Aerosol size distribution models based on in situ measurements

Abstract. The volcanic aerosol plume resulting from the Eyjafjallajökull eruption in Iceland in April and May 2010 was detected in clear layers above Switzerland during two periods (17–19 April 2010 and 16–19 May 2010). In-situ measurements of the airborne volcanic plume were performed both within ground-based monitoring networks and with a research aircraft up to an altitude of 6000 m a.s.l. The wide range of aerosol and gas phase parameters studied at the high altitude research station Jungfraujoch (3580 m a.s.l.) allowed for an in-depth characterization of the detected volcanic aerosol. Both the data from the Jungfraujoch and the aircraft vertical profiles showed a consistent volcanic ash mode in the aerosol volume size distribution with a mean optical diameter around 3 ± 0.3 μm. These particles were found to have an average chemical composition very similar to the trachyandesite-like composition of rock samples collected near the volcano. Furthermore, chemical processing of volcanic sulfur dioxide into sulfate clearly contributed to the accumulation mode of the aerosol at the Jungfraujoch. The combination of these in-situ data and plume dispersion modeling results showed that a significant portion of the first volcanic aerosol plume reaching Switzerland on 17 April 2010 did not reach the Jungfraujoch directly, but was first dispersed and diluted in the planetary boundary layer. The maximum PM10 mass concentrations at the Jungfraujoch reached 30 μgm−3 and 70 μgm−3 (for 10-min mean values) duri ng the April and May episode, respectively. Even low-altitude monitoring stations registered up to 45 μgm−3 of volcanic ash related PM10 (Basel, Northwestern Switzerland, 18/19 April 2010). The flights with the research aircraft on 17 April 2010 showed one order of magnitude higher number concentrations over the northern Swiss plateau compared to the Jungfraujoch, and a mass concentration of 320 (200–520) μgm−3 on 18 May 2010 over the northwestern Swiss plateau. The presented data significantly contributed to the time-critical assessment of the local ash layer properties during the initial eruption phase. Furthermore, dispersion models benefited from the detailed information on the volcanic aerosol size distribution and its chemical composition.

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Ground-based and airborne in-situ measurements of the Eyjafjallajökull volcanic aerosol plume in Switzerland in spring 2010

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-11-12949-2011 ◽

2011 ◽

Vol 11 (4) ◽

pp. 12949-13002 ◽

Cited By ~ 7

Author(s):

N. Bukowiecki ◽

P. Zieger ◽

E. Weingartner ◽

Z. Jurányi ◽

M. Gysel ◽

...

Keyword(s):

Chemical Composition ◽

Size Distribution ◽

Volcanic Ash ◽

In Situ Measurements ◽

Aerosol Size Distribution ◽

Volcanic Aerosol ◽

Research Aircraft ◽

Swiss Plateau ◽

Aerosol Plume

Abstract. The volcanic aerosol plume resulting from the Eyjafjallajökull eruption in Iceland in April and May 2010 was detected in clear layers above Switzerland during two periods (17–19 April 2010 and 16–19 May 2010). In-situ measurements of the airborne volcanic plume were performed both within ground-based monitoring networks and with a research aircraft up to an altitude of 6000 m a.s.l. The wide range of aerosol and gas phase parameters studied at the high altitude research station Jungfraujoch (3580 m a.s.l.) allowed for an in-depth characterization of the detected volcanic aerosol. Both the data from the Jungfraujoch and the aircraft vertical profiles showed a consistent volcanic ash mode in the aerosol volume size distribution with a mean optical diameter around 3 ± 0.3 μm. These particles were found to have an average chemical composition very similar to the trachyandesite-like composition of rock samples collected near the volcano. Furthermore, chemical processing of volcanic sulfur dioxide into sulfate clearly contributed to the accumulation mode of the aerosol at the Jungfraujoch. The combination of these in-situ data and plume dispersion modeling results showed that a significant portion of the first volcanic aerosol plume reaching Switzerland on 17 April 2010 did not reach the Jungfraujoch directly, but was first dispersed and diluted in the planetary boundary layer. The maximum PM10 mass concentrations at the Jungfraujoch reached 30 μg m−3 and 70 μg m−3 (for 10-min mean values) during the April and May episode, respectively. Even low-altitude monitoring stations registered up to 45 μg m−3 of volcanic ash related PM10 (Basel, Northwestern Switzerland, 18/19 April 2010). The flights with the research aircraft on 17 April 2010 showed one order of magnitude higher number concentrations over the northern Swiss plateau compared to the Jungfraujoch, and a mass concentration of 320 (200–520) μg m−3 on 18 May 2010 over the northwestern Swiss plateau. The presented data significantly contributed to the time-critical assessment of the local ash layer properties during the initial eruption phase. Furthermore, dispersion models benefited from the detailed information on the volcanic aerosol size distribution and its chemical composition.

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Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-9435-2016 ◽

2016 ◽

Vol 16 (14) ◽

pp. 9435-9455 ◽

Cited By ~ 8

Author(s):

Matthew J. Alvarado ◽

Chantelle R. Lonsdale ◽

Helen L. Macintyre ◽

Huisheng Bian ◽

Mian Chin ◽

...

Keyword(s):

Optical Properties ◽

Size Distribution ◽

Aerosol Size Distribution ◽

Visible Radiation ◽

Submicron Aerosol ◽

In Situ Data ◽

Aerosol Absorption ◽

Aerosol Scattering ◽

The Impact

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

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Aerosol measurements at the Gual Pahari EUCAARI station: preliminary results from in-situ measurements

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-7241-2010 ◽

2010 ◽

Vol 10 (15) ◽

pp. 7241-7252 ◽

Cited By ~ 41

Author(s):

A.-P. Hyvärinen ◽

H. Lihavainen ◽

M. Komppula ◽

T. S. Panwar ◽

V. P. Sharma ◽

...

Keyword(s):

Rainy Season ◽

In Situ Measurements ◽

Aerosol Size Distribution ◽

Finnish Meteorological Institute ◽

Convective Mixing ◽

Average Fraction ◽

Mode Size ◽

First Time ◽

Pm10 Mass

Abstract. The Finnish Meteorological Institute (FMI), together with The Energy and Resources Institute of India (TERI), contributed to the European Integrated project on Aerosol Cloud Climate and Air Quality Interactions, EUCAARI, by conducting aerosol measurements in Gual Pahari, India, from December 2007 to January 2010. This paper describes the station setup in detail for the first time and provides results from the aerosol in-situ measurements, which include PM and BCe masses, aerosol size distribution from 4 nm to 10 μm, and the scattering and absorption coefficients. The seasonal variation of the aerosol characteristics was very distinct in Gual Pahari. The highest concentrations were observed during the winter and the lowest during the rainy season. The average PM10 concentration (at STP conditions) was 216 μgm−3 and the average PM2.5 concentration was 126 μgm−3. A high percentage (4–9%) of the PM10 mass consisted of BCe which indicates anthropogenic influence. The percentage of BCe was higher during the winter; and according to the diurnal pattern of the BCe fraction, the peak occurred during active traffic hours. Another important source of aerosol particles in the area was new particle formation. The nucleated particles grew rapidly reaching the Aitken and accumulation mode size, thus contributing considerably to the aerosol load. The rainy season decreased the average fraction of particle mass in the PM2.5 size range, i.e. of secondary origin. The other mechanism decreasing the surface concentrations was based on convective mixing and boundary layer evolution. This diluted the aerosol when sun radiation and the temperature was high, i.e. especially during the pre-monsoon day time. The lighter and smaller particles were more effectively diluted.

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Combining airborne in situ and ground-based lidar measurements for attribution of aerosol layers

10.5194/acp-2017-1085 ◽

2018 ◽

Author(s):

Anna Nikandrova ◽

Ksenia Tabakova ◽

Antti Manninen ◽

Riikka Väänänen ◽

Tuukka Petäjä ◽

...

Keyword(s):

Boundary Layer ◽

Size Distribution ◽

Aerosol Size Distribution ◽

Long Range Transport ◽

Back Trajectories ◽

Clear Sky ◽

Temporal And Spatial Variability ◽

Range Transport ◽

Temporal And Spatial

Abstract. Understanding the distribution of aerosol layers is important for determining long range transport and aerosol radiative forcing. In this study we combine airborne in situ measurements of aerosol with data obtained by a ground-based High Spectral Resolution Lidar (HSRL) and radiosonde profiles to investigate the temporal and vertical variability of aerosol properties in the lower troposphere. The HSRL was deployed in Hyytiälä, Southern Finland, from January to September 2014 as a part of the US DoE ARM (Atmospheric Radiation Measurement) mobile facility during the BAECC (Biogenic Aerosols – Effects on Cloud and Climate) Campaign. Two flight campaigns took place in April and August 2014 with instruments measuring the aerosol size distribution from 10 nm to 10 µm at altitudes up to 3800 m. Two case studies from the flight campaigns, when several aerosol layers were identified, were selected for further investigation: one clear sky case, and one partly cloudy case. During the clear sky case, turbulent mixing ensured low temporal and spatial variability in the measured aerosol size distribution in the boundary layer whereas mixing was not as homogeneous in the boundary layer during the partly cloudy case. The elevated layers exhibited greater temporal and spatial variability in aerosol size distribution, indicating a lack of mixing. New particle formation was observed in the boundary layer during the clear sky case, and nucleation mode particles were also seen in the elevated layers that were not mixing with the boundary layer. Interpreting local measurements of elevated layers in terms of long-range transport can be achieved using back trajectories from Lagrangian models, but care should be taken in selecting appropriate arrival heights, since the modelled and observed layer heights did not always coincide. We conclude that higher confidence in attributing elevated aerosol layers with their air mass origin is attained when back trajectories are combined with lidar and radiosonde profiles.

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Validation of aerosol backscatter profiles from Raman lidar and ceilometer using balloon-borne measurements

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-2267-2021 ◽

2021 ◽

Vol 21 (3) ◽

pp. 2267-2285

Author(s):

Simone Brunamonti ◽

Giovanni Martucci ◽

Gonzague Romanens ◽

Yann Poltera ◽

Frank G. Wienhold ◽

...

Keyword(s):

Remote Sensing ◽

In Situ Measurements ◽

Aerosol Size Distribution ◽

Spatial And Temporal Variability ◽

Raman Lidar ◽

Backscatter Coefficient ◽

Custom Made ◽

Aerosol Backscatter ◽

Good Agreement

Abstract. Remote-sensing measurements by light detection and ranging (lidar) instruments are fundamental for the monitoring of altitude-resolved aerosol optical properties. Here we validate vertical profiles of aerosol backscatter coefficient (βaer) measured by two independent lidar systems using co-located balloon-borne measurements performed by Compact Optical Backscatter Aerosol Detector (COBALD) sondes. COBALD provides high-precision in situ measurements of βaer at two wavelengths (455 and 940 nm). The two analyzed lidar systems are the research Raman Lidar for Meteorological Observations (RALMO) and the commercial CHM15K ceilometer (Lufft, Germany). We consider in total 17 RALMO and 31 CHM15K profiles, co-located with simultaneous COBALD soundings performed throughout the years 2014–2019 at the MeteoSwiss observatory of Payerne (Switzerland). The RALMO (355 nm) and CHM15K (1064 nm) measurements are converted to 455 and 940 nm, respectively, using the Ångström exponent profiles retrieved from COBALD data. To account for the different receiver field-of-view (FOV) angles between the two lidars (0.01–0.02∘) and COBALD (6∘), we derive a custom-made correction using Mie-theory scattering simulations. Our analysis shows that both lidar instruments achieve on average a good agreement with COBALD measurements in the boundary layer and free troposphere, up to 6 km altitude. For medium-high-aerosol-content measurements at altitudes below 3 km, the mean ± standard deviation difference in βaer calculated from all considered soundings is −2 % ± 37 % (−0.018 ± 0.237 Mm−1 sr−1 at 455 nm) for RALMO−COBALD and +5 % ± 43 % (+0.009 ± 0.185 Mm−1 sr−1 at 940 mm) for CHM15K−COBALD. Above 3 km altitude, absolute deviations generally decrease, while relative deviations increase due to the prevalence of air masses with low aerosol content. Uncertainties related to the FOV correction and spatial- and temporal-variability effects (associated with the balloon's drift with altitude and different integration times) contribute to the large standard deviations observed at low altitudes. The lack of information on the aerosol size distribution and the high atmospheric variability prevent an accurate quantification of these effects. Nevertheless, the excellent agreement observed in individual profiles, including fine and complex structures in the βaer vertical distribution, shows that under optimal conditions, the discrepancies with the in situ measurements are typically comparable to the estimated statistical uncertainties in the remote-sensing measurements. Therefore, we conclude that βaer profiles measured by the RALMO and CHM15K lidar systems are in good agreement with in situ measurements by COBALD sondes up to 6 km altitude.

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Evaluating Model Parameterizations of Submicron Aerosol Scattering and Absorption with In Situ Data from ARCTAS 2008

10.5194/acp-2015-935 ◽

2016 ◽

Author(s):

M. J. Alvarado ◽

C. R. Lonsdale ◽

H. L. Macintyre ◽

H. Bian ◽

M. Chin ◽

...

Keyword(s):

Optical Properties ◽

Size Distribution ◽

Aerosol Size Distribution ◽

Visible Radiation ◽

Submicron Aerosol ◽

In Situ Data ◽

Aerosol Absorption ◽

Aerosol Scattering ◽

The Impact

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution is used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding in situ size distribution information, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction through out the aerosol size distribution. Using a core-shell mixing state in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for time-varying mixing states in future versions of ASP.

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On the Quantitative Low-Level Aerosol Measurements Using Ceilometer-Type Lidar

Journal of Atmospheric and Oceanic Technology ◽

10.1175/2009jtecha1252.1 ◽

2009 ◽

Vol 26 (11) ◽

pp. 2340-2352 ◽

Cited By ~ 19

Author(s):

Anu-Maija Sundström ◽

Timo Nousiainen ◽

Tuukka Petäjä

Keyword(s):

Size Distribution ◽

Theoretical Calculations ◽

Measurement Instrument ◽

Aerosol Size Distribution ◽

Lidar Measurement ◽

Size Distributions ◽

Absolute Accuracy ◽

Particle Composition ◽

Aerosol Measurement

Abstract The objective of this work is to investigate whether a commercial ceilometer-type lidar can be used as a quantitative aerosol measurement instrument. To this end, lidar backscattering measurements are compared with exact theoretical calculations of backscattering, which are based on in situ–measured size distributions and account for uncertainties in particle composition and shape. The results show that the differences between simulated and measured backscattering remain nearly constant and within the uncertainties involved. The differences are most plausibly explained by an error in the overlap function of the lidar and/or errors in the calibration of either the lidar or the in situ instruments used to measure the aerosol size distribution. Occasionally, large differences occur that are obviously connected to the unrepresentativeness of the in situ and lidar measurement volumes because of insufficient atmospheric mixing. The results imply that the absolute accuracy of the instrument investigated might be sufficient for quantitative aerosol measurements in some applications. A fix for the overlap function, however, would be desirable.

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A comparison of lognormal and gamma size distributions for characterizing the stratospheric aerosol phase function from optical particle counter measurements

Atmospheric Measurement Techniques ◽

10.5194/amt-13-1071-2020 ◽

2020 ◽

Vol 13 (3) ◽

pp. 1071-1087 ◽

Cited By ~ 2

Author(s):

Ernest Nyaku ◽

Robert Loughman ◽

Pawan K. Bhartia ◽

Terry Deshler ◽

Zhong Chen ◽

...

Keyword(s):

Gamma Distribution ◽

Phase Function ◽

Stratospheric Aerosol ◽

Aerosol Size Distribution ◽

Distribution Models ◽

Concentration Data ◽

Gamma Distributions ◽

Phase Functions ◽

Better Than

Abstract. A series of in situ measurements made by optical particle counters (OPCs) at Laramie, Wyoming, provides size-resolved stratospheric aerosol concentration data over the period 1971–2018. A subset of these data covering the period of 2008–2017 is analyzed in this study for the purpose of assessing the sensitivity of the stratospheric aerosol phase function to the aerosol size distribution (ASD) model used to fit the measurements. The two unimodal ASD models investigated are the unimodal lognormal (UMLN) and gamma distribution models, with the minimum χ2 method employed to assess how well each ASD fits the measurements. The aerosol phase function (Pa(Θ)) for each ASD is calculated using Mie theory and is compared to the Pa(Θ) derived from the Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics module. Comparing the χ2 values for the fits at altitudes of 20 and 25 km shows that the UMLN distribution better represents the OPC measurements; however, the gamma distribution fits the CARMA model results better than the UMLN model when the CARMA model results are subsetted into the OPC measurement bins. Comparing phase functions derived from the UMLN distribution fit to OPC data with gamma distributions fit to CARMA model results at the location of the OPC measurements shows a satisfying agreement (±5 %) within the scattering angle range of limb sounding satellites. This uncertainty is considerably larger if the CARMA data are fit with a UMLN.

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