доступа:
Lukzen, N.N.; Ivanov, K.L.; Sadovsky, V.M.; Садовский, Владимир Михайлович; Kaptein, R.; Sagdeev, R.Z.
Theoretical description of spin-selective reactions of radical pairs diffusing in spherical 2D and 3D microreactors
/ K. L. Ivanov, V. M. Sadovsky, N. N. Lukzen // J Chem Phys. - 2015. - Vol. 143, Is. 8, DOI 10.1063/1.4928648
. - ISSN 0021-9606
Кл.слова (ненормированные):
Chemical reactors -- Diffusion -- Green's function -- Magnetic fields -- Magnetism -- Micelles -- Reaction rates -- Spheres -- Spin dynamics -- Analytical expressions -- Chemically induced dynamic nuclear polarization -- Magnetic field dependences -- Magnetic field strengths -- Magnetic interactions -- Recombination efficiency -- Two dimensional diffusion -- Two dimensional model -- Magnetic field effects
Аннотация: In this work, we treat spin-selective recombination of a geminate radical pair (RP) in a spherical "microreactor," i.e., of a RP confined in a micelle, vesicle, or liposome. We consider the microreactor model proposed earlier, in which one of the radicals is located at the center of the micelle and the other one undergoes three-dimensional diffusion inside the micelle. In addition, we suggest a two-dimensional model, in which one of the radicals is located at the "pole" of the sphere, while the other one diffuses on the spherical surface. For this model, we have obtained a general analytical expression for the RP recombination yield in terms of the free Green function of two-dimensional diffusion motion. In turn, this Green function is expressed via the Legendre functions and thus takes account of diffusion over a restricted spherical surface and its curvature. The obtained expression allows one to calculate the RP recombination efficiency at an arbitrary magnetic field strength. We performed a comparison of the two models taking the same geometric parameters (i.e., the microreactor radius and the closest approach distance of the radicals), chemical reactivity, magnetic interactions in the RP and diffusion coefficient. Significant difference between the predictions of the two models is found, which is thus originating solely from the dimensionality effect: for different dimensionality of space, the statistics of diffusional contacts of radicals becomes different altering the reaction yield. We have calculated the magnetic field dependence of the RP reaction yield and chemically induced dynamic nuclear polarization of the reaction products at different sizes of the microreactor, exchange interaction, and spin relaxation rates. Interestingly, due to the intricate interplay of diffusional contacts of reactants and spin dynamics, the dependence of the reaction yield on the microreactor radius is non-monotonous. Our results are of importance for (i) interpreting experimental data for magnetic field effects on RP recombination in confined space and (ii) for describing kinetics of chemical reactions, which occur predominantly on the surfaces of biomembranes, i.e., lipid peroxidation reactions. © 2015 AIP Publishing LLC.
Scopus,
WOS
Держатели документа:
International Tomography Center, Siberian Branch, Russian Academy of Sciences, Institutskaya St. 3a, Novosibirsk, Russian Federation
Novosibirsk State University, Pirogova St. 2, Novosibirsk, Russian Federation
Institute of Computational Modeling, Siberian Branch, Russian Academy of Sciences, Akademgorodok 50/44, Krasnoyarsk, Russian Federation
Доп.точки доступа:
Sadovsky, V.M.; Садовский, Владимир Михайлович; Lukzen, N. N.
Кл.слова (ненормированные):
Chemical reactors -- Diffusion -- Green's function -- Magnetic fields -- Magnetism -- Micelles -- Reaction rates -- Spheres -- Spin dynamics -- Analytical expressions -- Chemically induced dynamic nuclear polarization -- Magnetic field dependences -- Magnetic field strengths -- Magnetic interactions -- Recombination efficiency -- Two dimensional diffusion -- Two dimensional model -- Magnetic field effects
Аннотация: In this work, we treat spin-selective recombination of a geminate radical pair (RP) in a spherical "microreactor," i.e., of a RP confined in a micelle, vesicle, or liposome. We consider the microreactor model proposed earlier, in which one of the radicals is located at the center of the micelle and the other one undergoes three-dimensional diffusion inside the micelle. In addition, we suggest a two-dimensional model, in which one of the radicals is located at the "pole" of the sphere, while the other one diffuses on the spherical surface. For this model, we have obtained a general analytical expression for the RP recombination yield in terms of the free Green function of two-dimensional diffusion motion. In turn, this Green function is expressed via the Legendre functions and thus takes account of diffusion over a restricted spherical surface and its curvature. The obtained expression allows one to calculate the RP recombination efficiency at an arbitrary magnetic field strength. We performed a comparison of the two models taking the same geometric parameters (i.e., the microreactor radius and the closest approach distance of the radicals), chemical reactivity, magnetic interactions in the RP and diffusion coefficient. Significant difference between the predictions of the two models is found, which is thus originating solely from the dimensionality effect: for different dimensionality of space, the statistics of diffusional contacts of radicals becomes different altering the reaction yield. We have calculated the magnetic field dependence of the RP reaction yield and chemically induced dynamic nuclear polarization of the reaction products at different sizes of the microreactor, exchange interaction, and spin relaxation rates. Interestingly, due to the intricate interplay of diffusional contacts of reactants and spin dynamics, the dependence of the reaction yield on the microreactor radius is non-monotonous. Our results are of importance for (i) interpreting experimental data for magnetic field effects on RP recombination in confined space and (ii) for describing kinetics of chemical reactions, which occur predominantly on the surfaces of biomembranes, i.e., lipid peroxidation reactions. © 2015 AIP Publishing LLC.
Scopus,
WOS
Держатели документа:
International Tomography Center, Siberian Branch, Russian Academy of Sciences, Institutskaya St. 3a, Novosibirsk, Russian Federation
Novosibirsk State University, Pirogova St. 2, Novosibirsk, Russian Federation
Institute of Computational Modeling, Siberian Branch, Russian Academy of Sciences, Akademgorodok 50/44, Krasnoyarsk, Russian Federation
Доп.точки доступа:
Sadovsky, V.M.; Садовский, Владимир Михайлович; Lukzen, N. N.
Magnetic field effect on recombination of radicals diffusing on a two-dimensional plane
/ N. N. Lukzen, K. L. Ivanov, V. M. Sadovsky, R. Z. Sagdeev // J Chem Phys. - 2020. - Vol. 152, Is. 3. - Ст. 034103, DOI 10.1063/1.5131583
. - ISSN 0021-9606
Кл.слова (ненормированные):
Cytology -- Electrospinning -- Free radical reactions -- Reaction kinetics -- Spin dynamics -- Diffusion controlled -- Dipole dipole interactions -- Lipid peroxidation -- Magneto sensitives -- Singlet-triplet -- Time-dependent rate coefficients -- Two dimensional plane -- Two-dimensional surface -- Magnetic field effects
Аннотация: Magnetic Field Effects (MFEs) on the recombination of radicals, which diffuse on an infinite plane, are studied theoretically. The case of spin-selective diffusion-controlled recombination of Radical Pairs (RPs) starting from a random spin state is considered assuming uniform initial distribution of the radicals. In this situation, reaction kinetics is described by a time-dependent rate coefficient K(t), which tends to zero at long times. Strong MFEs on K(t) are predicted that originate from the ?g and hyperfine driven singlet-triplet mixing in the RP. The effects of spin relaxation on the magnetic field are studied, as well as the influence of the dipole-dipole interaction between the electron spins of the RP. In the two-dimensional case, this interaction is not averaged out by diffusion and it strongly affects the MFE. The results of this work are of importance for interpreting MFEs on lipid peroxidation, a magnetosensitive process occurring on two-dimensional surfaces of cell membranes. © 2020 Author(s).
Scopus
Держатели документа:
International Tomography Center, Siberian Branch, Russian Academy of Sciences, Institutskaya Str. 3a, Novosibirsk, 630090, Russian Federation
Novosibirsk State University, Pirogova Str. 1, Novosibirsk, 630090, Russian Federation
Institute of Computational Modeling, Siberian Branch, Russian Academy of Sciences, Akademgorodok 50/44, Krasnoyarsk, 660036, Russian Federation
Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Science, Leninskii Prospect 31, Moscow, 19991, Russian Federation
Доп.точки доступа:
Lukzen, N. N.; Ivanov, K. L.; Sadovsky, V. M.; Sagdeev, R. Z.
Кл.слова (ненормированные):
Cytology -- Electrospinning -- Free radical reactions -- Reaction kinetics -- Spin dynamics -- Diffusion controlled -- Dipole dipole interactions -- Lipid peroxidation -- Magneto sensitives -- Singlet-triplet -- Time-dependent rate coefficients -- Two dimensional plane -- Two-dimensional surface -- Magnetic field effects
Аннотация: Magnetic Field Effects (MFEs) on the recombination of radicals, which diffuse on an infinite plane, are studied theoretically. The case of spin-selective diffusion-controlled recombination of Radical Pairs (RPs) starting from a random spin state is considered assuming uniform initial distribution of the radicals. In this situation, reaction kinetics is described by a time-dependent rate coefficient K(t), which tends to zero at long times. Strong MFEs on K(t) are predicted that originate from the ?g and hyperfine driven singlet-triplet mixing in the RP. The effects of spin relaxation on the magnetic field are studied, as well as the influence of the dipole-dipole interaction between the electron spins of the RP. In the two-dimensional case, this interaction is not averaged out by diffusion and it strongly affects the MFE. The results of this work are of importance for interpreting MFEs on lipid peroxidation, a magnetosensitive process occurring on two-dimensional surfaces of cell membranes. © 2020 Author(s).
Scopus
Держатели документа:
International Tomography Center, Siberian Branch, Russian Academy of Sciences, Institutskaya Str. 3a, Novosibirsk, 630090, Russian Federation
Novosibirsk State University, Pirogova Str. 1, Novosibirsk, 630090, Russian Federation
Institute of Computational Modeling, Siberian Branch, Russian Academy of Sciences, Akademgorodok 50/44, Krasnoyarsk, 660036, Russian Federation
Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Science, Leninskii Prospect 31, Moscow, 19991, Russian Federation
Доп.точки доступа:
Lukzen, N. N.; Ivanov, K. L.; Sadovsky, V. M.; Sagdeev, R. Z.