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Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight

机译:飞行中单个气溶胶粒子的分形形态,成像和质谱分析

摘要

The morphology of micrometre−size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X−ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub−micrometre particles to nanometre resolution in their native environment, using intense, coherent X−ray pulses from the Linac Coherent Light Source free−electron laser. We introduced individual aerosol particles into the pulsed X−ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non−equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large−scale production of nanoscale structures by flame synthesis
机译:从毒理学到气候科学,微米级颗粒物的形态至关重要,但令人惊讶的是,这些性质很难在颗粒的自然环境中测量。电子显微镜检查要求将颗粒收集在基材上。可见光散射无法提供足够的分辨率; X射线同步加速器研究仅限于粒子团。在这里,我们演示了使用直线加速器相干光源自由电子激光的强相干X射线脉冲在其自然环境中将单个亚微米级颗粒成像至纳米分辨率的原位方法。我们在脉冲X射线束中引入了单个气溶胶颗粒,其强度足够强,可以测量来自单个颗粒的衍射以进行形态分析。同时,使用质谱分析从束中射出的离子碎片,以确定单个气溶胶颗粒的组成。我们的结果表明,单个烟灰颗粒的内部膨胀对称性程度受到非平衡聚集的影响,其分形维数出人意料的大变化。更广泛地讲,我们的方法可以扩展为解析无序粒子一般合奏的静态和动态形态。这种一般的形态对诸如蛋白质中的溶剂可利用性,氨基酸的水动力相互作用引起的振动能量转移以及通过火焰合成大规模生产纳米级结构等主题具有影响。

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