Schneck Emanuel, Scoppola Ernesto, Drnec Jakub, Mocuta Cristian, Felici Roberto, Novikov Dmitri, Fragneto Giovanna, Daillant Jean
Biomaterials Department, Max Planck Institute of Colloids and Interfaces, 14476 Potsdam, Germany; Institut Laue-Langevin, 38000 Grenoble, France;
Institut Laue-Langevin, 38000 Grenoble, France; Institut de Chimie Séparative de Marcoule UMR 5257 Commissariat à l'énergie atomique/CNRS/École Nationale Supérieure de Chimie de Montpellier, Université Montpellier, 30207 Bagnols sur Cèze, France;
Proc Natl Acad Sci U S A. 2016 Aug 23;113(34):9521-6. doi: 10.1073/pnas.1603898113. Epub 2016 Aug 8.
In nature, biomolecules are often organized as functional thin layers in interfacial architectures, the most prominent examples being biological membranes. Biomolecular layers play also important roles in context with biotechnological surfaces, for instance, when they are the result of adsorption processes. For the understanding of many biological or biotechnologically relevant phenomena, detailed structural insight into the involved biomolecular layers is required. Here, we use standing-wave X-ray fluorescence (SWXF) to localize chemical elements in solid-supported lipid and protein layers with near-Ångstrom precision. The technique complements traditional specular reflectometry experiments that merely yield the layers' global density profiles. While earlier work mostly focused on relatively heavy elements, typically metal ions, we show that it is also possible to determine the position of the comparatively light elements S and P, which are found in the most abundant classes of biomolecules and are therefore particularly important. With that, we overcome the need of artificial heavy atom labels, the main obstacle to a broader application of high-resolution SWXF in the fields of biology and soft matter. This work may thus constitute the basis for the label-free, element-specific structural investigation of complex biomolecular layers and biological surfaces.
在自然界中,生物分子常常在界面结构中组织成功能性薄层,最突出的例子就是生物膜。生物分子层在生物技术表面的相关情境中也发挥着重要作用,例如,当它们是吸附过程的产物时。为了理解许多与生物学或生物技术相关的现象,需要对所涉及的生物分子层进行详细的结构洞察。在这里,我们使用驻波X射线荧光(SWXF)以接近埃的精度定位固体支持的脂质和蛋白质层中的化学元素。该技术补充了传统的镜面反射测量实验,后者仅能得出层的整体密度分布。虽然早期的工作大多集中在相对较重的元素,通常是金属离子上,但我们表明,确定相对较轻的元素S和P的位置也是可能的,这些元素存在于最丰富的生物分子类别中,因此特别重要。由此,我们克服了对人工重原子标记的需求,这是高分辨率SWXF在生物学和软物质领域更广泛应用的主要障碍。因此,这项工作可能构成对复杂生物分子层和生物表面进行无标记、元素特异性结构研究的基础。