Pumped Counterflow Virtual Impactor Research Articles

A phase separation inlet for droplets, ice residuals, and interstitial aerosol particles

Abstract. A new inlet for studying the aerosol particles and hydrometeor residuals that compose mixed-phase clouds – the phaSe seParation Inlet for Droplets icE residuals and inteRstitial aerosol particles (SPIDER) – is described here. SPIDER combines a large pumped counterflow virtual impactor (L-PCVI), a flow tube evaporation chamber, and a pumped counterflow virtual impactor (PCVI) to separate droplets, ice crystals (∼3–25 µm), and interstitial aerosol particles for simultaneous sampling. Laboratory verification tests of each individual component and the composite SPIDER system were conducted. Transmission efficiency, evaporation, and ice crystals' survival were determined to show the capability of the system. The experiments show the SPIDER system can separate distinct cloud elements and interstitial aerosol particles for subsequent analysis. As a field instrument, SPIDER will help explore the properties of different cloud elements and interstitial aerosol particles in mixed-phase clouds.

Direct Online Mass Spectrometry Measurements of Ice Nucleating Particles at a California Coastal Site

AbstractThe formation of ice in clouds can strongly impact cloud properties and precipitation processes during storms, including atmospheric rivers. Sea spray aerosol (SSA) particles are relatively inefficient as ice nucleating particles (INPs) compared to mineral dust. However, due to the vast coverage of the Earth's surface by the oceans, a number of recent studies have focused on identifying sources of marine INPs, particularly in regions lacking a strong influence from dust. This study describes the integration, validation, and application of a system coupling a continuous flow diffusion chamber with a single particle mass spectrometer using a pumped counterflow virtual impactor to remove nonnucleated particles and selectively measure the composition of INPs with a detection efficiency of 3.10 × 10−4. In situ measurements of immersion freezing INP composition were made at a coastal site in California using the integrated system. Mineral dust particles were the most abundant ice crystal residual type during the sampling period and found to be ice active despite having undergone atmospheric processing. SSA were more abundant in ambient measurements but represented only a minor fraction of the ice crystal residual population at −31 °C. Notably, the SSA particles that activated were enriched with organic nitrogen species that were likely transferred from the ocean. Calculations of ice nucleation active site densities were within good agreement with previous studies of mineral dust and SSA.

Activation of intact bacteria and bacterial fragments mixed with agar as cloud droplets and ice crystals in cloud chamber experiments

Abstract. Biological particles, including bacteria and bacterial fragments, have been of much interest due to the special ability of some to nucleate ice at modestly supercooled temperatures. This paper presents results from a recent study conducted on two strains of cultivated bacteria which suggest that bacterial fragments mixed with agar, and not whole bacterial cells, serve as cloud condensation nuclei (CCN). Due to the absence of whole bacteria cells in droplets, they are unable to serve as ice nucleating particles (INPs) in the immersion mode under the experimental conditions. Experiments were conducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber at the Karlsruhe Institute of Technology (KIT) by injecting bacteria-containing aerosol samples into the cloud chamber and inducing cloud formation by expansion over a temperature range of −5 to −12 ∘C. Cloud droplets and ice crystals were sampled through a pumped counterflow virtual impactor inlet (PCVI) and their residuals were characterized with a single particle mass spectrometer (miniSPLAT). The size distribution of the overall aerosol was bimodal, with a large particle mode composed of intact bacteria and a mode of smaller particles composed of bacterial fragments mixed with agar that were present in higher concentrations. Results from three expansions with two bacterial strains indicate that the cloud droplet residuals had virtually the same size distribution as the smaller particle size mode and had mass spectra that closely matched those of bacterial fragments mixed with agar. The characterization of ice residuals that were sampled through an ice-selecting PCVI (IS-PCVI) also shows that the same particles that activate to form cloud droplets, bacteria fragments mixed with agar, were the only particle type observed in ice residuals. These results indicate that the unavoidable presence of agar or other growth media in all laboratory studies conducted on cultivated bacteria can greatly affect the results and needs to be considered when interpreting CCN and IN activation data.

Development and characterization of an ice-selecting pumped counterflow virtual impactor (IS-PCVI) to study ice crystal residuals

Abstract. Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters (< 5 µm). Here, for the first time we describe a development of an ice-selecting PCVI (IS-PCVI) to separate ice in controlled mixed-phase cloud system based on the particle inertia with the cut-off diameter ≥ 10 µm. We also present its laboratory application demonstrating the use of the impactor under a wide range of temperature and humidity conditions. The computational fluid dynamics simulations were initially carried out to guide the design of the IS-PCVI. After fabrication, a series of validation laboratory experiments were performed coupled with the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) expansion cloud simulation chamber. In the AIDA chamber, test aerosol particles were exposed to the ice supersaturation conditions (i.e., RHice > 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter ≥ 10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of ~ 10–30 µm in diameter with small inadvertent intrusion (~ 5 %) of unwanted particles.

The Ice Selective Inlet: a novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds

Abstract. Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals.

Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques

Abstract. In the present work, three different techniques to separate ice-nucleating particles (INPs) as well as ice particle residuals (IPRs) from non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed-phase clouds and allow after evaporation in the instrument for the analysis of the residuals. The Fast Ice Nucleus Chamber (FINCH) coupled with the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated particles for analysis. The instruments were run during a joint field campaign which took place in January and February 2013 at the High Alpine Research Station Jungfraujoch (Switzerland). INPs and IPRs were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. Online analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPR separation techniques high abundances (median 20–70%) of instrumental contamination artifacts were observed (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH + IN-PCVI: steel particles). After removal of the instrumental contamination particles, silicates, Ca-rich particles, carbonaceous material and metal oxides were the major INP/IPR particle types obtained by all three techniques. In addition, considerable amounts (median abundance mostly a few percent) of soluble material (e.g., sea salt, sulfates) were observed. As these soluble particles are often not expected to act as INP/IPR, we consider them as potential measurement artifacts. Minor types of INP/IPR include soot and Pb-bearing particles. The Pb-bearing particles are mainly present as an internal mixture with other particle types. Most samples showed a maximum of the INP/IPR size distribution at 200–400 nm in geometric diameter. In a few cases, a second supermicron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the sub-micrometer range. Silicates and Ca-rich particles were mainly found with diameters above 1 μm (using ISI and FINCH), in contrast to the Ice-CVI which also sampled many submicron particles of both groups. Due to changing meteorological conditions, the INP/IPR composition was highly variable if different samples were compared. Thus, the observed discrepancies between the different separation techniques may partly result from the non-parallel sampling. The differences of the particle group relative number abundance as well as the mixing state of INP/IPR clearly demonstrate the need of further studies to better understand the influence of the separation techniques on the INP/IPR chemical composition. Also, it must be concluded that the abundance of contamination artifacts in the separated INP and IPR is generally large and should be corrected for, emphasizing the need for the accompanying chemical measurements. Thus, further work is needed to allow for routine operation of the three separation techniques investigated.

Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach

In this study chemical compositions of background aerosol and ice nuclei were examined through laboratory investigations using Raman spectroscopy and field measurements by single‐particle mass spectrometry. Aerosol sampling took place at Storm Peak Laboratory in Steamboat Springs, Colorado (elevation of 3210 m). A cascade impactor was used to collect coarse‐mode aerosol particles for laboratory analysis by Raman spectroscopy; the composition, mixing state, and heterogeneous ice nucleation activity of individual particles were examined. For in situ analysis of fine‐mode aerosol, ice nucleation on ambient particles was observed using a compact ice nucleation chamber. Ice crystals were separated from unactivated aerosol using a pumped counterflow virtual impactor, and ice nuclei were analyzed using particle analysis by laser mass spectrometry. For both fine and coarse modes, the ice nucleating particle fractions were enriched in minerals and depleted in sulfates and nitrates, compared to the background aerosol sampled. The vast majority of particles in both the ambient and ice active aerosol fractions contained a detectable amount of organic material. Raman spectroscopy showed that organic material is sometimes present in the form of a coating on the surface of inorganic particles. We find that some organic‐containing particles serve as efficient ice nuclei while others do not. For coarse‐mode aerosol, organic particles were only observed to initiate ice formation when oxygen signatures were also present in their spectra.

Combustion particles as ice nuclei in an urban environment: Evidence from single-particle mass spectrometry

This paper presents measurements of the single-particle composition of ice nuclei (IN) in downtown Toronto, Canada, made at 239 ± 1 K, 134 ± 2% relative humidity with respect to ice (RHi). IN were activated within the University of Toronto Continuous-Flow Diffusion Chamber (UT-CFDC), separated from background aerosol using a pumped counterflow virtual impactor (PCVI), and analyzed using a dual-polarity single-particle mass spectrometer (ATOFMS). To account for particles leaked by the PCVI, the ratio of particles observed at high RHi to low RHi was calculated. This ratio was greater than unity for EC (elemental carbon), BB (biomass burning) and dust particles, however only the increase in EC was statistically significant (1σ level) due to a low number of detected particles. The remaining particle categories were: metal-rich organic carbon (M/OC), potassium-rich OC (K/OC), OC potentially mixed with EC (OC/EC) and “other”, none of which were enhanced in number at high RHi. To complement the direct PCVI observations and enhance the number of spectra available, a second study was performed where particle composition and IN concentrations (CIN) were measured in parallel. IN concentrations were regressed against the same categories as above, and dust, BB and EC particles were identified as the best predictors of CIN. Consistency between these two methods provides increased confidence in their individual results and encourages additional study of these potential IN.

Studies of propane flame soot acting as heterogeneous ice nuclei in conjunction with single particle soot photometer measurements

Abstract. The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies). The organic carbon content (OC) of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI) to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2) to examine the mixing state of the BC containing ice residuals. Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content) where deposition freezing occurred at an ice saturation ratio Sice ~ 1.22 at a temperature T = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content) showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments) than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating. The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the onset of freezing occurred at colder temperatures and required a greater ice saturation ratio; for the medium and maximum OC flame soot, the addition of a sulphuric acid significantly reduced the freezing threshold.

Analysis of cloud condensation nuclei composition and growth kinetics using a pumped counterflow virtual impactor and aerosol mass spectrometer

Abstract. We present a new method of determining the size and composition of CCN-active aerosol particles. Method utility is illustrated through a series of ambient measurements. A continuous-flow thermal-gradient diffusion chamber (TGDC), pumped counterflow virtual impactor (PCVI), and Aerodyne time-of-flight mass spectrometer (AMS) are operated in series. Ambient particles are sampled into the TGDC, where a constant supersaturation is maintained, and CCN-active particles grow to ~2.5 ± 0.5 μm. The output flow from the TGDC is directed into the PCVI, where a counterflow of dry N2 gas opposes the particle-laden flow, creating a region of zero axial velocity. This stagnation plane can only be traversed by particles with sufficient momentum, which depends on their size. Particles that have activated in the TGDC cross the stagnation plane and are entrained in the PCVI output flow, while the unactivated particles are diverted to a pump. Because the input gas is replaced by the counterflow gas with better than 99 % efficiency at the stagnation plane, the output flow consists almost entirely of dry N2 and water evaporates from the activated particles. In this way, the system yields an ensemble of CCN-active particles whose chemical composition and size are analyzed using the AMS. Measurements of urban aerosol in downtown Toronto identified an external mixture of CCN-active particles consisting almost entirely of ammonium nitrate and ammonium sulfate, with CCN-inactive particles of the same size consisting of a mixture of ammonium nitrate, ammonium sulfate, and organics. We also discuss results from the first field deployment of the TGDC-PCVI-AMS system, conducted from mid-May to mid-June 2007 in Egbert, Ontario, a semirural site ~80 km north of Toronto influenced both by clean air masses from the north and emissions from the city. Organic-dominated particles sampled during a major biogenic event exhibited higher CCN activity and/or faster growth kinetics than urban outflow from Toronto, despite the latter having a higher inorganic content and higher O:C ratio. During both events, particles were largely internally mixed.

Comparison of Experimental and Numerical Studies of the Performance Characteristics of a Pumped Counterflow Virtual Impactor

Experiments and Computational Fluid Dynamic (CFD) simulations were performed to evaluate the performance characteristics of a Pumped Counterflow Virtual Impactor (PCVI). The diameter at which 50% of the particles were transmitted was determined for various flow configurations. Experimentally determined 50% cut sizes varied from 2.2 to 4.8 micrometers and CFD predicted diameters agreed within ±0.4 micrometers. Both experimental and CFD results showed similar transmission efficiency (TE) curves. CFD TE was always greater than experimental results, most likely due to impaction losses in fittings not included in the simulations. Ideal transmission, corresponding to 100% TE, was never realized in either case due to impaction losses and small-scale flow features such as eddies. Areas where CFD simulations showed such flow recirculation zones were also found to be the locations where particulate residue was deposited during experiments. CFD parametric tests showed that PCVI performance can be affected by the nozzle geometry and misalignment between the nozzle and collector orifice. We conclude that CFD can be used with confidence for counterflow virtual impactor (CVI) design. Modifications to improve the performance characteristics of the PCVI are suggested.

Single Particle Laser Mass Spectrometry Applied to Differential Ice Nucleation Experiments at the AIDA Chamber

Experiments conducted at the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) chamber located in Karlsruhe, Germany permit investigation of particle properties that affect the nucleation of ice at temperature and water vapor conditions relevant to cloud microphysics and climate issues. Ice clouds were generated by heterogeneous nucleation of Arizona test dust (ATD), illite, and hematite and homogeneous nucleation of sulfuric acid. Ice crystals formed in the chamber were inertially separated from unactivated, or “interstitial” aerosol particles with a pumped counterflow virtual impactor (PCVI), then evaporated. The ice residue (i.e., the aerosol which initiated ice nucleation plus any material which was scavenged from the gas- and/or particle-phase), was chemically characterized at the single particle level using a laser ionization mass spectrometer. In this manner the species that first nucleated ice could be identified out of a mixed aerosol population in the chamber. Bare mineral dust particle...

Design and Performance of a Pumped Counterflow Virtual Impactor

Counterflow virtual impaction uses a flow of gas in a direction opposite the motion of the particles to separate them from gas and smaller particles. In the past such devices have used aircraft flight or wind tunnel flow to impart momentum to the particles. Here we describe the design and performance of an apparatus, termed a pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to provide the flow. We show that this device is capable of inertial separation with a sub-micrometer cutoff diameter, particle enhancement approaching the ratio of the output to the input flow, and replacement of the ambient gas in the output flow with another gas that may be more suitable for downstream analysis techniques. Rejection of input gas and particles smaller than the cutoff diameter can exceed 99.9%.