A novel MRI method based on the intermolecular double-quantum coherence (DQC) for soft tissues is described. DQC images of human brain were obtained for the first time on a whole-body 1.5 T scanner. The combination of quantum and classical formalisms was used to characterize multiple-quantum coherences, and to aid in the design of a DQC imaging sequence. The theoretical analysis suggests that signals from the intermolecular DQCs have higher sensitivity than those from the zeroquantum coherence (ZQC) for human brain, and the sensitivity increases with increased field strength. The DQC signal may provide a new form of contrast for MRI.

In this paper, signals originating from a pure specific coherence of intermolecular three-spin orders were separated and characterized experimentally in highly polarized two-component spin systems. A modified CRAZED sequence with selective radio-frequency excitation was designed to separate the small signals from the strong conventional single-spin single-quantum signals. General theoretical expressions of the pulse sequence with arbitrary flip angle pulses were derived using dipolar field treatment. The expressions were used to predict the relaxation and diffusion properties and optimal xperimental parameters such as flip angles. For the first time, relaxation and diffusion properties of pure intermolecular single-quantum, double-quantum, and triple-quantum coherences of three-spin orders were characterized and analyzed in one-dimensional experiments. All experimental observations are in excellent agreement with the theoretical predictions. The theoretical results show that the quantum-mechanical treatment leads to exactly the same predictions as the dipolar field treatment. The quantitative study of intermolecular multiple-quantum coherences of three-spin orders presented herein provides a better nderstanding of their mechanisms.

To date, both the intermolecular multiple-quantum coherence (MQC) and demagnetizing field models have led to fully quantitative predictions of NMR signals in a highly polarized system using the CRAZED and similar sequences. In this paper, measurements of apparent MQC diffusion rates, Dn app, for a specific apparent coherence order, n, were used to investigate the equivalent between the intermolecular MQC and demagnetizing field treatments. A number of physical effects were analyzed both theoretically and experimentally. These effects include molecular diffusion, variation in dipolar correlation distance, radiation damping, inhomogeneous broadening, and spin relaxation, all of which may alter the NMR signal. Two variations of a two-pulse CRAZED sequence, where the signal attenuation is almost entirely caused by the diffusion weighting, were designed to accurately measure and characterize Dn app during the evolution period. Apparent diffusion rates were extracted from a least-squares fitting of a series of 1H spectra, measured with varying diffusion weighting factors. Complete theoretical formations were explicitly derived from both the intermolecular MQC and demagnetizing field treatments. Numerical simulations based on the demagnetizing field treatment were performed and it was found that the model can be used to predict the apparent diffusion rates. A novel diffusion model for intermolecular MQC is proposed in which the phase shift of each individual spin on different molecules is considered to be uncorrelated. This model successfully predicts the unconventional diffusion behaviors of intermolecular MQCs, specifically for differences of apparent diffusion rates between inter-and intramolecular MQCs. Our theoretical predictions and experimental confirmation demonstrate, for the first time, that Dn app for intermolecular MQCs of order n are characterized by Dn app5nDT for n>2 and D0 app52DT for n50, where DT is the translational molecular diffusion rate of the single quantum coherences. These results do not coincide with Dn5n2DT for n>0 which is a general relationship for an intramolecular n-quantum coherence. These works about the apparent diffusion rates during the evolution period of the CRAZED sequences provide additional evidence to support the argument of the equivalence between the intermolecular MQC and demagnetizing field models. The general results derived from both intermolecular MQC and demagnetizing field treatments in this report can reasonably explain new observations of diffusion phenomena in nonlinear spin echoes by Kimmich and co-workers. Even though the theoretical prediction about intermolecular MQC diffusion is verified only with specific experiments using tailor-made pulse sequences, it is demonstrated that the function dependence of diffusion rate on coherence order is general. These results provide independent evidence to support the intermolecular MQC theory proposed by Warren and co-workers.

Residual intermolecular dipolar interactions may result in undesired spectral features on highly concentrated samples in liquid NMR. Although homonuclear decoupling can be employed to suppress the interactions, it may cause a strong irradiation peak, which obscures the nearby peaks. In order to overcome this shortcoming, a modified CRAZED sequence with three radio-frequency pulses was proposed. The analytical expression derived from the dipolar field treatment was employed to select proper flip angles and phase cycling. Theoretical predictions, experimental observations, and computer simulations demonstrated that the new method effectively suppresses the undesired peaks due to residual dipolar effects.