MIMiX: A Multipurpose In-situ Microreactor system for X-ray microspectroscopy to mimic atmospheric aerosol processing

The dynamic processing of aerosols in the atmosphere is difficult to mimic under laboratory conditions, particularly on a single-particle level with high spatial and chemical resolution. Our new microreactor system for Xray microscopy facilitates observations under in situ conditions and extends the accessible parameter ranges of existing setups to very high humidities and low temperatures. With the parameter margins for pressure (180–1000 hPa), temperature (∼ 250 K to room temperature), and relative humidity (∼ 0 % to above 98 %), a wide range of tropospheric conditions is covered. Unique features are the mobile design and compact size that make the instrument applicable to different synchrotron facilities. Successful first experiments were conducted at two X-ray microscopes, MAXYMUS, located at beamline UE46 of the synchrotron BESSY II, and PolLux, located at beamline X07DA of the Swiss Light Source in the Paul Scherrer Institute. Here we present the design and analytical scope of the system, along with first results from hydration–dehydration experiments on ammonium sulfate and potassium sulfate particles and the tentative observation of water ice at low temperature and high relative humidity in a secondary organic aerosol particle from isoprene oxidation.

[1]  C. Pöhlker,et al.  Visualizing reaction and diffusion in xanthan gum aerosol particles exposed to ozone. , 2019, Physical chemistry chemical physics : PCCP.

[2]  M. Ammann,et al.  Pre-melting and the adsorption of formic acid at the air-ice interface at 253 K as seen by NEXAFS and XPS. , 2018, Physical chemistry chemical physics : PCCP.

[3]  M. Ammann,et al.  Experimental Evidence for the Formation of Solvation Shells by Soluble Species at a Nonuniform Air–Ice Interface , 2017 .

[4]  M. Andreae,et al.  Tandem configuration of differential mobility and centrifugal particle mass analysers for investigating aerosol hygroscopic properties , 2016 .

[5]  A. Laskin,et al.  Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization , 2015 .

[6]  U. Pöschl,et al.  Multiphase chemistry at the atmosphere-biosphere interface influencing climate and public health in the anthropocene. , 2015, Chemical reviews.

[7]  D. Worsnop,et al.  Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield , 2015 .

[8]  U. Pöschl,et al.  Competition between water uptake and ice nucleation by glassy organic aerosol particles , 2014 .

[9]  Stefan M. Wild,et al.  Non-negative matrix analysis for effective feature extraction in X-ray spectromicroscopy. , 2014, Faraday discussions.

[10]  E. Coz,et al.  The influence of physical state on shikimic acid ozonolysis: a case for in situ microspectroscopy , 2014 .

[11]  Chris Jacobsen,et al.  MANTiS: a program for the analysis of X-ray spectromicroscopy data. , 2014, Journal of synchrotron radiation.

[12]  T. Tyliszczak,et al.  Comparison of x-ray absorption spectra between water and ice: new ice data with low pre-edge absorption cross-section. , 2014, The Journal of chemical physics.

[13]  M. Andreae,et al.  Efflorescence upon humidification? X‐ray microspectroscopic in situ observation of changes in aerosol microstructure and phase state upon hydration , 2014 .

[14]  Douglas Sparks,et al.  Output Drifting of Vacuum Packaged MEMS Sensors Due to Room Temperature Helium Exposure , 2013 .

[15]  T. Tyliszczak,et al.  An environmental sample chamber for reliable scanning transmission x-ray microscopy measurements under water vapor. , 2013, The Review of scientific instruments.

[16]  J. Seinfeld,et al.  Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology. , 2013, Physical chemistry chemical physics : PCCP.

[17]  Similarities in STXM-NEXAFS Spectra of Atmospheric Particles and Secondary Organic Aerosol Generated from Glyoxal, α-Pinene, Isoprene, 1,2,4-Trimethylbenzene, and d-Limonene , 2013 .

[18]  Corinna Hoose,et al.  Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments , 2012 .

[19]  Claudia Marcolli,et al.  Exploring the complexity of aerosol particle properties and processes using single particle techniques. , 2012, Chemical Society reviews.

[20]  D. Worsnop,et al.  Chemistry and composition of atmospheric aerosol particles. , 2012, Annual review of physical chemistry.

[21]  U. Baltensperger,et al.  Aging induced changes on NEXAFS fingerprints in individual combustion particles , 2011 .

[22]  Ulrich Pöschl,et al.  Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere. , 2011, Physical chemistry chemical physics : PCCP.

[23]  G. Schütz,et al.  High Contrast Magnetic and Nonmagnetic Sample Current Microscopy for Bulk and Transparent Samples Using Soft X-Rays , 2011, Microscopy and Microanalysis.

[24]  Y. Rudich,et al.  Humidity driven nanoscale chemical separation in complex organic matter , 2011 .

[25]  A. Tivanski,et al.  Scanning Transmission X-ray Microscopy: Applications in Atmospheric Aerosol Research , 2011 .

[26]  G. Tzvetkov,et al.  Direct observation of water uptake and release in individual submicrometer sized ammonium sulfate and ammonium sulfate/adipic acid particles using X-ray microspectroscopy , 2011 .

[27]  D. Worsnop,et al.  Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements , 2010 .

[28]  G. Tzvetkov,et al.  An in situ cell to study phase transitions in individual aerosol particles on a substrate using scanning transmission x-ray microspectroscopy. , 2010, The Review of scientific instruments.

[29]  A. Tivanski,et al.  Hygroscopic behavior of individual submicrometer particles studied by X-ray spectromicroscopy. , 2010, Analytical chemistry.

[30]  U. Frommherz,et al.  Higher Order Suppressor (HOS) for the PolLux microspectroscope beamline at the Swiss Light Source SLS , 2010 .

[31]  Markus A. Weigand,et al.  The X-ray microscopy beamline UE46-PGM2 at BESSY , 2010 .

[32]  P. Wernet,et al.  X-ray absorption spectroscopy and X-ray Raman scattering of water and ice; an experimental view , 2010 .

[33]  U. Pöschl,et al.  Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations , 2009 .

[34]  S. Martin,et al.  Deliquescence and Efflorescence of Potassium Salts Relevant to Biomass-Burning Aerosol Particles , 2009 .

[35]  N. Sewald,et al.  Ice recrystallization kinetics in the presence of synthetic antifreeze glycoprotein analogues using the framework of LSW theory. , 2009, The journal of physical chemistry. B.

[36]  A. Wexler,et al.  Thermodynamic Model of the System H , 2009 .

[37]  T. Tyliszczak,et al.  PolLux: a new facility for soft x-ray spectromicroscopy at the Swiss Light Source. , 2008, The Review of scientific instruments.

[38]  J. F. Creemer,et al.  Nanoscale chemical imaging of a working catalyst by scanning transmission X-ray microscopy , 2008, Nature.

[39]  Meinrat O. Andreae,et al.  Aerosol cloud precipitation interactions. Part 1. The nature and sources of cloud-active aerosols , 2008 .

[40]  Jonathan P. Reid,et al.  Optical manipulation and characterisation of aerosol particles using a single-beam gradient force optical trap. , 2008, Chemical Society reviews.

[41]  T. Tyliszczak,et al.  Chemical speciation of sulfur in marine cloud droplets and particles: Analysis of individual particles from the marine boundary layer over the California current , 2008 .

[42]  D. Toohey,et al.  under a Creative Commons License. Atmospheric Chemistry and Physics Introducing the concept of Potential Aerosol Mass (PAM) , 2007 .

[43]  H. Ade,et al.  The PolLux Microspectroscopy Beam line at the Swiss Light Source , 2007 .

[44]  Ulrich Pöschl,et al.  Atmospheric aerosols: composition, transformation, climate and health effects. , 2005, Angewandte Chemie.

[45]  Jörg Maser,et al.  Cluster analysis in soft X-ray spectromicroscopy : Finding the patterns in complex specimens , 2005 .

[46]  T. Tyliszczak,et al.  An in-situ cell for characterization of solids by soft X-ray absorption , 2004 .

[47]  M Lerotic,et al.  Cluster analysis of soft X-ray spectromicroscopy data. , 2003, Ultramicroscopy.

[48]  S. Kreidenweis,et al.  Predicting Particle Critical Supersaturation from Hygroscopic Growth Measurements in the Humidified TDMA. Part I: Theory and Sensitivity Studies , 2000 .

[49]  S. Kreidenweis,et al.  Predicting Particle Critical Supersaturation from Hygroscopic Growth Measurements in the Humidified TDMA. Part II: Laboratory and Ambient Studies , 2000 .

[50]  A. Coustenis,et al.  Chemistry and Composition , 1999 .

[51]  P. Sopp Cluster analysis. , 1996, Veterinary immunology and immunopathology.

[52]  K. H. Fung,et al.  Phase transformation and metastability of hygroscopic microparticles , 1995 .

[53]  I. Tang,et al.  Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance , 1994 .

[54]  I. Tang,et al.  Composition and temperature dependence of the deliquescence properties of hygroscopic aerosols , 1993 .

[55]  J. Seinfeld,et al.  Studies of concentrated electrolyte solutions using the electrodynamic balance. 3. Solute nucleation , 1987 .

[56]  J. Seinfeld,et al.  Studies of concentrated electrolyte solutions using the electrodynamic balance. 1. Water activities for single-electrolyte solutions , 1987 .

[57]  L. Greenspan Humidity Fixed Points of Binary Saturated Aqueous Solutions , 1977, Journal of Research of the National Bureau of Standards. Section A, Physics and Chemistry.