Thermal Gradient Cloud Condensation Nuclei Research Articles

Exploring CCN droplet suppression with a higher sensitivity optical particle counter

ABSTRACTThe continuous flow thermal gradient cloud condensation nuclei counter (CCNc) is the instrument currently widely used in exploring the interactions of aerosol with water vapor in the supersaturated regime. In this study we use a CCNc with an optical particle counter (OPC) modified to twice the sensitivity of the default OPC on the standard CCNc built by DMT, Inc. The standard OPC and the modified OPC-β are used to explore the droplet growth of inorganic and organic salts and the effects of cloud condensation nuclei concentrations on the final droplet sizes. We also couple the higher sensitivity OPC-β with the continuous flow streamwise thermal gradient CCNc (CFSTGC) model to estimate the mass accommodation coefficient, α. For inorganic and organic aerosol, a mass accommodation coefficient, α >> 0.2 will yield modeled droplet diameters consistent with experimental and ambient observations. However, using higher sensitivity CCN data, the final droplet diameters of CCN appear independent of aerosol h...

Cloud condensation nuclei (CCN) activity of aliphatic amine secondary aerosol

Abstract. Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g., hydroxyl radical and nitrate radical). The particle can contain both secondary organic aerosol (SOA) and inorganic salts. The ratio of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ, ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3) contains less volatile compounds than the primary aliphatic amine (BA) aerosol. As relative humidity (RH) increases, inorganic amine salts are formed as a result of acid–base reactions. The CCN activity of the humid TMA–N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. The humid BA + N2O5 aerosol products were found to be very sensitive to the temperature at which the measurements were made within the streamwise continuous-flow thermal gradient CCN counter; κ ranges from 0.4 to 0.7 dependent on the instrument supersaturation (ss) settings. The variance of the measured aerosol κ values indicates that simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems' κ ranges within 0.2 < κ < 0.7. This work indicates that aerosols formed via nighttime reactions with amines are likely to produce hygroscopic and volatile aerosol, whereas photochemical reactions with OH produce secondary organic aerosol of lower CCN activity. The contributions of semivolatile secondary organic and inorganic material from aliphatic amines must be considered for accurate hygroscopicity and CCN predictions from aliphatic amine systems.

Aircraft Measurements of Atmospheric Aerosol over North China in Autumn

Using an aircraft equipped with Passive Cavity Aerosol Spectrum Probe (PCASP-100X) and streamwise thermal gradient cloud condensation nuclei (CCN) counter, six flight measurements of atmospheric aerosol and CCN were conducted over North China in autumn. Five flight observations over Shijiazhuang urban area show that there is great difference of aerosol microphysical character between clear day and haze day. Vertical distributions show that aerosols mainly concentrated on the levels from near surface to the low level of troposphere and the concentration generally decreased with height increasing. The max aerosol concentration was 8110 cm-3on haze day and 1614 cm-3on clear day. There was more than 4 times difference in concentration of aerosol in boundary layer between haze day and clear day. CCN has the similar vertical distributions as aerosol. Most CCN concentrated on the boundary layer suggesting that the main source of CCN is from surface. Observation over Bohai Bay shows that the marine aerosol and CCN were greatly influenced by anthropogenic emissions.

Comparison of Approaches for Measuring the Mass Accommodation Coefficient for the Condensation of Water and Sensitivities to Uncertainties in Thermophysical Properties

We compare and contrast measurements of the mass accommodation coefficient of water on a water surface made using ensemble and single particle techniques under conditions of supersaturation and subsaturation, respectively. In particular, we consider measurements made using an expansion chamber, a continuous flow streamwise thermal gradient cloud condensation nuclei chamber, the Leipzig Aerosol Cloud Interaction Simulator, aerosol optical tweezers, and electrodynamic balances. Although this assessment is not intended to be comprehensive, these five techniques are complementary in their approach and give values that span the range from near 0.1 to 1.0 for the mass accommodation coefficient. We use the same semianalytical treatment to assess the sensitivities of the measurements made by the various techniques to thermophysical quantities (diffusion constants, thermal conductivities, saturation pressure of water, latent heat, and solution density) and experimental parameters (saturation value and temperature). This represents the first effort to assess and compare measurements made by different techniques to attempt to reduce the uncertainty in the value of the mass accommodation coefficient. Broadly, we show that the measurements are consistent within the uncertainties inherent to the thermophysical and experimental parameters and that the value of the mass accommodation coefficient should be considered to be larger than 0.5. Accurate control and measurement of the saturation ratio is shown to be critical for a successful investigation of the surface transport kinetics during condensation/evaporation. This invariably requires accurate knowledge of the partial pressure of water, the system temperature, the droplet curvature and the saturation pressure of water. Further, the importance of including and quantifying the transport of heat in interpreting droplet measurements is highlighted; the particular issues associated with interpreting measurements of condensation/evaporation rates with varying pressure are discussed, measurements that are important for resolving the relative importance of gas diffusional transport and surface kinetics.

Aerosol hygroscopicity and CCN activation kinetics in a boreal forest environment during the 2007 EUCAARI campaign

Abstract. Measurements of size-resolved cloud condensation nuclei (CCN) concentrations, subsaturated hygroscopic growth, size distribution, and chemical composition were collected from March through May, 2007, in the remote Boreal forests of Hyytiälä, Finland, as part of the European Integrated project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaign. Hygroscopicity parameter, κ, distributions were derived independently from Continuous Flow-Streamwise Thermal Gradient CCN Chamber (CFSTGC) and Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) measurements. CFSTGC-derived κ values for 40, 60, and 80 nm particles range mostly between 0.10 and 0.40 with an average characteristic of highly oxidized organics of 0.20 ± 0.10, indicating that organics play a dominant role for this environment. HTDMA-derived κ were generally 30% lower. Diurnal trends of κ show a minimum at sunrise and a maximum in the late afternoon; this trend covaries with inorganic mass fraction and the m/z 44 organic mass fraction given by a quadrupole aerosol mass spectrometer, further illustrating the importance of organics in aerosol hygroscopicity. The chemical dispersion inferred from the observed κ distributions indicates that while 60 and 80 nm dispersion increases around midday, 40 nm dispersion remains constant. Additionally, 80 nm particles show a markedly higher level of chemical dispersion than both 40 and 60 nm particles. An analysis of droplet activation kinetics for the sizes considered indicates that most of the CCN activate as rapidly as (NH4)2SO4 calibration aerosol.

Development of a cloud condensation nuclei (CCN) counter using a laser and charge-coupled device (CCD) camera

A continuous flow streamwise thermal gradient cloud condensation nuclei (CCN) counter with an aerosol focusing and a laser-charge-coupled device (CCD) camera detector system was developed here. The counting performance of the laser-CCD camera detector system was evaluated by comparing its measured number concentrations with those measured with a condensation particle counter (CPC) using polystyrene latex (PSL) and NaCl particles of varying sizes. The CCD camera parameters (e.g. brightness, gain, gamma, and exposure time) were optimized to detect moving particles in the sensing volume and to provide the best image to count them. The CCN counter worked well in the particle number concentration range of 0.6–8000 #·cm−3 and the minimum detectable size was found to be 0.5 μm. The supersaturation in the CCN counter with varying temperature difference was determined by using size-selected sodium chloride particles based on Kohler equation. The developed CCN counter was applied to investigate CCN activity of atmospheric ultrafine particles at 0.5% supersaturation. Data showed that CCN activity increased with increasing particle size and that the higher CCN activation for ultrafine particles occurred in the afternoon, suggesting the significant existence of hygroscopic or soluble species in photochemically-produced ultrafine particles.

Cloud condensation nuclei activity of isoprene secondary organic aerosol

[1] This work explores the cloud condensation nuclei (CCN) activity of isoprene secondary organic aerosol (SOA), likely a significant source of global organic particulate matter and CCN, produced from the oxidation with OH from HONO/HOOH photolysis in a temperature-controlled SOA chamber. CCN concentrations, activation diameter, and droplet growth kinetic information were monitored as a function of supersaturation (from 0.3% to 1.5%) for several hours using a cylindrical continuous-flow streamwise thermal gradient CCN counter connected to a scanning mobility particle sizer. The initial SOA concentrations ranged from 2 to 30 μg m−3 and presented CCN activity similar to monoterpene SOA with an activation diameter of 35 nm for 1.5% supersaturation and 72 nm for 0.6% supersaturation. The CCN activity improved slightly in some experiments as the SOA aged chemically and did not depend significantly on the level of NOx during the SOA production. The measured activation diameters correspond to a hygroscopicity parameter κ value of 0.12, similar to κ values of 0.1 ± 0.04 reported for monoterpene SOA. Analysis of the water-soluble carbon extracted from filter samples of the SOA suggest that it has a κ of 0.2–0.3 implying an average molar mass between 90 and 150 g mol−1 (assuming a zero and 5% surface tension reduction with respect to water, respectively). These findings are consistent with known oxidation products of isoprene. Using threshold droplet growth analysis, the CCN activation kinetics of isoprene SOA was determined to be similar to pure ammonium sulfate aerosol.

Cloud‐nucleating properties of the Amazonian biomass burning aerosol: Cloud condensation nuclei measurements and modeling

The cloud‐nucleating properties of the atmospheric aerosol were studied in an area under strong influence of vegetation burning. The measurements were part of Large‐Scale Biosphere Atmosphere Experiment in Amazonia–Smoke Aerosols, Clouds, Rainfall and Climate (LBA‐SMOCC) and were carried out at a ground site located in the state of Rondônia in southwestern Amazonia, Brazil, September to November 2002, covering the dry season, a transition period, and the onset of the wet season. The concentrations of cloud condensation nuclei (CCN) were measured with a static thermal gradient CCN counter for supersaturations ranging between 0.23 and 1.12%. As a closure test, the CCN concentrations were predicted with a time resolution of 10 min from measurements of the dry particle number size distribution (3–850 nm, Differential Mobility Analyzer (DMPS)) and hygroscopic growth at 90% relative humidity (Hygroscopic Tandem Differential Mobility Analyzer (H‐TDMA)). No chemical information was needed. The predicted and measured CCN concentrations were highly correlated (r2 = 0.97–0.99), and the predictions were only slightly lower than those measured, typically by 15–20%. Parameterizations of the predicted CCN concentrations are given for each of the three meteorological periods. These are based on averages taken during the afternoon hours when the measurements at ground level were representative for the aerosol entering the base of convective clouds. Furthermore, a more detailed parameterization including the mixing state of the aerosol is given, where the hygroscopic properties are expressed as the number of soluble ions or nondissociating molecules per unit volume dry particle.

Mapping the Operation of the DMT Continuous Flow CCN Counter

This work thoroughly analyzes a new commercial instrument for measuring Cloud Condensation Nuclei (CCN), the Droplet Measurement Technologies Cylindrical Continuous-Flow Streamwise Thermal Gradient CCN Chamber (CFSTGC). This instrument can measure CCN concentrations at supersaturations from 0.06% to 3% (potentially up to 6%), at a 1 Hz sampling rate that is sufficient for airborne operation. Our analysis employs a fully coupled numerical flow model to simulate the water vapor supersaturation, temperature, velocity profiles and CCN growth in the CFSTGC for its entire range of operation (aerosol sample flow rates 0.25–2.0 L min − 1 , temperature differences 2–15 K and ambient pressures 100–1000 mb). The model was evaluated by comparing simulated instrument responses for calibration aerosol against actual measurements from an existing CCN instrument. The model was used to evaluate the CCN detection efficiency for a wide range of ambient pressures, flow rates, temperature gradients, and droplet growth kinetic...