Sivanandam V N, Cai Jingfei, Redfield Alfred G, Roberts Mary F
Department of Chemistry and Biochemistry and the Rosenstiel Basic Medical Sciences Research Institute, Brandeis University, Waltham, Massachusetts 02454, USA.
J Am Chem Soc. 2009 Mar 18;131(10):3420-1. doi: 10.1021/ja808431h.
High resolution (13)C NMR field cycling (covering 11.7 down to 0.002 T) relaxation studies of the sn-2 carbonyl of phosphatidylcholines in vesicles provide a detailed look at the dynamics of this position of the phospholipid in vesicles. The spin-lattice relaxation rate, R(1), observed down to 0.05 T is the result of dipolar and CSA relaxation components characterized by a single correlation time tau(c), with a small contribution from a faster motion contributing to CSA relaxation. At lower fields, R(1) increases further with a correlation time consistent with vesicle tumbling. The tau(c) is particularly interesting since it is 2-3 times slower than what is observed for (31)P of the same phospholipid. However, cholesterol increases the tau(c) for both (31)P and (13)C sites to the same value, approximately 25 ns. These observations suggest faster local motion dominates the dipolar relaxation of the (31)P, while a slower rotation or wobble dominates the relaxation of the carbonyl carbon by the alpha-CH(2) group. The faster motion must be damped with the sterol present. As a general methodology, high resolution (13)C field cycling may be useful for quantifying dynamics in other complex systems as long as a (13)C label (without attached protons) can be introduced.
对囊泡中磷脂酰胆碱sn-2羰基进行高分辨率(13)C核磁共振场循环(覆盖11.7至0.002 T)弛豫研究,能详细观察磷脂在此位置在囊泡中的动力学情况。在低至0.05 T时观察到的自旋晶格弛豫率R(1),是由具有单一相关时间tau(c)的偶极和CSA弛豫分量导致的,其中快速运动对CSA弛豫有小贡献。在更低场强下,R(1)随着与囊泡翻滚一致的相关时间进一步增加。tau(c)特别有趣,因为它比同一磷脂的(31)P观察到的相关时间慢2至3倍。然而,胆固醇会使(31)P和(13)C位点的tau(c)增加到相同值,约25纳秒。这些观察结果表明,更快的局部运动主导了(31)P的偶极弛豫,而较慢的旋转或摆动主导了α-CH(2)基团对羰基碳的弛豫。只要能引入(13)C标记(无连接质子),高分辨率(13)C场循环作为一种通用方法,可能对量化其他复杂系统中的动力学有用。