scholarly journals Spatiotemporal changes in aerosol properties by hygroscopic growth and impacts on radiative forcing and heating rates during DISCOVER-AQ 2011

2021 ◽  
Vol 21 (15) ◽  
pp. 12021-12048
Author(s):  
Daniel Pérez-Ramírez ◽  
David N. Whiteman ◽  
Igor Veselovskii ◽  
Richard Ferrare ◽  
Gloria Titos ◽  
...  

Abstract. This work focuses on the characterization of vertically resolved aerosol hygroscopicity properties and their direct radiative effects through a unique combination of ground-based and airborne remote sensing measurements during the Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) 2011 field campaign in the Baltimore–Washington DC metropolitan area. To that end, we combined aerosol measurements from a multiwavelength Raman lidar located at NASA Goddard Space Flight Center and the airborne NASA Langley High Spectral Resolution Lidar-1 (HSRL-1) lidar system. In situ measurements aboard the P-3B airplane and ground-based Aerosol Robotic Network – Distributed Regional Aerosol Gridded Observational Network (AERONET-DRAGON) served to validate and complement quantifications of aerosol hygroscopicity from lidar measurements and also to extend the study both temporally and spatially. The focus here is on 22 and 29 July 2011, which were very humid days and characterized by a stable atmosphere and increasing relative humidity with height in the planetary boundary layer (PBL). Combined lidar and radiosonde (temperature and water vapor mixing ratio) measurements allowed the retrieval of the Hänel hygroscopic growth factor which agreed with that obtained from airborne in situ measurements and also explained the significant increase of extinction and backscattering with height. Airborne measurements also confirmed aerosol hygroscopicity throughout the entire day in the PBL and identified sulfates and water-soluble organic carbon as the main species of aerosol particles. The combined Raman and HSRL-1 measurements permitted the inversion for aerosol microphysical properties revealing an increase of particle radius with altitude consistent with hygroscopic growth. Aerosol hygroscopicity pattern served as a possible explanation of aerosol optical depth increases during the day, particularly for fine-mode particles. Lidar measurements were used as input to the libRadtran radiative transfer code to obtain vertically resolved aerosol radiative effects and heating rates under dry and humid conditions, and the results reveal that aerosol hygroscopicity is responsible for larger cooling effects in the shortwave range (7–10 W m−2 depending on aerosol load) near the ground, while heating rates produced a warming of 0.12 K d−1 near the top of PBL where aerosol hygroscopic growth was highest.

2021 ◽  
Author(s):  
Daniel Pérez-Ramírez ◽  
David N. Whiteman ◽  
Igor Veselovskii ◽  
Richard Ferrare ◽  
Gloria Titos ◽  
...  

Abstract. This work focuses on the characterization of vertically-resolved aerosol hygroscopicity properties and their direct radiative effects through a unique combination of ground-based and airborne remote sensing measurements during the DISCOVER-AQ 2011 field campaign in the Washington D.C. – Baltimore metropolitan area. To that end, we combined measurements from a multiwavelength Raman lidar located at NASA Goddard Space Flight Center and the airborne NASA Langley HSRL-1 lidar system. In-situ measurements on board the P-3B airplane and ground-based AERONET-DRAGON served to validate and complement quantifications of aerosol hygroscopicity from lidar measurements and also to extend the study both temporally and spatially. The focus here is on the 22nd and 29th of July, 2011 which were very humid days and characterized by a stable atmosphere and increasing relative humidity with height in the planetary boundary layer (PBL). Combined lidar and radiosonde measurements allowed the retrieval of the Hänel hygroscopic growth factor which agreed with that obtained from airborne in-situ measurements, and also explained the significant increase of extinction and backscattering with height. Airborne measurements also confirmed aerosol hygroscopicity throughout the entire day in the PBL and identified sulfates and water soluble organic carbon as the main species of aerosol particles. The combined Raman and HSRL-1 measurements permitted the inversion for aerosol microphysical properties revealing an increase of particle radius with altitude consistent with hygroscopic growth. Aerosol hygroscopicity was identified as the main reason to explain aerosol optical depth increases during the day, particularly for fine mode particles. Lidar measurements were used as input to the libRadtram radiative transfer code to obtain vertically-resolved aerosol radiative effects and heating rates under dry and humid conditions, and the results reveal that aerosol hygroscopicity is responsible for larger cooling effects in the shortwave range (7–10 W/m2 depending on aerosol load) near the ground, while heating rates produced a warming of 0.12 K/day near the top of PBL where aerosol hygroscopic growth was highest.


2019 ◽  
Author(s):  
Andrés Esteban Bedoya-Velásquez ◽  
Gloria Titos ◽  
Juan Antonio Bravo-Aranda ◽  
Martial Haeffelin ◽  
Olivier Favez ◽  
...  

Abstract. An experimental setup to study aerosol hygroscopicity is proposed based on the time evolution of attenuated backscatter coefficients from a ceilometer co-located to an instrumented-tower equipped with meteorological sensors at different heights. This setup is used to analyse a 4.5-year database at the ACTRIS SIRTA observatory in Palaiseau (Paris, France, 2.208º E, 48.713º N, 160 m above sea level). A strict criterion has been established to identify hygroscopic growth cases using ancillary information such as on-line chemical composition, resulting in eight hygroscopic growth cases from a total of 120 potential cases. For the eight cases, the hygroscopic growth-related properties such as the attenuated backscatter enhancement factor fβ (RH) and the hygroscopic growth coefficient γ are evaluated. This study evidence that the hygroscopicity parameter γ increases as the contribution of organic aerosols decreases. In this sense, organic mass fraction is anti-correlated with γ while it shows a positive correlation with the inorganic mass fraction. Among inorganic species, the higher correlation was found for NO3−. This is the first time that hygroscopic enhancement factors retrieved directly for ambient aerosols using remote sensing techniques are combined with on-line chemical composition in-situ measurements to evaluate the role of the different aerosol species on aerosol hygroscopicity.


2019 ◽  
Vol 19 (11) ◽  
pp. 7883-7896 ◽  
Author(s):  
Andrés Esteban Bedoya-Velásquez ◽  
Gloria Titos ◽  
Juan Antonio Bravo-Aranda ◽  
Martial Haeffelin ◽  
Olivier Favez ◽  
...  

Abstract. An experimental setup to study aerosol hygroscopicity is proposed based on the temporal evolution of attenuated backscatter coefficients from a ceilometer colocated with an instrumented tower equipped with meteorological sensors at different heights. This setup is used to analyze a 4.5-year database at the ACTRIS SIRTA observatory in Palaiseau (Paris, France, 2.208∘ E, 48.713∘ N; 160 m above sea level). A strict criterion-based procedure has been established to identify hygroscopic growth cases using ancillary information, such as online chemical composition, resulting in 8 hygroscopic growth cases from a total of 107 potential cases. For these eight cases, hygroscopic growth-related properties, such as the attenuated backscatter enhancement factor fβ (RH) and the hygroscopic growth coefficient γ, are evaluated. This study shows that the hygroscopicity parameter γ is negatively correlated with the aerosol organic mass fraction but shows a positive correlation with the aerosol inorganic mass fraction. Among inorganic species, nitrate exhibited the highest correlation. This is the first time that hygroscopic enhancement factors are directly retrieved under ambient aerosols using remote-sensing techniques, which are combined with online chemical composition in situ measurements to evaluate the role of the different aerosol species in aerosol hygroscopicity.


2014 ◽  
Vol 7 (9) ◽  
pp. 3095-3112 ◽  
Author(s):  
P. Sawamura ◽  
D. Müller ◽  
R. M. Hoff ◽  
C. A. Hostetler ◽  
R. A. Ferrare ◽  
...  

Abstract. Retrievals of aerosol microphysical properties (effective radius, volume and surface-area concentrations) and aerosol optical properties (complex index of refraction and single-scattering albedo) were obtained from a hybrid multiwavelength lidar data set for the first time. In July 2011, in the Baltimore–Washington DC region, synergistic profiling of optical and microphysical properties of aerosols with both airborne (in situ and remote sensing) and ground-based remote sensing systems was performed during the first deployment of DISCOVER-AQ. The hybrid multiwavelength lidar data set combines ground-based elastic backscatter lidar measurements at 355 nm with airborne High-Spectral-Resolution Lidar (HSRL) measurements at 532 nm and elastic backscatter lidar measurements at 1064 nm that were obtained less than 5 km apart from each other. This was the first study in which optical and microphysical retrievals from lidar were obtained during the day and directly compared to AERONET and in situ measurements for 11 cases. Good agreement was observed between lidar and AERONET retrievals. Larger discrepancies were observed between lidar retrievals and in situ measurements obtained by the aircraft and aerosol hygroscopic effects are believed to be the main factor in such discrepancies.


2017 ◽  
Author(s):  
Sebastian Düsing ◽  
Birgit Wehner ◽  
Patric Seifert ◽  
Albert Ansmann ◽  
Holger Baars ◽  
...  

Abstract. This study presents vertical profiles up to a height of 2300 m a.s.l. of aerosol microphysical and optical properties and cloud condensation nuclei (CCN). Corresponding data have been measured during a field campaign as part of the High-Definition Clouds and Precipitation for Advancing Climate Prediction (HD(CP)2) Observational Prototype Experiments (HOPE), which took place at Melpitz, Germany from September 9 to 29, 2013. The helicopter-borne payload ACTOS (Airborne Cloud and Turbulence Observation System) was used to determine the aerosol particle number size distribution (PNSD), the number concentrations of aerosol particles (PNC) and cloud condensation nuclei (CCN) (CCN-NC), the ambient relative humidity (RH), and temperature (T). Simultaneous measurements on ground provided a holistic view on aerosol microphysical properties such as the PNSD, the chemical composition and the CCN-NC. Additional measurements of a 3 + 2 wavelength polarization lidar system (PollyXT) provided profiles of the aerosol particle light backscatter coefficient (σbsc) for three wavelengths (355, 532 and 1064 nm). From profiles of σbsc profiles of the aerosol particle light extinction coefficient (σext) were determined using the extinction-to-backscatter ratio. Furthermore, CCN-NC profiles were estimated on basis of the lidar-measurements. Ambient state optical properties of aerosol particles were derived on the basis of airborne in situ measurements of ACTOS (PNSD) and in situ measurements on ground (chemical aerosol characterization) using Mie-theory. On the basis of ground-based and airborne measurements, this work investigates the representativeness of ground-based aerosol microphysical properties for the boundary layer for two case-studies. The PNSD measurements on ground showed a good agreement with the measurements provided with ACTOS for lower altitudes. The ground-based measurements of PNC and CCN-NC are representative for the PBL when the PBL is well mixed. Locally isolated new particle formation events on ground or at the top of the PBL led to vertical variability in the here presented cases and ground-based measurements are not representative for the PBL. Furthermore, the lidar-based estimates of CCN-NC profiles were compared with the airborne in situ measurements of ACTOS. This comparison showed good agreements within the uncertainty range. Finally, this work provides a closure study between the optical aerosol particle properties in ambient state based on the airborne ACTOS measurements and derived with the lidar measurements. The investigation of the optical properties shows for 14 measurement-points that the airborne-based particle light backscatter coefficient is for 1064 nm 50 % smaller than the measurements of the lidar system, 27.6 % smaller for 532 nm and 29.9 % smaller for 355 nm. These results are quite promising, since in-situ measurement based Mie-calculations of the particle light backscattering are scarce and the modelling is quite challenging. In contradiction for the particle light extinction coefficient retrieved from the airborne in situ measurements were found a good agreement. The airborne-based particle light extinction coefficient was just 7.9 % larger for 532 nm and 3.5 % smaller for 355 nm, for an assumed lidar ratio (LR) of 55 sr. The particle light extinction coefficient for 1064 nm was derived with a LR of 30 sr. For this wavelength, the airborne-based particle light extinction coefficient is 5.2 % smaller than the lidar-measurements. Also, the correlation for the particle light extinction coefficient in combination with Mie-based LR's are in agreement for typical LR's of European background aerosol.


2018 ◽  
Vol 18 (2) ◽  
pp. 1263-1290 ◽  
Author(s):  
Sebastian Düsing ◽  
Birgit Wehner ◽  
Patric Seifert ◽  
Albert Ansmann ◽  
Holger Baars ◽  
...  

Abstract. This paper examines the representativeness of ground-based in situ measurements for the planetary boundary layer (PBL) and conducts a closure study between airborne in situ and ground-based lidar measurements up to an altitude of 2300 m. The related measurements were carried out in a field campaign within the framework of the High-Definition Clouds and Precipitation for Advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in September 2013 in a rural background area of central Europe.The helicopter-borne probe ACTOS (Airborne Cloud and Turbulence Observation System) provided measurements of the aerosol particle number size distribution (PNSD), the aerosol particle number concentration (PNC), the number concentration of cloud condensation nuclei (CCN-NC), and meteorological atmospheric parameters (e.g., temperature and relative humidity). These measurements were supported by the ground-based 3+2 wavelength polarization lidar system PollyXT, which provided profiles of the particle backscatter coefficient (σbsc) for three wavelengths (355, 532, and 1064 nm). Particle extinction coefficient (σext) profiles were obtained by using a fixed backscatter-to-extinction ratio (also lidar ratio, LR). A new approach was used to determine profiles of CCN-NC for continental aerosol. The results of this new approach were consistent with the airborne in situ measurements within the uncertainties.In terms of representativeness, the PNSD measurements on the ground showed a good agreement with the measurements provided with ACTOS for lower altitudes. The ground-based measurements of PNC and CCN-NC are representative of the PBL when the PBL is well mixed. Locally isolated new particle formation events on the ground or at the top of the PBL led to vertical variability in the cases presented here and ground-based measurements are not entirely representative of the PBL. Based on Mie theory (Mie, 1908), optical aerosol properties under ambient conditions for different altitudes were determined using the airborne in situ measurements and were compared with the lidar measurements. The investigation of the optical properties shows that on average the airborne-based particle light backscatter coefficient is 50.1 % smaller for 1064 nm, 27.4 % smaller for 532 nm, and 29.5 % smaller for 355 nm than the measurements of the lidar system. These results are quite promising, since in situ measurement-based Mie calculations of the particle light backscattering are scarce and the modeling is quite challenging. In contrast, for the particle light extinction coefficient we found a good agreement. The airborne-based particle light extinction coefficient was just 8.2 % larger for 532 nm and 3 % smaller for 355 nm, for an assumed LR of 55 sr. The particle light extinction coefficient for 1064 nm was derived with a LR of 30 sr. For this wavelength, the airborne-based particle light extinction coefficient is 5.2 % smaller than the lidar measurements. For the first time, the lidar ratio of 30 sr for 1064 nm was determined on the basis of in situ measurements and the LR of 55 sr for 355 and 532 nm wavelength was reproduced for European continental aerosol on the basis of this comparison. Lidar observations and the in situ based aerosol optical properties agree within the uncertainties. However, our observations indicate that a determination of the PNSD for a large size range is important for a reliable modeling of aerosol particle backscattering.


2020 ◽  
Author(s):  
Ma Yining ◽  
Xin Jinyuan

<p><strong>Abstract:</strong> Ecological region in southern China has been perennially affected by monsoon climate and anthropogenic emissions, resulting in complex aerosol components and frequent long-range transport. In this study, a Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model is applied to estimate aerosol radiative forcing (ARF) and multiple aerosol observation datasets is used to estimate the aerosol chemical components and optical properties. The aerosol loading and the radiative effects in the ecological region exhibited strong seasonal changes. The average major components (NH<sub>4</sub><sup>+</sup>, NO<sub>3</sub><sup>−</sup>, SO<sub>4</sub><sup>2−</sup>) in Total water soluble ionic (TWSI) ,organic carbon (OC) concentration, the ratio of organic carbon to element carbon (OC/EC) and biogenic secondary organic aerosol (BSOA) tracers were 3.20±1.22 μg·m<sup>-3</sup>, 2.19±1.39 μg·m<sup>-3</sup>, 3.17 and 74.00±35.23 ng·m<sup>-3 </sup>in the dry season and 2.22±0.91 μg·m<sup>-3</sup>, 3.14±1.62 μg·m<sup>-3</sup>, 7.13 and 186.34±113.82 ng·m<sup>-3</sup> in the wet season, respectively. The average radiative forcing at the top of atmosphere (TOA) is -11.73±11.36 W/m<sup>2</sup> and -0.41±10.08 W/m<sup>2</sup> in dry and wet season. When the aerosol single scattering albedo (SSA) less than 0.9, the retrieve frequency in wet season reached account for 75%. The increase of OC and BSOA transformed by forests in the wet season weaken the cooling effects. However, the dry season is mainly composed of anthropogenic inorganic aerosols, which enhances the scattering effect. The aerosol observation baseline also verified the seasonal variation of ARF in the ecological region. Driven by multiple factors such as meteorological conditions, emission sources, and the mixed state of particulate matter, the transport patterns of air masses in ecological area exhibits completely opposite affects to ARF.</p>


2011 ◽  
Vol 4 (3) ◽  
pp. 3055-3081
Author(s):  
S. J. Cooper ◽  
T. J. Garrett

Abstract. In a prior paper (Cooper and Garrett, 2010), an infrared remote sensing technique was developed that quantifies the effective radius re of ice crystals in cirrus clouds. By accounting for a broad range of expected inversion uncertainties, this retrieval scheme isolates those radiometric signatures that can only occur if the cirrus has nominally "small" values of re below 20 μm. The method is applicable only for specific cloud and atmospheric conditions. However, it can be particularly useful in constraining in-situ estimates of cirrus cloud re obtained from aircraft. Recent studies suggest that airborne measurements may be compromised by the shattering of ice crystals on airborne instrument inlets, so robust, independent confirmation of these measurements is needed. Here, we expand the Cooper and Garrett (2010) retrieval scheme to identify ice clouds that are likely to have "large" values of re greater than 20 μm. Using MODIS observations, we then compare assessments of cirrus cloud re with in-situ measurements obtained during three test cases from the 2010 SpartICus campaign. In general, there is good agreement between retrievals and in-situ measurements for a "small" and "large" crystal case. For a more ambiguously "small" re case, the 2D-S cloud probe indicates values of re that are slightly larger than expected from infrared retrievals, possibly indicating a slight bias in the 2D-S results towards large particles. There is no evidence to support that an FSSP-100 with unmodified inlets produces measurements of re in cirrus that are strongly biased low, as has been claimed.


2011 ◽  
Vol 11 (20) ◽  
pp. 10705-10726 ◽  
Author(s):  
P. Royer ◽  
P. Chazette ◽  
K. Sartelet ◽  
Q. J. Zhang ◽  
M. Beekmann ◽  
...  

Abstract. An innovative approach using mobile lidar measurements was implemented to test the performances of chemistry-transport models in simulating mass concentrations (PM10) predicted by chemistry-transport models. A ground-based mobile lidar (GBML) was deployed around Paris onboard a van during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer experiment in July 2009. The measurements performed with this Rayleigh-Mie lidar are converted into PM10 profiles using optical-to-mass relationships previously established from in situ measurements performed around Paris for urban and peri-urban aerosols. The method is described here and applied to the 10 measurements days (MD). MD of 1, 15, 16 and 26 July 2009, corresponding to different levels of pollution and atmospheric conditions, are analyzed here in more details. Lidar-derived PM10 are compared with results of simulations from POLYPHEMUS and CHIMERE chemistry-transport models (CTM) and with ground-based observations from the AIRPARIF network. GBML-derived and AIRPARIF in situ measurements have been found to be in good agreement with a mean Root Mean Square Error RMSE (and a Mean Absolute Percentage Error MAPE) of 7.2 μg m−3 (26.0%) and 8.8 μg m−3 (25.2%) with relationships assuming peri-urban and urban-type particles, respectively. The comparisons between CTMs and lidar at ~200 m height have shown that CTMs tend to underestimate wet PM10 concentrations as revealed by the mean wet PM10 observed during the 10 MD of 22.4, 20.0 and 17.5 μg m−3 for lidar with peri-urban relationship, and POLYPHEMUS and CHIMERE models, respectively. This leads to a RMSE (and a MAPE) of 6.4 μg m−3 (29.6%) and 6.4 μg m−3 (27.6%) when considering POLYPHEMUS and CHIMERE CTMs, respectively. Wet integrated PM10 computed (between the ground and 1 km above the ground level) from lidar, POLYPHEMUS and CHIMERE results have been compared and have shown similar results with a RMSE (and MAPE) of 6.3 mg m−2 (30.1%) and 5.2 mg m−2 (22.3%) with POLYPHEMUS and CHIMERE when comparing with lidar-derived PM10 with periurban relationship. The values are of the same order of magnitude than other comparisons realized in previous studies. The discrepancies observed between models and measured PM10 can be explained by difficulties to accurately model the background conditions, the positions and strengths of the plume, the vertical turbulent diffusion (as well as the limited vertical model resolutions) and chemical processes as the formation of secondary aerosols. The major advantage of using vertically resolved lidar observations in addition to surface concentrations is to overcome the problem of limited spatial representativity of surface measurements. Even for the case of a well-mixed boundary layer, vertical mixing is not complete, especially in the surface layer and near source regions. Also a bad estimation of the mixing layer height would introduce errors in simulated surface concentrations, which can be detected using lidar measurements. In addition, horizontal spatial representativity is larger for altitude integrated measurements than for surface measurements, because horizontal inhomogeneities occurring near surface sources are dampened.


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