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Abstract. Field-deployable real-time aerosol mass spectrometers (AMSs) typically use an aerodynamic lens as an inlet that collimates aerosols into a narrow beam over a wide range of particle sizes. Such lenses need constant upstream pressure to work consistently. Deployments in environments where the ambient pressure changes, e.g., on aircraft, typically use pressure-controlled inlets (PCIs). These have performed less well for supermicron aerosols, such as the larger particles in stratospheric air and some urban hazes. In this study, we developed and characterized a new PCI design (“CU PCI-D”) coupled with a recently developed PM2.5 aerodynamic lens, with the goal of sampling the full accumulation mode of ambient aerosols with minimal losses up to upper troposphere and lower stratosphere (UTLS) altitudes. A new computer-controlled lens alignment system and a new 2D particle beam imaging device that improves upon the Aerodyne aerosol beam width probe (BWP) have been developed and tested. These techniques allow for fast automated aerosol beam width and position measurements and ensure the aerodynamic lens is properly aligned and characterized for accurate quantification, in particular for small sizes that are hard to access with monodisperse measurements. The automated lens alignment tool also allows position-dependent thermal decomposition to be investigated on the vaporizer surface. The CU PCI-D was tested on the TI3GER campaign aboard the NCAR/NSF G-V aircraft. Based on comparisons with the co-sampling UHSAS particle sizer, the CU aircraft AMS with the modified PCI consistently measured ∼ 89 % of the accumulation-mode particle mass in the UTLS. 

This study introduces an atmospheric pressure chemical ionization method that relies on low-energy thermal collisions (i.e., <0.05 eV) of aerosolized analytes with bipolar ions pre-seeded in a sample dilution flow and allows for the detection of weakly bound molecular clusters. Herein, the potential of the method is explored in the context of soot inception by performing mass spectrometric analysis of a laminar premixed flame of ethylene and air whose products are sampled through a tiny orifice and quickly diluted in nitrogen pre-flowed through a Kr85 based neutralizer to generate the bipolar ions. Analyses were performed with an Atmospheric Pressure Interface Time-of-Flight (APi-TOF, Tofwerk AG) Mass Spectrometer whose high sensitivity, mass accuracy, and resolution (over 4000) allowed for the discrimination of the flame products from the pre-seeded ions. Since ionization of neutrals occurs by either ion attachment or charge exchange following ion collision, the identification of the origin of each peak in the measured mass spectra is not-trivial. Nevertheless, the results provide valuable information on the overall elemental composition of the neutral flame products ionized in either polarity. Results show that the clustering of hydrocarbons lighter than 400 Da and having a C/H ratio between 2 and 3 leads to soot inception in the flame. The dehydrogenation of the flame products, expected to occur as they are convected in the flame, is observed only for measurements in positive polarity because of a higher probability of soot nuclei and precursors to get a positive rather than a negative charge. 

Glass transitions from liquid to semi-solid and solid phase states have important implications for reactivity, growth, and cloud-forming (cloud condensation nuclei and ice nucleation) capabilities of secondary organic aerosols (SOAs). The small size and relatively low mass concentration of SOAs in the atmosphere make it difficult to measure atmospheric SOA glass transitions using conventional methods. To circumvent these difficulties, we have adapted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols. Aerosol particles to be studied are deposited in the form of a thin film onto an interdigitated electrode (IDE) using electrostatic precipitation. Dielectric spectroscopy provides dipole relaxation rates for organic aerosols as a function of temperature (373 to 233 K) that are used to calculate the glass transition temperatures for several cooling or heating rates. IDE-enabled broadband dielectric spectroscopy (BDS) was successfully used to measure the kinetically controlled glass transition temperatures of aerosols consisting of glycerol and four other compounds with selected cooling and heating rates. The glass transition results agree well with available literature data for these five compounds. The results indicate that the IDE-BDS method can provide accurate glass transition data for organic aerosols under atmospheric conditions. The BDS data obtained with the IDE-BDS technique can be used to characterize glass transitions for both simulated and ambient organic aerosols and to model their climate effects.