A. Water Exchange 2326 B. Proton Exchange 2327 C. Electronic Relaxation 2327 D. Relaxivity 2331 E. Outerand Second-Sphere Relaxivity 2334 F. Methods of Improving Relaxivity 2336 V. Macromolecular Conjugates 2336 A. Introduction 2336 B. General Conjugation Methods 2336 C. Synthetic Linear Polymers 2336 D. Synthetic Dendrimer-Based Agents 2338 E. Naturally Occurring Polymers (Proteins, Polysaccharides, and Nucleic Acids) 2339

https://mriquestions.com/uploads/3/4/5/7/34572113/lauffer_1999_review.pdf

Gadolinium(III) Chelates as MRI Contrast Agents: Structure, Dynamics, and Applications

https://febs.onlinelibrary.wiley.com/doi/pdf/10.1016/0014-5793%2881%2980608-4

A highly resolved, oxygen-evolving photosystem II preparation from spinach thylakoid membranes

Gadolinium(III) complexes are often used in clinical MRI to increase contrast by selectively relaxing the water molecules near the complex. There is a desire to improve the sensitivity (relaxivity) of these contrast agents in order to detect molecular targets. This tutorial review describes the molecular factors that contribute to relaxivity and illustrates with recent examples how these can be optimized. It may be of interest to senior undergraduates and more advanced researchers interested in lanthanide chemistry, biophysics, and/or molecular imaging.

Strategies for increasing the sensitivity of gadolinium based MRI contrast agents.

The manganese and calcium ions of photosynthetic oxygen evolution.

Oxygenic photosynthesis, the principal converter of sunlight into chemical energy on earth, is catalyzed by four multi-subunit membrane-protein complexes: photosystem I (PSI), photosystem II (PSII), the cytochrome b6f complex, and F-ATPase PSI generates the most negative redox potential in nature and largely determines the global amount of enthalpy in living systems PSII generates an oxidant whose redox potential is high enough to enable it to oxidize H2O, a substrate so abundant that it assures a practically unlimited electron source for life on earth During the last century, the sophisticated techniques of spectroscopy, molecular genetics, and biochemistry were used to reveal the structure and function of the two photosystems The new structures of PSI and PSII from cyanobacteria, algae, and plants has shed light not only on the architecture and mechanism of action of these intricate membrane complexes, but also on the evolutionary forces that shaped oxygenic photosynthesis

/pdf/structure-and-function-of-photosystems-i-and-ii-3adv0rc3ct.pdf

Structure and function of photosystems i and ii

Chloroplast thylakoid membranes isolated in the presence of EDTA retain high rates of O2 evolution (≥340 μmol·h-1·mg chlorophyll-1) but contain no Mn2+ that is detectable by electron paramagnetic resonance (EPR) at room temperature. The total Mn2+ content of these preparations is 4.6 per 400 chlorophylls; 0.6 Mn2+ can be released by addition of Ca2+, a treatment that does not affect O2 evolution. The remaining Mn2+ (4 per 400 chlorophylls) appears to be functionally associated with O2 evolution activity. Inhibition by Tris, NH2OH, or heat will release a small fraction of Mn2+ from these membranes (≈25% with Tris, for example). Addition of Ca2+ further enhances Mn2+ release so that for Tris and for NH2OH, 2 and 3, respectively, Mn2+ per 400 chlorophylls are extracted from the O2-evolving complex. Based on the microwave power-saturation properties of the EPR signal IIf, which arises from an intermediate electron carrier in the water splitting process, it appears that one of the four Mn2+ associated with photosystem II is uniquely sensitive to Tris. A new model is proposed for the organization and inhibitor sensitivity of manganese in the O2-evolving complex.

Stoichiometry, inhibitor sensitivity, and organization of manganese associated with photosynthetic oxygen evolution.

The enhancement of the spin-lattice relaxation rate for nuclear spins in a ligand bound to a paramagnetic metal ion [known as the paramagnetic relaxation enhancement (PRE)] arises primarily through the dipole-dipole (DD) interaction between the nuclear spins and the electron spins. In solution, the DD interaction is modulated mostly by reorientation of the nuclear spin-electron spin axis and by electron spin relaxation. Calculations of the PRE are in general complicated, mainly because the electron spin interacts so strongly with the other degrees of freedom that its relaxation cannot be described by second-order perturbation theory or the Redfield theory. Three approaches to resolve this problem exist in the literature: The so-called slow-motion theory, originating from Swedish groups [Benetis et al., Mol. Phys. 48, 329 (1983); Kowalewski et al., Adv. Inorg. Chem. 57, (2005); Larsson et al., J. Chem. Phys. 101, 1116 (1994); T. Nilsson et al., J. Magn. Reson. 154, 269 (2002)] and two different methods based on simulations of the dynamics of electron spin in time domain, developed in Grenoble [Fries and Belorizky, J. Chem. Phys. 126, 204503 (2007); Rast et al., ibid. 115, 7554 (2001)] and Ann Arbor [Abernathy and Sharp, J. Chem. Phys. 106, 9032 (1997); Schaefle and Sharp, ibid. 121, 5387 (2004); Schaefle and Sharp, J. Magn. Reson. 176, 160 (2005)], respectively. In this paper, we report a numerical comparison of the three methods for a large variety of parameter sets, meant to correspond to large and small complexes of gadolinium(III) and of nickel(II). It is found that the agreement between the Swedish and the Grenoble approaches is very good for practically all parameter sets, while the predictions of the Ann Arbor model are similar in a number of the calculations but deviate significantly in others, reflecting in part differences in the treatment of electron spin relaxation. The origins of the discrepancies are discussed briefly.

Comparison of different methods for calculating the paramagnetic relaxation enhancement of nuclear spins as a function of the magnetic field.

The nuclear magnetic resonance spectra of phosphabenzene, arsabenzene, and stibabenzene

Spin dynamics (SD) methods have been developed to compute NMR paramagnetic relaxation enhancements (NMR-PRE) produced by solutes with electron spin S⩾1 in solution. The spin dynamics algorithms, which are implemented as the computer program SpinDyn.f, are similar in spirit to molecular dynamics calculations in statistical mechanics, except that the spin motion is propagated numerically in time using quantum mechanical equations of motion of the spin operators, rather than Newtonian equations of motion of the molecular degrees of freedom as in MD simulations. SD simulations as implemented in SpinDyn.f provide accurate, flexible, and rapid calculations of NMR-PRE phenomena with few of the assumptions or limitations of previous analytical theories. The program calculates inter- and intramolecular NMR-PRE phenomena for both integer and half-integer spin systems processing under arbitrary Zeeman and zfs Hamiltonians in the presence of Brownian reorientation. Isotropic Brownian reorientation is simulated by mea...

/pdf/spin-dynamics-calculations-of-electron-and-nuclear-spin-1av9n0r0w4.pdf

Spin dynamics calculations of electron and nuclear spin relaxation times in paramagnetic solutions

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Stoichiometry, inhibitor sensitivity, and organization of manganese associated with photosynthetic oxygen evolution.

Comparison of different methods for calculating the paramagnetic relaxation enhancement of nuclear spins as a function of the magnetic field.

The nuclear magnetic resonance spectra of phosphabenzene, arsabenzene, and stibabenzene

Spin dynamics calculations of electron and nuclear spin relaxation times in paramagnetic solutions

The nuclear magnetic resonance spectra of phosphabenzene, arsabenzene, and stibabenzene