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

被引:158
作者
Loh, N. D. [1 ]
Hampton, C. Y. [1 ]
Martin, A. V. [2 ]
Starodub, D. [1 ]
Sierra, R. G. [1 ]
Barty, A. [2 ]
Aquila, A. [2 ,3 ]
Schulz, J. [2 ,3 ]
Lomb, L. [4 ]
Steinbrener, J. [4 ]
Shoeman, R. L. [4 ]
Kassemeyer, S. [4 ]
Bostedt, C. [5 ]
Bozek, J. [5 ]
Epp, S. W. [6 ,7 ]
Erk, B. [6 ,7 ]
Hartmann, R. [8 ]
Rolles, D. [4 ,6 ]
Rudenko, A. [6 ,7 ]
Rudek, B. [6 ,7 ]
Foucar, L. [4 ,6 ]
Kimmel, N. [9 ,10 ]
Weidenspointner, G. [9 ,10 ]
Hauser, G. [9 ,10 ]
Holl, P. [8 ]
Pedersoli, E. [11 ]
Liang, M. [2 ]
Hunter, M. M. [12 ]
Gumprecht, L. [2 ]
Coppola, N. [3 ]
Wunderer, C. [13 ]
Graafsma, H. [13 ]
Maia, F. R. N. C. [14 ]
Ekeberg, T. [15 ]
Hantke, M. [15 ]
Fleckenstein, H. [2 ]
Hirsemann, H. [13 ]
Nass, K. [2 ,16 ]
White, T. A. [2 ]
Tobias, H. J. [17 ]
Farquar, G. R. [12 ]
Benner, W. H. [12 ]
Hau-Riege, S. P. [12 ]
Reich, C. [8 ]
Hartmann, A. [8 ]
Soltau, H. [8 ]
Marchesini, S. [18 ]
Bajt, S. [13 ]
Barthelmess, M. [13 ]
Bucksbaum, P. [1 ]
机构
[1] PULSE Inst, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA
[2] DESY, Ctr Free Electron Laser Sci, D-22607 Hamburg, Germany
[3] European XFEL GmbH, D-22761 Hamburg, Germany
[4] Max Planck Inst Med Res, D-69120 Heidelberg, Germany
[5] SLAC Natl Accelerator Lab, LCLS, Menlo Pk, CA 94025 USA
[6] Ctr Free Electron Laser Sci CFEL, Max Planck Adv Study Grp, D-22607 Hamburg, Germany
[7] Max Planck Inst Kernphys, D-69117 Heidelberg, Germany
[8] PNSensor GmbH, D-81739 Munich, Germany
[9] Max Planck Inst Halbleiterlab, D-81739 Munich, Germany
[10] Max Planck Inst Extraterr Phys, D-85741 Garching, Germany
[11] Sincrotrone Trieste, Microscopy Sect, I-34149 Trieste, Italy
[12] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA
[13] DESY, Photon Sci, D-22607 Hamburg, Germany
[14] Natl Energy Res Sci Comp Ctr NERSC, Berkeley, CA 94720 USA
[15] Uppsala Univ, Dept Cell & Mol Biol, Lab Mol Biophys, SE-75124 Uppsala, Sweden
[16] Univ Hamburg, D-22761 Hamburg, Germany
[17] Cornell Univ, Div Nutr Sci, Ithaca, NY 14853 USA
[18] Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA
基金
欧洲研究理事会; 瑞典研究理事会;
关键词
FREE-ELECTRON LASER; OPTICAL-PROPERTIES; SOOT AEROSOLS; BLACK CARBON; MIXING STATE; SCATTERING; CLIMATE; FLAME;
D O I
10.1038/nature11222
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology(1) to climate science(2), yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate(3); visible light scattering provides insufficient resolution(4); and X-ray synchrotron studies have been limited to ensembles of particles(5). 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(6) 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(7), vibrational energy transfer by the hydrodynamic interaction of amino acids(8), and large-scale production of nanoscale structures by flame synthesis(9).
引用
收藏
页码:513 / 517
页数:5
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