[논문]Calculating NMR paramagnetic relaxation enhancements without adjustable parameters: the spin-3/2 complex Cr(III)(AcAc)3

Miller, Jeremy; Schaefle, Nathaniel; Sharp, Robert

doi:10.1002/mrc.1251

[해외논문] Calculating NMR paramagnetic relaxation enhancements without adjustable parameters: the spin-3/2 complex Cr(III)(AcAc)3

Magnetic resonance in chemistry : MRC, v.41 no.10, 2003년, pp.806 - 812

Miller, Jeremy (Department of Chemistry, State University of New York–) , Schaefle, Nathaniel (Oneonta, Oneonta, NY 13820, USA) , Sharp, Robert (Department of Chemistry, The University of Michigan, Ann Arbor, MI 48109, USA)

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NMR paramagnetic relaxation enhancement (NMR-PRE) produced by the electron spin S = 3/2 complex Cr(III)(acac)3 (acac = acetylacetonato) has been simulated by spin dynamic (SD) simulation methods in order to test current theory of NMR-PRE. This system provides a particularly demanding test of theory, since the Zeeman and zero field splitting (zfs) contributions to the electron spin Hamiltonian are of comparable magnitude in the range of magnetic field variation of the data, and Brownian reorientation of both the zfs tensor and the interspin vector play important roles in the relaxation mechanism. For Cr(III)(acac)3, all of the sensitive parameters of theory were known from independent experiments, so that a calculation was possible without variation of parameters. The R1 field dispersion profile (fdp), reported by Wang et al. (J. Magn. Reson. 1987; 73: 277), exhibit a single pronounced dispersive feature between 0.23 and 2.1 T. SD simulations showed that this feature results physically from the change in spatial quantization of the electron spin motion that occurs in the intermediate regime of field strengths where the Zeeman and zfs energies are comparable. Thus, the observed R1 dispersion for Cr(III)(acac)3 has a qualitatively different physical origin than the dispersions of Solomon–Bloembergen–Morgan theory, where R1 dispersions result from Zeeman breaking of level degeneracies. The shape of the experimental fdp suggests that the point-dipole approximation is invalid for Cr(III)(acac)3 due to delocalization of electron spin density onto the π-system of the acac ligand. After accounting for the altered geometry, good agreement with experiment was obtained. Copyright © 2003 John Wiley & Sons, Ltd.

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참고문헌 (41)

Solomon, I.. Relaxation Processes in a System of Two Spins. Physical review, vol.99, no.2, 559-565.

상세보기
Bloembergen, N.. Proton Relaxation Times in Paramagnetic Solutions. The Journal of chemical physics, vol.27, no.2, 572-573.

상세보기
Bloembergen, N.. Comments on ``Proton Relaxation Times in Paramagnetic Solutions''. The Journal of chemical physics, vol.27, no.2, 595-596.

상세보기
Bloembergen, N., Morgan, L. O.. Proton Relaxation Times in Paramagnetic Solutions. Effects of Electron Spin Relaxation. The Journal of chemical physics, vol.34, no.3, 842-850.

상세보기
Sharp, Robert R.. Nuclear spin relaxation in paramagnetic solutions. Effects of large zero-field splitting in the electron spin Hamiltonian. The Journal of chemical physics, vol.93, no.10, 6921-6928.

상세보기
Sharp, Robert R.. Effect of zero field splitting interactions on the paramagnetic relaxation enhancement of nuclear spin relaxation rates in solution. The Journal of chemical physics, vol.98, no.2, 912-921.

상세보기
Sharp, Robert, Abernathy, Shawn M., Lohr, Lawrence L.. Paramagnetically induced nuclear magnetic resonance relaxation in solutions containing S⩾1 ions: A molecular-frame theoretical and physical model. The Journal of chemical physics, vol.107, no.19, 7620-7629.

상세보기
NILSSON, T., KOWALEWSKI, J.. Low-field theory of nuclear spin relaxation in paramagnetic low-symmetry complexes for electron spin systems of S = 1, 3/2, 2, 5/2, 3 and 7/2. Molecular physics, vol.98, no.20, 1617-1638.

상세보기
Wang, Pei-Lein, Lee, Jing-Huei, Huang, Shiou-Mei, Hwang, Lian-Pin. Proton spin relaxation in solutions of the complex tris(acetylacetonato)chromium(III). Journal of magnetic resonance, vol.73, no.2, 277-286.

상세보기
Morosin, B.. The crystal structure of trisacetylacetonatochromium(III). Acta crystallographica, vol.19, no.1, 131-137.

상세보기
Singer, L. S.. Paramagnetic Resonance Absorption in Some Cr+3 Complexes. The Journal of chemical physics, vol.23, no.2, 379-388.

상세보기
Dokl. Akad. Nauk SSSR Vishnevskaya GP 1072 185 1969
Sharp, R., Lohr, L., Miller, J.. Paramagnetic NMR relaxation enhancement: recent advances in theory. Progress in nuclear magnetic resonance spectroscopy, vol.38, no.2, 115-158.

상세보기
J. Magn. Reson. Sharp RR 491 100 1992

상세보기
Bertini, I., Galas, O., Luchinat, C., Parigi, G.. A Computer Program for the Calculation of Paramagnetic Enhancements of Nuclear-Relaxation Rates in Slowly Rotating Systems. Journal of magnetic resonance. Series A, vol.113, no.2, 151-158.

상세보기
Bertini, Ivano, Kowalewski, Jozef, Luchinat, Claudio, Nilsson, Tomas, Parigi, Giacomo. Nuclear spin relaxation in paramagnetic complexes of S=1: Electron spin relaxation effects. The Journal of chemical physics, vol.111, no.13, 5795-5807.

상세보기
Kruk, Danuta, Nilsson, Tomas, Kowalewski, Jozef. Nuclear spin relaxation in paramagnetic systems with zero-field splitting and arbitrary electron spin. Physical chemistry chemical physics : PCCP, vol.3, no.22, 4907-4917.

상세보기
Sharp, Robert, Lohr, Lawrence. Thermal relaxation of electron spin motion in a thermal equilibrium ensemble: Relation to paramagnetic nuclear magnetic resonance relaxation. The Journal of chemical physics, vol.115, no.11, 5005-5014.

상세보기
J. Chem. Phys. Sharp R 269 154 2002
Abernathy, Shawn M., Sharp, Robert R.. Spin dynamics calculations of electron and nuclear spin relaxation times in paramagnetic solutions. The Journal of chemical physics, vol.106, no.22, 9032-9043.

상세보기
Miller, J. C., Sharp, R. R.. Paramagnetic NMR Relaxation Enhancement: Spin Dynamics Simulations of the Effect of Zero-Field Splitting Interactions for S = ⁵/₂. The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment & general theory, vol.104, no.21, 4889-4895.

상세보기
Larsson, Tomas, Westlund, Per-Olof, Kowalewski, Jozef, Koenig, Seymour H.. Nuclear-spin relaxation in paramagnetic complexes in the slow-motion regime for the electron spin: The anisotropic pseudorotation model for S=1 and the interpretation of nuclear magnetic relaxation dispersion results for a low-symmetry Ni(II) complex. The Journal of chemical physics, vol.101, no.2, 1116-1128.

상세보기
Nilsson, T., Parigi, G., Kowalewski, J.. Experimental NMRD Profiles for Some Low-Symmetry Ni(II) Complexes (S = 1) in Solution and Their Interpretation Using Slow-Motion Theory. The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment & general theory, vol.106, no.18, 4476-4488.

상세보기
Nilsson, T., Svoboda, J., Westlund, P.-O., Kowalewski, J.. Slow-motion theory of nuclear spin relaxation in paramagnetic complexes (S=1) of arbitrary symmetry. The Journal of chemical physics, vol.109, no.15, 6364-6375.

상세보기
Nilsson, T, Kowalewski, J. Slow-Motion Theory of Nuclear Spin Relaxation in Paramagnetic Low-Symmetry Complexes: A Generalization to High Electron Spin. Journal of magnetic resonance, vol.146, no.2, 345-358.

상세보기
Odelius, Michael, Ribbing, Carl, Kowalewski, Jozef. Molecular dynamics simulation of the zero-field splitting fluctuations in aqueous Ni(II). The Journal of chemical physics, vol.103, no.5, 1800-1811.

상세보기
Odelius, Michael, Ribbing, Carl, Kowalewski, Jozef. Spin dynamics under the Hamiltonian varying with time in discrete steps: Molecular dynamics-based simulation of electron and nuclear spin relaxation in aqueous nickel(II). The Journal of chemical physics, vol.104, no.9, 3181-3188.

상세보기
Kruk, Danuta, Kowalewski, Jozef. Vibrational motions and nuclear spin relaxation in paramagnetic complexes: Hexaaquonickel(II) as an example. The Journal of chemical physics, vol.116, no.10, 4079-4086.

상세보기
Doddrell, DM, Bendall, MR, O'Connor, AJ, Pegg, DT. Measurement, employing 1H and 13C spin-lattice relaxation times, of the temperature dependence of the correlation time for rotational reorientation (τR)of diamagnetic transition-metal Bis- and Tris-acetylacetonate complexes. Australian journal of chemistry, vol.30, no.5, 943-.

상세보기
Sharp, Robert R.. Characteristic properties of the nuclear magnetic resonance-paramagnetic relaxation enhancement arising from integer and half-integer electron spins. The Journal of chemical physics, vol.98, no.4, 2507-2515.

상세보기
Sharp, Robert R.. Nuclear spin relaxation due to paramagnetic species in solution: Effect of anisotropy in the zero field splitting tensor. The Journal of chemical physics, vol.98, no.8, 6092-6101.

상세보기
Bovet, Jean-Marc, Sharp, Robert R.. Nuclear magnetic resonance relaxation enhancements produced by paramagnetic solutes: Effects of rhombicity in the zero field splitting tensor with the S=2 spin system as an example. The Journal of chemical physics, vol.99, no.1, 18-26.

상세보기
Abernathy, S. M., Miller, J. C., Lohr, L. L., Sharp, R. R.. Nuclear magnetic resonance-paramagnetic relaxation enhancements: Influence of spatial quantization of the electron spin when the zero-field splitting energy is larger than the Zeeman energy. The Journal of chemical physics, vol.109, no.10, 4035-4046.

상세보기
Miller, J.C., Lohr, L.L., Sharp, R.R.. NMR Paramagnetic Relaxation Enhancement: Test of the Controlling Influence of ZFS Rhombicity for S = 1. Journal of magnetic resonance, vol.148, no.2, 267-276.

상세보기
Bertini, Ivano, Galas, Oleg, Luchinat, Claudio, Messori, Luigi, Parigi, Glacomo. A theoretical analysis of the 1H nuclear magnetic relaxation dispersion profiles of diferric transferrin. The Journal of physical chemistry, vol.99, no.39, 14217-14222.

상세보기
Gottlieb, Hans P. W., Barfield, Michael, Doddrell, David M.. An electron spin density matrix description of nuclear spin-lattice relaxation in paramagnetic molecules. The Journal of chemical physics, vol.67, no.8, 3785-3794.

상세보기
Doddrell, David M., Pegg, David T., Bendall, M.Robin, Gottlieb, Hans P.W.. ¹³C spin-relaxation times in some paramagnetic transition-metal acetylacetonate complexes. Importance of ligand-centred relaxation. Chemical physics letters, vol.39, no.1, 65-68.

상세보기
Kowalewski, Jozef, Laaksonen, Aatto, Nordenskiöld, Lars, Blomberg, Margareta. A nonempirical SCF-MO study of the validity of the Solomon-Bloembergen equation for the hexa-aquonickel (II) ion. The Journal of chemical physics, vol.74, no.5, 2927-2930.

상세보기
Nordenskiold, Lars, Laaksonen, Aatto, Kowalewski, Jozef. Applicability of the Solomon-Bloembergen equation to the study of paramagnetic transition metal-water complexes. An ab initio SCF-MO study. Journal of the American Chemical Society, vol.104, no.2, 379-382.

상세보기
Ma, L., Jorgensen, A.-M. M., Sorensen, G. O., Ulstrup, J., Led, J. J.. Elucidation of the Paramagnetic R₁ Relaxation of Heteronuclei and Protons in Cu(II) Plastocyanin from Anabaena variabilis. Journal of the American Chemical Society, vol.122, no.39, 9473-9485.

상세보기
Wilkens, S. J., Xia, B., Volkman, B. F., Weinhold, F., Markley, J. L., Westler, W. M.. Inadequacies of the Point-Dipole Approximation for Describing Electron−Nuclear Interactions in Paramagnetic Proteins: Hybrid Density Functional Calculations and the Analysis of NMR Relaxation of High-Spin Iron(III) Rubredoxin. The journal of physical chemistry. B, Condensed matter, materials, surfaces, interfaces & biophysical, vol.102, no.42, 8300-8305.

상세보기

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[해외논문] Calculating NMR paramagnetic relaxation enhancements without adjustable parameters: the spin-3/2 complex Cr(III)(AcAc)3

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