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- ItemIntercomparison study and optical asphericity measurements of small ice particles in the CERN CLOUD experiment(Katlenburg-Lindau : Copernicus, 2017) Nichman, Leonid; Järvinen, Emma; Dorsey, James; Connolly, Paul; Duplissy, Jonathan; Fuchs, Claudia; Ignatius, Karoliina; Sengupta, Kamalika; Stratmann, Frank; Möhler, Ottmar; Schnaiter, Martin; Gallagher, MartinOptical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of -30, -40 and -50°C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot separate perfectly spherical ice particles from supercooled droplets. Correlation analysis of bulk averaged path depolarisation measurements and single particle measurements of these clouds showed higher R2 values at high concentrations and small diameters, but these results require further confirmation. We find that none of these instruments were able to determine unambiguously the phase of the small particles. These results have implications for the interpretation of atmospheric measurements and parametrisations for modelling, particularly for low particle number concentration clouds.
- ItemVertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events(Katlenburg-Lindau : Copernicus, 2018) Mamali, Dimitra; Marinou, Eleni; Sciare, Jean; Pikridas, Michael; Kokkalis, Panagiotis; Kottas, Michael; Binietoglou, Ioannis; Tsekeri, Alexandra; Keleshis, Christos; Engelmann, Ronny; Baars, Holger; Ansmann, Albert; Amiridis, Vassilis; Russchenberg, Herman; Biskos, GeorgeIn situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 μm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.
- ItemGARRLiC and LIRIC: Strengths and limitations for the characterization of dust and marine particles along with their mixtures(Katlenburg-Lindau : Copernicus, 2017) Tsekeri, Alexandra; Lopatin, Anton; Amiridis, Vassilis; Marinou, Eleni; Igloffstein, Julia; Siomos, Nikolaos; Solomos, Stavros; Kokkalis, Panagiotis; Engelmann, Ronny; Baars, Holger; Gratsea, Myrto; Raptis, Panagiotis I.; Binietoglou, Ioannis; Mihalopoulos, Nikolaos; Kalivitis, Nikolaos; Kouvarakis, Giorgos; Bartsotas, Nikolaos; Kallos, George; Basart, Sara; Schuettemeyer, Dirk; Wandinger, Ulla; Ansmann, Albert; Chaikovsky, Anatoli P.; Dubovik, OlegThe Generalized Aerosol Retrieval from Radiometer and Lidar Combined data algorithm (GARRLiC) and the LIdar-Radiometer Inversion Code (LIRIC) provide the opportunity to study the aerosol vertical distribution by combining ground-based lidar and sun-photometric measurements. Here, we utilize the capabilities of both algorithms for the characterization of Saharan dust and marine particles, along with their mixtures, in the south-eastern Mediterranean during the CHARacterization of Aerosol mixtures of Dust and Marine origin Experiment (CHARADMExp). Three case studies are presented, focusing on dust-dominated, marinedominated and dust-marine mixing conditions. GARRLiC and LIRIC achieve a satisfactory characterization for the dust-dominated case in terms of particle microphysical properties and concentration profiles. The marine-dominated and the mixture cases are more challenging for both algorithms, although GARRLiC manages to provide more detailed microphysical retrievals compared to AERONET, while LIRIC effectively discriminates dust and marine particles in its concentration profile retrievals. The results are also compared with modelled dust and marine concentration profiles and surface in situ measurements.
- ItemTarget categorization of aerosol and clouds by continuous multiwavelength-polarization lidar measurements(Katlenburg-Lindau : Copernicus, 2017) Baars, Holger; Seifert, Patric; Engelmann, Ronny; Wandinger, UllaAbsolute calibrated signals at 532 and 1064 nm and the depolarization ratio from a multiwavelength lidar are used to categorize primary aerosol but also clouds in high temporal and spatial resolution. Automatically derived particle backscatter coefficient profiles in low temporal resolution (30 min) are applied to calibrate the lidar signals. From these calibrated lidar signals, new atmospheric parameters in temporally high resolution (quasi-particle-backscatter coefficients) are derived. By using thresholds obtained from multiyear, multisite EARLINET (European Aerosol Research Lidar Network) measurements, four aerosol classes (small; large, spherical; large, non-spherical; mixed, partly nonspherical) and several cloud classes (liquid, ice) are defined. Thus, particles are classified by their physical features (shape and size) instead of by source. The methodology is applied to 2 months of continuous observations (24 h a day, 7 days a week) with the multiwavelength-Raman-polarization lidar PollyXT during the High-Definition Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in spring 2013. Cloudnet equipment was operated continuously directly next to the lidar and is used for comparison. By discussing three 24 h case studies, it is shown that the aerosol discrimination is very feasible and informative and gives a good complement to the Cloudnet target categorization. Performing the categorization for the 2-month data set of the entire HOPE campaign, almost 1 million pixel (5 min×30 m) could be analysed with the newly developed tool. We find that the majority of the aerosol trapped in the planetary boundary layer (PBL) was composed of small particles as expected for a heavily populated and industrialized area. Large, spherical aerosol was observed mostly at the top of the PBL and close to the identified cloud bases, indicating the importance of hygroscopic growth of the particles at high relative humidity. Interestingly, it is found that on several days non-spherical particles were dispersed from the ground into the atmosphere.
- ItemProfiling water vapor mixing ratios in Finland by means of a Raman lidar, a satellite and a model(Katlenburg-Lindau : Copernicus, 2017) Filioglou, Maria; Nikandrova, Anna; Niemelä, Sami; Baars, Holger; Mielonen, Tero; Leskinen, Ari; Brus, David; Romakkaniemi, Sami; Giannakaki, Elina; Komppula, MikaWe present tropospheric water vapor profiles measured with a Raman lidar during three field campaigns held in Finland. Co-located radio soundings are available throughout the period for the calibration of the lidar signals. We investigate the possibility of calibrating the lidar water vapor profiles in the absence of co-existing on-site soundings using water vapor profiles from the combined Advanced InfraRed Sounder (AIRS) and the Advanced Microwave Sounding Unit (AMSU) satellite product; the Aire Limitée Adaptation dynamique Développement INternational and High Resolution Limited Area Model (ALADIN/HIRLAM) numerical weather prediction (NWP) system, and the nearest radio sounding station located 100 km away from the lidar site (only for the permanent location of the lidar). The uncertainties of the calibration factor derived from the soundings, the satellite and the model data are < 2.8, 7.4 and 3.9 %, respectively. We also include water vapor mixing ratio intercomparisons between the radio soundings and the various instruments/model for the period of the campaigns. A good agreement is observed for all comparisons with relative errors that do not exceed 50 % up to 8 km altitude in most cases. A 4-year seasonal analysis of vertical water vapor is also presented for the Kuopio site in Finland. During winter months, the air in Kuopio is dry (1.15±0.40 †kg-1); during summer it is wet (5.54±1.02 †kg-1); and at other times, the air is in an intermediate state. These are averaged values over the lowest 2 km in the atmosphere. Above that height a quick decrease in water vapor mixing ratios is observed, except during summer months where favorable atmospheric conditions enable higher mixing ratio values at higher altitudes. Lastly, the seasonal change in disagreement between the lidar and the model has been studied. The analysis showed that, on average, the model underestimates water vapor mixing ratios at high altitudes during spring and summer.
- ItemCharacterization and source apportionment of organic aerosol using offline aerosol mass spectrometry(Katlenburg-Lindau : Copernicus, 2016) Daellenbach, K.R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J.G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; El Haddad, I.; Prévôt, A.S.H.Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 µm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60–91 %) achieved using this technique, together with low detection limits (0.8 µg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.
- ItemSeparation of the optical and mass features of particle components in different aerosol mixtures by using POLIPHON retrievals in synergy with continuous polarized Micro-Pulse Lidar (P-MPL) measurements(Katlenburg-Lindau : Copernicus, 2018) Córdoba-Jabonero, Carmen; Sicard, Michaël; Ansmann, Albert; del Águila, Ana; Baars, HolgerThe application of the POLIPHON (POlarization-LIdar PHOtometer Networking) method is presented for the first time in synergy with continuous 24/7 polarized Micro-Pulse Lidar (P-MPL) measurements to derive the vertical separation of two or three particle components in different aerosol mixtures, and the retrieval of their particular optical properties. The procedure of extinction-to-mass conversion, together with an analysis of the mass extinction efficiency (MEE) parameter, is described, and the relative mass contribution of each aerosol component is also derived in a further step. The general POLIPHON algorithm is based on the specific particle linear depolarization ratio given for different types of aerosols and can be run in either 1-step (POL-1) or 2 steps (POL-2) versions with dependence on either the 2- or 3-component separation. In order to illustrate this procedure, aerosol mixing cases observed over Barcelona (NE Spain) are selected: a dust event on 5 July 2016, smoke plumes detected on 23 May 2016 and a pollination episode observed on 23 March 2016. In particular, the 3-component separation is just applied for the dust case: a combined POL-1 with POL-2 procedure (POL-1/2) is used, and additionally the fine-dust contribution to the total fine mode (fine dust plus non-dust aerosols) is estimated. The high dust impact before 12:00 UTC yields a mean mass loading of 0.6±0.1 g m'2 due to the prevalence of Saharan coarse-dust particles. After that time, the mean mass loading is reduced by two-thirds, showing a rather weak dust incidence. In the smoke case, the arrival of fine biomass-burning particles is detected at altitudes as high as 7 km. The smoke particles, probably mixed with less depolarizing non-smoke aerosols, are observed in air masses, having their origin from either North American fires or the Arctic area, as reported by HYSPLIT back-trajectory analysis. The particle linear depolarization ratio for smoke shows values in the 0.10-0.15 range and even higher at given times, and the daily mean smoke mass loading is 0.017±0.008 g m'2, around 3 % of that found for the dust event. Pollen particles are detected up to 1.5 km in height from 10:00 UTC during an intense pollination event with a particle linear depolarization ratio ranging between 0.10 and 0.15. The maximal mass loading of Platanus pollen particles is 0.011±0.003 g m'2, representing around 2 % of the dust loading during the higher dust incidence. Regarding the MEE derived for each aerosol component, their values are in agreement with others referenced in the literature for the specific aerosol types examined in this work: 0.5±0.1 and 1.7±0.2 m2 g'1 are found for coarse and fine dust particles, 4.5±1.4 m2 g'1 is derived for smoke and 2.4±0.5 m2 g'1 for non-smoke aerosols with Arctic origin, and a MEE of 2.4±0.8 m2 g'1 is obtained for pollen particles, though it can reach higher or lower values depending on predominantly smaller or larger pollen grain sizes. Results reveal the high potential of the P-MPL system, a simple polarization-sensitive elastic backscatter lidar working in a 24/7 operation mode, to retrieve the relative optical and mass contributions of each aerosol component throughout the day, reflecting the daily variability of their properties. In fact, this procedure can be simply implemented in other P-MPLs that also operate within the worldwide Micro-Pulse Lidar Network (MPLNET), thus extending the aerosol discrimination at a global scale. Moreover, the method has the advantage of also being relatively easily applicable to space-borne lidars with an equivalent configuration such as the ongoing Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on board NASA CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) and the forthcoming Atmospheric Lidar (ATLID) on board the ESA EarthCARE mission.
- ItemThe Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): Laboratory intercomparison of ice nucleation measurements(Katlenburg-Lindau : Copernicus, 2018) DeMott, Paul J.; Möhler, Ottmar; Cziczo, Daniel J.; Hiranuma, Naruki; Petters, Markus D.; Petters, Sarah S.; Belosi, Franco; Bingemer, Heinz G.; Brooks, Sarah D.; Budke, Carsten; Burkert-Kohn, Monika; Collier, Kristen N.; Danielczok, Anja; Eppers, Oliver; Felgitsch, Laura; Garimella, Sarvesh; Grothe, Hinrich; Herenz, Paul; Hill, Thomas C. J.; Höhler, Kristina; Kanji, Zamin A.; Kiselev, Alexei; Koop, Thomas; Kristensen, Thomas B.; Krüger, Konstantin; Kulkarni, Gourihar; Levin, Ezra J. T.; Murray, Benjamin J.; Nicosia, Alessia; O'Sullivan, Daniel; Peckhaus, Andreas; Polen, Michael J.; Price, Hannah C.; Reicher, Naama; Rothenberg, Daniel A.; Rudich, Yinon; Santachiara, Gianni; Schiebel, Thea; Schrod, Jann; Seifried, Teresa M.; Stratmann, Frank; Sullivan, Ryan C.; Suski, Kaitlyn J.; Szakáll, Miklós; Taylor, Hans P.; Ullrich, Romy; Vergara-Temprado, Jesus; Wagner, Robert; Whale, Thomas F.; Weber, Daniel; Welti, André; Wilson, Theodore W.; Wolf, Martin J.; Zenker, JakeThe second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber-Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than -10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax° data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.
- ItemAlgorithms and uncertainties for the determination of multispectral irradiance components and aerosol optical depth from a shipborne rotating shadowband radiometer(Katlenburg-Lindau : Copernicus, 2017) Witthuhn, Jonas; Deneke, Hartwig; Macke, Andreas; Bernhard, GermarThe 19-channel rotating shadowband radiometer GUVis-3511 built by Biospherical Instruments provides automated shipborne measurements of the direct, diffuse and global spectral irradiance components without a requirement for platform stabilization. Several direct sun products, including spectral direct beam transmittance, aerosol optical depth, Ångström exponent and precipitable water, can be derived from these observations. The individual steps of the data analysis are described, and the different sources of uncertainty are discussed. The total uncertainty of the observed direct beam transmittances is estimated to be about 4% for most channels within a 95% confidence interval for shipborne operation. The calibration is identified as the dominating contribution to the total uncertainty. A comparison of direct beam transmittance with those obtained from a Cimel sunphotometer at a land site and a manually operated Microtops II sunphotometer on a ship is presented. Measurements deviate by less than 3 and 4% on land and on ship, respectively, for most channels and in agreement with our previous uncertainty estimate. These numbers demonstrate that the instrument is well suited for shipborne operation, and the applied methods for motion correction work accurately. Based on spectral direct beam transmittance, aerosol optical depth can be retrieved with an uncertainty of 0.02 for all channels within a 95% confidence interval. The different methods to account for Rayleigh scattering and gas absorption in our scheme and in the Aerosol Robotic Network processing for Cimel sunphotometers lead to minor deviations. Relying on the cross calibration of the 940 nm water vapor channel with the Cimel sunphotometer, the column amount of precipitable water can be estimated with an uncertainty of ±0.034 cm.
- ItemSingle-particle measurements of bouncing particles and in situ collection efficiency from an airborne aerosol mass spectrometer (AMS) with light-scattering detection(Katlenburg-Lindau : Copernicus, 2017) Liao, Jin; Brock, Charles A.; Murphy, Daniel M.; Sueper, Donna T.; Welti, André; Middlebrook, Ann M.A light-scattering module was coupled to an airborne, compact time-of-flight aerosol mass spectrometer (LS-AMS) to investigate collection efficiency (CE) while obtaining nonrefractory aerosol chemical composition measurements during the Southeast Nexus (SENEX) campaign. In this instrument, particles scatter light from an internal laser beam and trigger saving individual particle mass spectra. Nearly all of the single-particle data with mass spectra that were triggered by scattered light signals were from particles larger than ĝ1/4 280ĝ€nm in vacuum aerodynamic diameter. Over 33ĝ€000 particles are characterized as either prompt (27ĝ€%), delayed (15ĝ€%), or null (58ĝ€%), according to the time and intensity of their total mass spectral signals. The particle mass from single-particle spectra is proportional to that derived from the light-scattering diameter (dva-LS) but not to that from the particle time-of-flight (PToF) diameter (dva-MS) from the time of the maximum mass spectral signal. The total mass spectral signal from delayed particles was about 80ĝ€% of that from prompt ones for the same dva-LS. Both field and laboratory data indicate that the relative intensities of various ions in the prompt spectra show more fragmentation compared to the delayed spectra. The particles with a delayed mass spectral signal likely bounced off the vaporizer and vaporized later on another surface within the confines of the ionization source. Because delayed particles are detected by the mass spectrometer later than expected from their dva-LS size, they can affect the interpretation of particle size (PToF) mass distributions, especially at larger sizes. The CE, measured by the average number or mass fractions of particles optically detected that had measurable mass spectra, varied significantly (0.2-0.9) in different air masses. The measured CE agreed well with a previous parameterization when CE > 0.5 for acidic particles but was sometimes lower than the minimum parameterized CE of 0.5.