Spin diffusion driven by R-symmetry sequences: applications to homonuclear correlation spectroscopy in MAS NMR of biological and organic solids.
Spin diffusion driven by R-symmetry sequences: applications to homonuclear correlation spectroscopy in MAS NMR of biological and organic solids.
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DOI：
10.1021/ja108650x
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发表时间：
2011-03-23
影响因子：
15
通讯作者：
Polenova, Tatyana
中科院分区：
文献类型：
--
作者：
Hou, Guangjin;Yan, Si;Sun, Shangjin;Han, Yun;Byeon, In-Ja L.;Ahn, Jinwoo;Concel, Jason;Samoson, Ago;Gronenborn, Angela M.;Polenova, Tatyana
本文报道了一系列基于R2 π（n = 1，2，v = 1，2）对称性序列的homonucleotide ~（13）C-~（13）C魔角自旋扩散实验.这些实验非常适合于生物和有机系统中的13 C-13 C相关光谱，并且在非常快的MAS条件下特别有利，其中常规的PDSD和DARR实验失败。在非常快的MAS频率下，R211、R221和R222序列在模型化合物和蛋白质中产生优异质量的相关光谱。在这些条件下，各个R2 π显示出不同的偏振转移效率-依赖于各向同性化学位移差异：R221有效地重新耦合小的和大的化学位移差（在蛋白质中，这些分别对应于脂肪族与脂肪族和羰基与脂肪族的相关性），而R211和R222分别表现出最大的重偶联效率。在中等MAS频率（10-20 kHz）下，在这项工作中引入的所有R2 R序列显示出类似的传输效率，并且它们的性能与PDSD和DARR的性能非常相似。对[U-13 C，15 N]-丙氨酸和[U-13 C，15 N] N-甲酰-Met-Leu-Phe（MLF）三肽的极化转移动力学和化学位移依赖性进行了实验评估和数值模拟研究。这种方法的进一步应用说明了几种蛋白质：HIV-1 U-13 C，15 N CA蛋白，U-13 C，15 N富集的动力蛋白轻链DLC 8，和稀疏13 C/均匀15 N富集的CAP-Gly结构域的dynactin的球形组件。由于其优异的性能和易于实现，所提出的R2 π对称序列有望在蛋白质和蛋白质组装体以及其他有机固体的MAS NMR光谱研究中具有广泛的适用性。
We present a family of homonuclear 13C-13C magic angle spinning spin diffusion experiments, based on R2nv (n = 1 and 2, v = 1 and 2) symmetry sequences. These experiments are well suited for 13C-13C correlation spectroscopy in biological and organic systems, and are especially advantageous at very fast MAS conditions, where conventional PDSD and DARR experiments fail. At very fast MAS frequencies the R211, R221, and R222 sequences result in excellent quality correlation spectra both in model compounds and in proteins. Under these conditions, individual R2nv display different polarization transfer efficiency-dependencies on isotropic chemical shift differences: R221 recouples efficiently both small and large chemical shift differences (in proteins these correspond to aliphatic-to-aliphatic and carbonyl-to-aliphatic correlations, respectively), while R211 and R222 exhibit the maximum recoupling efficiency for the aliphatic-to-aliphatic or carbonyl-to-aliphatic correlations, respectively. At moderate MAS frequencies (10–20 kHz), all R2nv sequences introduced in this work display similar transfer efficiencies, and their performance is very similar to that of PDSD and DARR. Polarization transfer dynamics and chemical shift dependencies of these R2-driven spin diffusion (RDSD) schemes are experimentally evaluated and investigated by numerical simulations for [U-13C,15N]-alanine and the [U-13C,15N] N-formyl-Met-Leu-Phe (MLF) tripeptide. Further applications of this approach are illustrated for several proteins: spherical assemblies of HIV-1 U-13C,15N CA protein, U-13C,15N enriched dynein light chain DLC8, and sparsely 13C/uniformly 15N enriched CAP-Gly domain of dynactin. Due to the excellent performance and ease of implementation, the presented R2nv symmetry sequences are expected to be of wide applicability in studies of proteins and protein assemblies as well as other organic solids by MAS NMR spectroscopy.
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