Alston Roy W, Lasagna Mauricio, Grimsley Gerald R, Scholtz J Martin, Reinhart Gregory D, Pace C Nick
Department of Molecular and Cellular Medicine, Texas A&M University Health Science Center, Texas A&M University, College Station, Texas 77843, USA.
Biophys J. 2008 Mar 15;94(6):2280-7. doi: 10.1529/biophysj.107.116921. Epub 2007 Dec 7.
This article probes the denatured state ensemble of ribonuclease Sa (RNase Sa) using fluorescence. To interpret the results obtained with RNase Sa, it is essential that we gain a better understanding of the fluorescence properties of tryptophan (Trp) in peptides. We describe studies of N-acetyl-L-tryptophanamide (NATA), a tripeptide: AWA, and six pentapeptides: AAWAA, WVSGT, GYWHE, HEWTV, EAWQE, and DYWTG. The latter five peptides have the same sequence as those surrounding the Trp residues studied in RNase Sa. The fluorescence emission spectra, the fluorescence lifetimes, and the fluorescence quenching by acrylamide and iodide were measured in concentrated solutions of urea and guanidine hydrochloride. Excited-state electron transfer from the indole ring of Trp to the carbonyl groups of peptide bonds is thought to be the most important mechanism for intramolecular quenching of Trp fluorescence. We find the maximum fluorescence intensities vary from 49,000 for NATA with two carbonyls, to 24,400 for AWA with four carbonyls, to 28,500 for AAWAA with six carbonyls. This suggests that the four carbonyls of AWA are better able to quench Trp fluorescence than the six carbonyls of AAWAA, and this must reflect a difference in the conformations of the peptides. For the pentapeptides, EAWQE has a fluorescence intensity that is more than 50% greater than DYWTG, showing that the amino acid sequence influences the fluorescence intensity either directly through side-chain quenching and/or indirectly through an influence on the conformational ensemble of the peptides. Our results show that peptides are generally better models for the Trp residues in proteins than NATA. Finally, our results emphasize that we have much to learn about Trp fluorescence even in simple compounds.
本文利用荧光技术探究核糖核酸酶Sa(RNase Sa)的变性态系综。为了解释用RNase Sa获得的结果,我们必须更好地理解肽中色氨酸(Trp)的荧光特性。我们描述了对N - 乙酰 - L - 色氨酸酰胺(NATA)、三肽AWA以及六个五肽AAWAA、WVSGT、GYWHE、HEWTV、EAWQE和DYWTG的研究。后五个肽与RNase Sa中研究的Trp残基周围的序列相同。在尿素和盐酸胍的浓溶液中测量了荧光发射光谱、荧光寿命以及丙烯酰胺和碘化物对荧光的猝灭作用。从Trp的吲哚环到肽键羰基的激发态电子转移被认为是Trp荧光分子内猝灭的最重要机制。我们发现最大荧光强度从具有两个羰基的NATA的49000,到具有四个羰基的AWA的24400,再到具有六个羰基的AAWAA的28500不等。这表明AWA的四个羰基比AAWAA的六个羰基更能猝灭Trp荧光,这必然反映了肽构象的差异。对于五肽,EAWQE的荧光强度比DYWTG高50%以上,表明氨基酸序列要么通过侧链猝灭直接影响荧光强度,要么通过对肽构象系综的影响间接影响荧光强度。我们的结果表明,肽通常比NATA更适合作为蛋白质中Trp残基的模型。最后,我们的结果强调,即使在简单化合物中,我们对Trp荧光仍有很多需要了解的地方。