Condensation Particle Counter System Research Articles

The Asian tropopause aerosol layer within the 2017 monsoon anticyclone: microphysical properties derived from aircraft-borne in situ measurements

Abstract. The Asian summer monsoon is an effective pathway for aerosol particles and precursors from the planetary boundary layer over Central, South, and East Asia into the upper troposphere and lower stratosphere. An enhancement of aerosol particles within the Asian monsoon anticyclone (AMA), called the Asian tropopause aerosol layer (ATAL), has been observed by satellites. We discuss airborne in situ and remote sensing observations of aerosol microphysical properties conducted during the 2017 StratoClim field campaign within the AMA region. The aerosol particle measurements aboard the high-altitude research aircraft M55 Geophysica (maximum altitude reached of ∼20.5 km) were conducted with a modified ultra-high-sensitivity aerosol spectrometer – airborne (UHSAS-A; particle diameter detection range of 65 nm to 1 µm), the COndensation PArticle counting System (COPAS, detecting total concentrations of submicrometer-sized particles), and the New Ice eXpEriment – Cloud and Aerosol Spectrometer with Detection of POLarization (NIXE-CAS-DPOL). In the COPAS and UHSAS-A vertical particle mixing ratio (PMR) profiles and the size distribution profiles (for number, surface area, and volume concentration), the ATAL is evident as a distinct layer between ∼370 and 420 K potential temperature (Θ). Within the ATAL, the maximum detected PMRs (from the median profiles) were ∼700 mg−1 for particle diameters between 65 nm and 1 µm (UHSAS-A) and higher than 2500 mg−1 for diameters larger than 10 nm (COPAS). These values are up to 2 times higher than those previously found at similar altitudes in other tropical locations. The difference between the PMR profiles measured by the UHSAS-A and the COPAS indicate that the region below the ATAL at Θ levels from 350 to 370 K is influenced by the nucleation of aerosol particles (diameter <65 nm). We provide detailed analyses of the vertical distribution of the aerosol particle size distributions and the PMR and compare these with previous tropical and extratropical measurements. The backscatter ratio (BR) was calculated based on the aerosol particle size distributions measured in situ. The resulting data set was compared with the vertical profiles of the BR detected by the multiwavelength aerosol scatterometer (MAS) and an airborne miniature aerosol lidar (MAL) aboard the M55 Geophysica and by the satellite-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The data of all four methods largely agree with one another, showing enhanced BR values in the altitude range of the ATAL (between ∼15 and 18.5 km) with a maximum at 17.5 km altitude. By means of the AMA-centered equivalent latitude calculated from meteorological reanalysis data, it is shown that such enhanced values of the BR larger than 1.1 could only be observed within the confinement of the AMA.

In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 1: Summary of StratoClim results

Abstract. During the monsoon season of the year 2017 the airborne StratoClim mission took place in Kathmandu, Nepal, with eight mission flights of the M-55 Geophysica in the upper troposphere–lower stratosphere (UTLS) of the Asian monsoon anticyclone (AMA) over northern India, Nepal, and Bangladesh. More than 100 events of new particle formation (NPF) were observed. In total, more than 2 h of flight time was spent under NPF conditions as indicated by the abundant presence of nucleation-mode aerosols, i.e. with particle diameters dp smaller than 15 nm, which were detected in situ by means of condensation nuclei counting techniques. Mixing ratios of nucleation-mode particles (nnm) of up to ∼ 50 000 mg−1 were measured at heights of 15–16 km (θ ≈ 370 K). NPF was most frequently observed at ∼ 12–16 km altitude (θ ≈ 355–380 K) and mainly below the tropopause. Resulting nnm remained elevated (∼ 300–2000 mg−1) up to altitudes of ∼ 17.5 km (θ ≈ 400 K), while under NPF conditions the fraction (f) of sub-micrometre-sized non-volatile residues (dp > 10 nm) remained below 50 %. At ∼ 12–14 km (θ ≈ 355–365 K) the minimum of f (< 15 %) was found, and underneath, the median f generally remains below 25 %. The persistence of particles at nucleation-mode sizes is limited to a few hours, mainly due to coagulation, as demonstrated by a numerical simulation. The frequency of NPF events observed during StratoClim 2017 underlines the importance of the AMA as a source region for UTLS aerosols and for the formation and maintenance of the Asian tropopause aerosol layer (ATAL). The observed abundance of NPF-produced nucleation-mode particles within the AMA is not unambiguously attributable to (a) specific source regions in the boundary layer (according to backward trajectory analyses), or (b) the direct supply with precursor material by convective updraught (from correlations of NPF with carbon monoxide), or (c) the recent release of NPF-capable material from the convective outflow (according to air mass transport times in the tropical tropopause layer, TTL). Temperature anomalies with ΔT of 2 K (peak-to-peak amplitude), as observed at a horizontal wavelength of ∼ 70–100 km during a level flight of several hours, match with NPF detections and represent an additional mechanism for local increases in supersaturation of the NPF precursors. Effective precursor supply and widely distributed temperature anomalies within the AMA can explain the higher frequency of intense NPF observed during StratoClim 2017 than all previous NPF detections with COPAS (COndensation PArticle counting System) at TTL levels over Brazil, northern Australia, or West Africa.

Comparison study on characteristics of nano-sized particle number distribution by using condensation particle counter calibrated with spray and soot type particle generation methods

In the year 2011, the Particle Measurement Program (PMP) in Europe started the regulation of the diesel vehicle’s nano-sized particle number density (PN) due to its high degree of harm to the human body. Concretely, the standard level of PN emission was introduced in the Euro 5+ and 6 emissions regulation with a limit (<6.0 × 1011#/km) for diesel light-duty vehicle. Therefore, the determination of suitable and sophisticated instruments for reliable particle sampling and analysis was essential in taking exact experimental data. Now, among the PN emission measuring devices suggested by the PMP, condensation particle counter (CPC) is a key equipment for measuring the particle number density in real time and it has been used extensively. However, CPC can cause different results depending on operating conditions of the saturator and condensation that induce different rates of particle growth. This study was conducted to analyze the effect of CPC calibrated by a two-particle generator with spray and soot type methods applied on the nano-sized particle distribution’s parameters such as number concentration and linearity. Also, in order to ensure the reliability for particle sensor system named as PPS, which had emerged as a useful diagnostic to making spatially and temporally resolved quantitative measurements of diesel PN concentration, it was compared with calibrated CPC system. As a result, nano-sized particle measuring system with CPC calibrated by spray type particle generator had a much higher counting efficiency, indicating a larger nano size available than soot type particle generator. And, comparative experimental results on the correlation between the particle number of CPC to a reflectance PPS system showed that above 5,000 #/cm3 in number concentrations measured by CPC as well as PPS were found to be similar with good linear relationship.

Quantitative analysis of vehicle particle emission by using calibrated CPC system

Particle size distribution and particle number concentration from diesel engines are subjects of significant environmental concerns especially in the EU. A few years ago, the UN-ECE PMP proposed a method for measuring particle emissions in the diluted exhaust of internal combustion engine vehicles, which has become a key method used in new dilution systems and sampling condition. This paper describes the effects of parameters such as condensation particle counter (CPC) according to test procedures, test fuel and vehicle test mode, including NEDC and CVS-75 mode. The main results obtained from this study can be summarized as follows: (1) Periodic calibration of the CPC system is essential because the long-term usage of a CPC leads to an underestimation in the measurements of small particles. (2) Particle emissions measured by the UN-ECE PMP method were found to exhibit comparable repeatability as compared to other regulated emissions. (3) In particle number concentration emitted from different-fueled vehicles, the sources of particle emissions in an ascending order of magnitude are as follows: DPF equipped diesel passenger vehicles, gasoline and LPG fueled vehicles, and DPF unequipped diesel passenger vehicles. Also, we found that the particle numbers of DPF equipped diesel passenger vehicles, gasoline and LPG-fueled vehicles can meet the EU regulation limit (<6.0×1011#/km), while DPF unequipped diesel passenger vehicles do not meet the EU limit.

Effect of various LPG supply systems on exhaust particle emission in spark-ignited combustion engine

The particle size distribution and particle number (PN) concentration emitted by internal combustion engine are a subject of significant environmental concern because of their adverse health effects and environmental impact. This subject has recently attracted the attention of the Particle Measurement Programme (PMP). In 2007, the UN-ECE GRPE PMP proposed a new method to measure particle emissions in the diluted exhaust of automotive engines and a regulation limit (<6.0×1011 #/km, number of particles). The specific PN regulation of spark-ignited combustion engine will be regulated starting on September 1, 2014 (EURO 6). In this study, three types of LPG supply systems (a mixer system and a multi-point injection system with gas-phase or liquid-phase LPG fuel) were used for a comparison of the particulate emission characteristics, including the nano-sized particle number density. Each of the three LPG vehicles with various LPG injection systems contained a multi-cylinder engine with same displacement volumes of 2,000 cm3 and a three-way catalytic converter. The test fuel that was used in this study for the spark-ignited combustion engine was n-butane basis LPG fuel, which is primarily used for taxi vehicles in Korea. The characteristics of nano-particle size distribution and number concentration of particle sizes ranging from 20 to 1,000 nm (aerodynamic diameter) that were emitted from the three LPG vehicles with various LPG supply systems were investigated by using a condensation particle counter (CPC), which is recommended by the PMP under both the NEDC and FTP-75 test modes on a chassis dynamometer. The experimental results indicate that the PN emission characteristics that were obtained by the CPC system using the PMP procedure are sufficiently reliable compared to other regulated emissions. Additionally, the sources of PN emissions in ascending order of magnitude are as follows: mixer type, gas-phase LPG injection (LPGi) and liquid-phase LPG injection (LPLi) passenger vehicles. The liquid-phase LPG injection system produced relatively large particle sizes and number concentrations compared to the gaseous system, regardless of the vehicle driving cycle. This phenomenon can be explained by unburned micro-fuel droplets that were generated due to a relatively short homogeneous fuel-air mixture duration in the engine intake manifold. Also the particle number emissions from the LPG vehicle were influenced by the vehicle driving cycle.

Aerosols in the tropical and subtropical UT/LS: in-situ measurements of submicron particle abundance and volatility

Abstract. Processes occurring in the tropical upper troposphere (UT), the Tropical Transition Layer (TTL), and the lower stratosphere (LS) are of importance for the global climate, for stratospheric dynamics and air chemistry, and for their influence on the global distribution of water vapour, trace gases and aerosols. In this contribution we present aerosol and trace gas (in-situ) measurements from the tropical UT/LS over Southern Brazil, Northern Australia, and West Africa. The instruments were operated on board of the Russian high altitude research aircraft M-55 "Geophysica" and the DLR Falcon-20 during the campaigns TROCCINOX (Araçatuba, Brazil, February 2005), SCOUT-O3 (Darwin, Australia, December 2005), and SCOUT-AMMA (Ouagadougou, Burkina Faso, August 2006). The data cover submicron particle number densities and volatility from the COndensation PArticle counting System (COPAS), as well as relevant trace gases like N2O, ozone, and CO. We use these trace gas measurements to place the aerosol data into a broader atmospheric context. Also a juxtaposition of the submicron particle data with previous measurements over Costa Rica and other tropical locations between 1999 and 2007 (NASA DC-8 and NASA WB-57F) is provided. The submicron particle number densities, as a function of altitude, were found to be remarkably constant in the tropical UT/LS altitude band for the two decades after 1987. Thus, a parameterisation suitable for models can be extracted from these measurements. Compared to the average levels in the period between 1987 and 2007 a slight increase of particle abundances was found for 2005/2006 at altitudes with potential temperatures, Θ, above 430 K. The origins of this increase are unknown except for increases measured during SCOUT-AMMA. Here the eruption of the Soufrière Hills volcano in the Caribbean caused elevated particle mixing ratios. The vertical profiles from Northern hemispheric mid-latitudes between 1999 and 2006 also are compact enough to derive a parameterisation. The tropical profiles all show a broad maximum of particle mixing ratios (between Θ≈340 K and 390 K) which extends from below the TTL to above the thermal tropopause. Thus these particles are a "reservoir" for vertical transport into the stratosphere. The ratio of non-volatile particle number density to total particle number density was also measured by COPAS. The vertical profiles of this ratio have a maximum of 50% above 370 K over Australia and West Africa and a pronounced minimum directly below. Without detailed chemical composition measurements a reason for the increase of non-volatile particle fractions cannot yet be given. However, half of the particles from the tropical "reservoir" contain compounds other than sulphuric acid and water. Correlations of the measured aerosol mixing ratios with N2O and ozone exhibit compact relationships for the tropical data from SCOUT-AMMA, TROCCINOX, and SCOUT-O3. Correlations with CO are more scattered probably because of the connection to different pollution source regions. We provide additional data from the long distance transfer flights to the campaign sites in Brazil, Australia, and West-Africa. These were executed during a time window of 17 months within a period of relative volcanic quiescence. Thus the data represent a "snapshot picture" documenting the status of a significant part of the global UT/LS fine aerosol at low concentration levels 15 years after the last major (i.e., the 1991 Mount Pinatubo) eruption. The corresponding latitudinal distributions of the measured particle number densities are presented in this paper to provide data of the UT/LS background aerosol for modelling purposes.

Experimental characterization of the COndensation PArticle counting System for high altitude aircraft-borne application

Abstract. A characterization of the ultra-fine aerosol particle counter COPAS (COndensation PArticle counting System) for operation on board the Russian high altitude research aircraft M-55 Geophysika is presented. The COPAS instrument consists of an aerosol inlet and two dual-channel continuous flow Condensation Particle Counters (CPCs) operated with the chlorofluorocarbon FC-43. It operates at pressures between 400 and 50 hPa for aerosol detection in the particle diameter (dp) range from 6 nm up to 1 μm. The aerosol inlet, designed for the M-55, is characterized with respect to aspiration, transmission, and transport losses. The experimental characterization of counting efficiencies of three CPCs yields dp50 (50% detection particle diameter) of 6 nm, 11 nm, and 15 nm at temperature differences (ΔT) between saturator and condenser of 17°C, 30°C, and 33°C, respectively. Non-volatile particles are quantified with a fourth CPC, with dp50=11 nm. It includes an aerosol heating line (250°C) to evaporate H2SO4-H2O particles of 11 nm&lt;dp&lt;200 nm at pressures between 70 and 300 hPa. An instrumental in-flight inter-comparison of the different COPAS CPCs yields correlation coefficients of 0.996 and 0.985. The particle emission index for the M-55 in the range of 1.4–8.4×1016 kg−1 fuel burned has been estimated based on measurements of the Geophysika's own exhaust.

Experimental investigation and comparison of nanoparticle emission characteristics in light-duty vehicles for two different fuels

In recent years, particle number emissions rather than particulate mass emissions in automotive engines have become the subject with controversial discussions. Recent results from studies of health effects imply that it is possible that particulate mass does not properly correlate with the variety of health effects attributed to engine exhaust. The concern is now focusing on nano-sized particles emitted from I. C. engines. In this study, particulate mass and particle number concentration emitted from light-duty vehicles were investigated for a better understanding of the characteristics of the engine PM from different types of fuels, such as gasoline and diesel fuel. Engine nano-particle mass and size distributions of four test vehicles were measured by a condensation particle counter system, which is recommended by the particle measurement program in Europe (PMP), at the end of a dilution tunnel along a NEDC test mode on a chassis dynamometer. We found that particle number concentrations of diesel passenger vehicles with DPF system are lower than gasoline passenger vehicles, but PM mass has some similar values. However, in diesel vehicles with DPF system, PM mass and particle number concentrations were greatly influenced by PM regeneration. Particle emissions in light-duty vehicles emitted about 90% at the ECE15 cycle in NEDC test mode, regardless of vehicle fuel type. Particle emissions at the early cold condition of engine were highly emitted in the test mode.

Observations of meteoric material and implications for aerosol nucleation in the winter Arctic lower stratosphere derived from in situ particle measurements

Abstract. Number concentrations of total and non-volatile aerosol particles with size diameters &gt;0.01 μm as well as particle size distributions (0.4–23 μm diameter) were measured in situ in the Arctic lower stratosphere (10–20.5 km altitude). The measurements were obtained during the campaigns European Polar Stratospheric Cloud and Lee Wave Experiment (EUPLEX) and Envisat-Arctic-Validation (EAV). The campaigns were based in Kiruna, Sweden, and took place from January to March 2003. Measurements were conducted onboard the Russian high-altitude research aircraft Geophysica using the low-pressure Condensation Nucleus Counter COPAS (COndensation PArticle Counter System) and a modified FSSP 300 (Forward Scattering Spectrometer Probe). Around 18–20 km altitude typical total particle number concentrations nt range at 10–20 cm−3 (ambient conditions). Correlations with the trace gases nitrous oxide (N2O) and trichlorofluoromethane (CFC-11) are discussed. Inside the polar vortex the total number of particles &gt;0.01 μm increases with potential temperature while N2O is decreasing which indicates a source of particles in the above polar stratosphere or mesosphere. A separate channel of the COPAS instrument measures the fraction of aerosol particles non-volatile at 250°C. Inside the polar vortex a much higher fraction of particles contained non-volatile residues than outside the vortex (~67% inside vortex, ~24% outside vortex). This is most likely due to a strongly increased fraction of meteoric material in the particles which is transported downward from the mesosphere inside the polar vortex. The high fraction of non-volatile residual particles gives therefore experimental evidence for downward transport of mesospheric air inside the polar vortex. It is also shown that the fraction of non-volatile residual particles serves directly as a suitable experimental vortex tracer. Nanometer-sized meteoric smoke particles may also serve as nuclei for the condensation of gaseous sulfuric acid and water in the polar vortex and these additional particles may be responsible for the increase in the observed particle concentration at low N2O. The number concentrations of particles &gt;0.4 μm measured with the FSSP decrease markedly inside the polar vortex with increasing potential temperature, also a consequence of subsidence of air from higher altitudes inside the vortex. Another focus of the analysis was put on the particle measurements in the lowermost stratosphere. For the total particle density relatively high number concentrations of several hundred particles per cm3 at altitudes below ~14 km were observed in several flights. To investigate the origin of these high number concentrations we conducted air mass trajectory calculations and compared the particle measurements with other trace gas observations. The high number concentrations of total particles in the lowermost stratosphere are probably caused by transport of originally tropospheric air from lower latitudes and are potentially influenced by recent particle nucleation.