Atmospheric Aerosol Measurements Research Articles

Validation of initial observation from the first spaceborne high-spectral-resolution lidar with a ground-based lidar network

Abstract. On 16 April 2022, China successfully launched the world's first spaceborne high-spectral-resolution lidar (HSRL), which is called the Aerosol and Carbon Detection Lidar (ACDL), on board the Atmospheric Environment Monitoring Satellite known as Daqi-1 (DQ-1). The ACDL is expected to precisely detect the three-dimensional distribution of aerosol and cloud globally with high spatial–temporal resolutions. To assess the performance of the newly launched satellite lidar, the ACDL-retrieved observations were compared with ground-based lidar measurements of atmospheric aerosol and cloud over northwest China from May to July 2022 using the Belt and Road lidar network (BR-lidarnet) initiated by Lanzhou University in China and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations. A total of six cases in the daytime and nighttime, including clear days, dust events, and cloudy conditions, were selected for further analysis. Moreover, profiles of the total attenuated backscatter coefficient (TABC) and the volume depolarization ratio (VDR) at 532 nm measured by the ACDL, the CALIPSO lidar, and ground-based lidar are compared in detail. Comparison is made between the 532 nm extinction coefficient and lidar ratio obtained from ACDL HSRL retrieval and the Raman retrieval results obtained from BR-lidarnet. The achieved results revealed that the ACDL observations were in good agreement with the ground-based lidar measurements during dust events with a relative deviation of about −10.5 ± 25.4 % for the TABC and −6.0 ± 38.5 % for the VDR. Additionally, the heights of the cloud top and bottom from these two measurements were well matched and comparable. Compared with the observation of CALIPSO, the ACDL also shows high consistency. This study proves that the ACDL provides reliable observations of aerosol and cloud in the presence of various climatic conditions, which helps to further evaluate the impacts of aerosol on climate and the environment, as well as on the ecosystem in the future.

Raman lidar at 355 nm using low dead time photon counting for atmospheric aerosol measurements.

Photon counting is an effective way to enhance the dynamic range of the data acquisition system (DAQ) in Raman lidars. However, there exists a deficiency of relatively high dead times among current options, which necessitates an additional calibration procedure for the nonlinearity of the photon counting signal, thus leading to unanticipated errors. A field programmable gate array (FPGA)-based photon counting module has been proposed and implemented in a Raman lidar, offering two operational channels. Through observational experiments, it was determined that this module has an overall dead time of 1.13ns taking advantage of the high-speed amplifier/discriminator pair and the logic design, a significant improvement compared to the 4.35ns of a commercially used Licel transient recorder within the same counting rate range. This notably low dead time implies that its output maintains sufficient linearity even at substantially high counting rates. As a result, the need for a dead time calibration procedure prior to signal integration with the analog signal is eliminated, reducing uncertainty in the final integrated signal, and even in the retrieval result. The backscattering result of the comparison between this module and a transient recorder indicates that a more precise performance can be acquired benefiting from this hardware upgrading.

Aerosol absorption using in situ filter-based photometers and ground-based sun photometry in the Po Valley urban atmosphere

Abstract. Light-absorbing aerosols (LAAs) are short-lived climate forcers with a significant impact on Earth's radiative balance. LAAs include dust aerosols, black carbon (BC) and organic light-absorbing carbonaceous aerosol (collectively termed brown carbon, BrC), which have also been proven to be highly toxic. In this study, aerosol absorption at five wavelengths (ranging from ultraviolet to infrared) was monitored continuously using filter-based photometers during two winter seasons in 2020 and 2021 in the city of Modena (southern central Po Valley, northern Italy), at two regulatory air quality monitoring sites, along with other pollutants (coarse particulate matter, PM10; fine particulate matter, PM2.5; O3; NO; NO2; and C6H6) and the vehicular traffic rate. The aerosol optical depth (AOD) and other column aerosol optical properties were concurrently monitored at four wavelengths by an AErosol RObotic NETwork (AERONET) sun photometer under urban background conditions within Modena. In situ absorption levels were apportioned to both sources (fossil fuel and biomass burning) and species (BC and BrC), while columnar absorption was apportioned to BC, BrC and mineral dust. The combined analysis of the atmospheric aerosol and gas measurements and of the meteorological conditions (in situ and from the ERA5 reanalysis) identified the location of potential urban sources of BC and BrC, most likely related to traffic and biomass burning. In situ data show different diurnal/weekly patterns for BrC from biomass burning and BC from traffic, with minor differences between the background and the urban traffic conditions. AERONET version 3 absorption aerosol optical depth (AAOD) retrievals at four wavelengths allowed the estimation of the absorptive direct radiative effect due to LAAs over the same period under the reasonable assumption that the AOD signal is concentrated within the mixing layer. AERONET retrievals showed a modest correlation of columnar absorption with planetary boundary layer (PBL)-scaled in situ observations, although the correlation improved significantly during a desert dust transport event that affected both in situ aerosol and columnar absorption, particularly in the blue spectrum range. A low correlation occurred between the contribution of BrC to aerosol absorption for the in situ and the columnar observations, with the BrC contribution being generally larger for in situ observations. Finally, evidence of a highly layered atmosphere during the study period, featuring significant spatial mixing and modest vertical mixing, was shown by ERA5-based atmospheric temperature profiles and by the large correlation of concurrent AERONET AOD retrievals in Modena and in Ispra (on the northwestern side of the Po Valley, ca. 225 km from Modena).

The Design and Performance Evaluation of a 1550 nm All-Fiber Dual-Polarization Coherent Doppler Lidar for Atmospheric Aerosol Measurements

A 1550 nm all-fiber dual-polarization coherent Doppler lidar (DPCDL) was constructed to measure the depolarization ratio of atmospheric aerosols. In lidar systems, the polarization state of the laser source is typically required to be that of linearly parallel polarization. However, due to the influence of the fiber-optical transmission and the large-mode field output of the telescope, the laser polarization state changes. Hence, a polarizer was mounted to the emitting channel of the telescope to eliminate the depolarization effect. A fiber-optical polarization beam splitter divided the backscattered light into components with parallel and perpendicular polarization. The DPCDL used two coherent channels to receive each of these two polarization components. A calibration procedure was designed for the depolarization ratio to determine the differences in gain and non-responsiveness in the two polarization channels. The calibration factor was found to be 1.13. Additionally, the systematic error and the measured random error of the DPCDL were estimated to evaluate the performance of the system. The DPCDL’s systematic error was found to be about 0.0024, and the standard deviation was lower than 0.0048. The Allan deviations of a 1-min averaging window with a low SNR of 19 dB and a high SNR of 27 dB were 0.0104 and 0.0031, respectively. The random errors at different measured heights were mainly distributed below 0.015. To confirm the authenticity of the atmospheric depolarization ratio measured with the DPCDL, two field observations were conducted with the use of a co-located DPCDL and micro-pulse polarization lidar to perform a comparison. The results showed that the correlation coefficients of the aerosol depolarization ratios were 0.73 and 0.77, respectively. Moreover, the two continuous observations demonstrated the robustness and stability of the DPCDL. The depolarization ratios were detected in different weather conditions.

Free-tropospheric aerosols contribute to large aerosol optical depth at a remote, inland location with insignificant anthropogenic emissions

In-situ measurements of atmospheric aerosols from remote environments marked with negligible human activities are required to reduce the uncertainties associated with natural aerosols in pre-industrial climate forcings (particularly the aerosol-cloud interactions). In this study, we present long-term continuous aerosol measurements, carried out using ground-based and satellite observations, both close to the surface and in the vertical column, over a remote, rural, inland location in southern peninsular India. The near-surface aerosol concentrations were low, in general conformity to the typical pattern expected for a remote location, with the temporal changes being primarily governed by the background meteorology. However, the columnar aerosol optical depth (AOD) was surprisingly high and resembled that of a typical semi-urban continental location, with an yearly mean AOD of 0.47 ± 0.06. Spaceborne lidar observations in conjunction with ground-based radiometer measurements revealed that around 60% of this AOD was contributed by free-tropospheric aerosol layers during summer and monsoon seasons. Airmass back-trajectory analysis along with particle depolarisation ratio profiles indicate that these aerosol layers are mostly associated with long-range transported dust aerosols. Our findings indicate that benign surface concentration of aerosols at a location need not necessarily be sufficient to consider it as an optimal choice for studying background aerosols.

Quantifying the Viscosity of Individual Submicrometer Semisolid Particles Using Atomic Force Microscopy.

Atmospheric aerosols' viscosities can vary significantly depending on their composition, mixing states, relative humidity (RH) and temperature. The diffusion time scale of atmospheric gases into an aerosol is largely governed by its viscosity, which in turn influences heterogeneous chemistry and climate-relevant aerosol effects. Quantifying the viscosity of aerosols in the semisolid phase state is particularly important as they are prevalent in the atmosphere and have a wide range of viscosities. Currently, direct viscosity measurements of submicrometer individual atmospheric aerosols are limited, largely due to the inherent size limitations of existing experimental techniques. Herein, we present a method that utilizes atomic force microscopy (AFM) to directly quantify the viscosity of substrate-deposited individual submicrometer semisolid aerosol particles as a function of RH. The method is based on AFM force spectroscopy measurements coupled with the Kelvin-Voigt viscoelastic model. Using glucose, sucrose, and raffinose as model systems, we demonstrate the accuracy of the AFM method within the viscosity range of ∼104-107 Pa s. The method is applicable to individual particles with sizes ranging from tens of nanometers to several micrometers. Furthermore, the method does not require prior knowledge on the composition of studied particles. We anticipate future measurements utilizing the AFM method on atmospheric aerosols at various RH to aid in our understanding of the range of aerosols' viscosities, the extent of particle-to-particle viscosity variability, and how these contribute to the particle diversity observable in the atmosphere.

Evaluation of a method to quantify the number concentrations of submicron water-insoluble aerosol particles based on filter sampling and complex forward-scattering amplitude measurements

Water-insoluble aerosol particles (WIAPs), such as black carbon (BC), mineral dust, and primary biological aerosol particles (PBAPs), affect climate through their interaction with radiation and clouds. However, with the exception of BC, methods to identify WIAP types and quantify their number concentrations are limited. Here, we evaluated a method that has been recently developed to measure the number concentrations of submicron WIAPs based on atmospheric aerosol measurements at an urban site in Nagoya, Japan. In this method, atmospheric aerosol particles are collected on a filter and dispersed in water. Then, the complex forward-scattering amplitudes of individual particles are measured. This complex parameter reflects the complex refractive index, volume, and shape of each measured particle, enabling the characterization of these physical properties from the signals. The WIAPs were classified as BC-like, dust-like, and PBAP-like particles based on their complex amplitude data. The number concentrations of BC-like particles were strongly correlated with those of refractory BC particles measured by a Single Particle Soot Photometer. BC-like and dust-like particles dominated the population of the submicron WIAPs, which was also confirmed using electron microscopy and Wideband Integrated Bioaerosol Sensor observations. Under the observed atmospheric conditions, the number concentrations of WIAPs were measured with their dispersion efficiency from a filter to water of approximately 50%. These results indicate that our method based on filter sampling and complex forward-scattering amplitude measurements has the potential to become a new technique for quantifying the spatio-temporal distributions of WIAPs.

Shape Discrimination of Individual Aerosol Particles Using Light Scattering

We established an experimental apparatus by combining polarized light scattering and angle-resolved light scattering measurement technology to rapidly identify the shape of an individual aerosol particle. The experimental data of scattered light of Oleic acid, rod-shaped Silicon dioxide, and other particles with typical shape characteristics were analyzed statistically. To better study the relationship between the shape of particles and the properties of scattered light, the partial least squares discriminant analysis (PLS-DA) method was used to analyze the scattered light of aerosol samples based on the size screening of particles, and the shape recognition and classification method of the individual aerosol particle was established based on the analysis of the spectral data after nonlinear processing and grouping by particle size with the area under the receiver operating characteristic curve (AUC) as reference. The experimental results show that the proposed classification method has a good discrimination ability for spherical, rod-shaped, and other non-spherical particles, which can provide more information for atmospheric aerosol measurement, and has application value for traceability and exposure hazard assessment of aerosol particles.

Mass Absorption Efficiency of PM1 in Mexico City during ACU15

From January to March 2015, an atmospheric aerosol measurement campaign, “Aerosoles en Ciudad Universitaria 2015” (ACU15), was carried out in Mexico City to determine the particles’ optical properties and chemical composition. Two photoacoustic spectrometers measured the scattering and absorption coefficient at two different wavelengths. The average absorption coefficient at 532 nm was 12.71 ± 9.48 Mm−1 and at 870 nm was 10.35 ± 7.36 Mm−1. The average scattering coefficient was 65.63 ± 47.12 Mm−1 (532 nm) and 21.12 ± 14.24 Mm−1 (870 nm). The chemical composition was determined via an aerosol chemical speciation monitor. The organic aerosol fraction represented 53% of the total PM1 and was made up of 63% low volatile (4.64 µg m−3), 22% hydrogenated (1.90 µg m−3), and 15% semi-volatile organics (1.54 µg m−3). The correlation coefficient of chemical species (NO3−, NH4+, SO42−, low-volatile, and semi-volatile organics) and optical properties was 0.92. The multilinear regression showed a good agreement among chemical species and optical properties (r > 0.7). The mass absorption coefficient calculated for the measuring site at 870 nm was MAE870 = 5.8 m2 g−1, instead of the default 4.74 m2 g−1. Furthermore, based on the median AAE, the 532 nm MAE532 resulting from the multiple linear regression (MLR) showed the following coefficients: 7.70 m2 g−1 (eBC), 0.22 m2 g−1 (HOA), and 0.16 m2 g−1 (LV–OOA). The coefficients of MLR were: 7.08 m2 g−1 (eBC), 5.83 m2 g−1 (NO3−), 5.69 m2 g−1 (low volatile organic aerosol), 2.78 m2 g−1 (SO42−), 2.40 m2 g−1 (hydrocarbon-like organic aerosol), and 1.04 m2 g−1 (semi volatile organic aerosol).

Beyond the Ångström Exponent: Probing Additional Information in Spectral Curvature and Variability of In Situ Aerosol Hyperspectral (0.3-0.7μm) Optical Properties.

Ångström exponents (α) allow reconstruction of aerosol optical spectra over a broad range of wavelengths from measurements at two or more wavelengths. Hyperspectral measurements of atmospheric aerosols provide opportunities to probe measured spectra for information inaccessible from only a few wavelengths. Four sets of hyperspectral in situ aerosol optical coefficients (aerosol-phase total extinction, σ ext, and absorption, σ abs; liquid-phase soluble absorption from methanol, σ MeOH-abs, and water, σ DI-abs, extracts) were measured from biomass burning aerosols (BBAs). Hyperspectral single scattering albedo (ω), calculated from σ ext and σ abs, provide spectral resolution over a wide spectral range rare for this optical parameter. Observed spectral shifts between σ abs and σ MeOH-abs/σ DI-abs argue in favor of measuring σ abs rather than reconstructing it from liquid extracts. Logarithmically transformed spectra exhibited curvature better fit by second-order polynomials than linear α. Mapping second order fit coefficients (a 1, a 2) revealed samples from a given fire tended to cluster together, that is, aerosol spectra from a given fire were similar to each other and somewhat distinct from others. Separation in (a 1, a 2) space for spectra with the same α suggest additional information in second-order parameterization absent from the linear fit. Spectral features found in the fit residuals indicate more information in the measured spectra than captured by the fits. Above-detection σ MeOH-abs at 0.7μm suggests assuming all absorption at long visible wavelengths is BC to partition absorption between BC and brown carbon (BrC) overestimates BC and underestimates BrC across the spectral range. Hyperspectral measurements may eventually discriminate BBA among fires in different ecosystems under variable conditions.

Single-Particle Analysis of Atmospheric Aerosols: Applications of Raman Spectroscopy

Atmospheric aerosols, produced as a consequence of different anthropogenic and natural processes, impart significant control over the global energy budget, climate, and human–environmental health. Their size varies across the nano–micrometer scale. Based on their origin, they may be classified into primary or secondary aerosols. Biomass burning, incomplete combustion of fossil fuels, volcanic eruptions, and traffic-related and wind-driven suspensions contribute to primary aerosol emissions. In contrast, gas-to-particle conversion within the atmosphere leads to secondary particle production. The study of atmospheric aerosols is vital to the field of atmospheric research. The dynamic nature (highly variable concentration composition and size with space and time) of aerosols makes them difficult to investigate. Today, aerosol research involves the application of various spectrometric and spectroscopic techniques. The single-particle analysis of aerosols is yet a challenge. In this review, the merits and demerits of various offline and online techniques used for aerosol research are discussed in a nutshell. Mass spectrometric techniques fail in distinguishing certain species. However, Raman spectroscopy’s emergence for the compositional analysis of aerosols resolves most of the present characterization challenges. This review focuses on Raman spectroscopy applications, the merits of this technique, and its immense scope for the measurement of various types of aerosols and their properties. Surface-enhanced Raman spectroscopy (SERS) has an advantage over conventional micro-Raman spectroscopy (MRS). The review depicts the dominance of SERS, specifically in the context of the measurement of ambient atmospheric aerosols. This review discusses two important components, namely laboratory simulation and ambient aerosol studies.

Visible, near-infrared dual-polarization lidar based on polarization cameras: system design, evaluation and atmospheric measurements.

A visible, near-infrared (VIS-NIR) dual-polarization lidar technique employing laser diodes and polarization cameras has been designed and implemented for all-day unattended field measurements of atmospheric aerosols. The linear volume depolarization ratios (LVDR) and the offset angles can be retrieved from four-directional polarized backscattering signals at wavelengths of 458 nm and 808 nm without additional optical components and sophisticated system adjustments. Evaluations on the polarization crosstalk of the polarization camera and the offset angle have been performed in detail. A rotating linear polarizer (RLP) method based on the Stokes-Mueller formalism has been proposed and demonstrated for measuring extinction ratios of the polarization camera, which can be used to eliminate the polarization crosstalk between different polarization signals. The offset angles can be online measured with a precision of 0.1°, leading to negligible measurement errors on the LVDR. One-month statistical analysis revealed a small temporal variation of the offset angles, namely -0.13°±0.07° at 458 nm and 0.33°±0.09° at 808 nm, indicating good system stability for long-term measurement. Atmospheric measurements have been carried out to verify the system performance and investigate aerosol optical properties. The spectral characteristics of the aerosol extinction coefficient, the color ratio, the linear particle polarization ratio (LPDR) and the ratio of LPDR were retrieved and evaluated based on one-month continuous atmospheric measurements, from which different types of aerosols can be classified. The promising results showed great potential of employing the VIS-NIR dual-polarization lidar in characterizing aerosol optical properties, discriminating aerosol types and analyzing long-range aerosol transportation.

Surface photovoltage measurement of PM10 atmospheric aerosols collected over SRMIST-Kattankulathur campus (12.81° N & 80.03° E): a step towards utilization of atmospheric aerosols in optoelectronic applications

Surface photovoltage measurement of PM10 atmospheric aerosols collected over SRMIST-Kattankulathur campus (12.81° N & 80.03° E): a step towards utilization of atmospheric aerosols in optoelectronic applications

Atmospheric Carbon and Transport - America (ACT-America) Data Sets: Description, Management, and Delivery.

The ACT‐America project is a NASA Earth Venture Suborbital‐2 mission designed to study the transport and fluxes of greenhouse gases. The open and freely available ACT‐America data sets provide airborne in situ measurements of atmospheric carbon dioxide, methane, trace gases, aerosols, clouds, and meteorological properties, airborne remote sensing measurements of aerosol backscatter, atmospheric boundary layer height and columnar content of atmospheric carbon dioxide, tower‐based measurements, and modeled atmospheric mole fractions and regional carbon fluxes of greenhouse gases over the Central and Eastern United States. We conducted 121 research flights during five campaigns in four seasons during 2016–2019 over three regions of the US (Mid‐Atlantic, Midwest and South) using two NASA research aircraft (B‐200 and C‐130). We performed three flight patterns (fair weather, frontal crossings, and OCO‐2 underflights) and collected more than 1,140 h of airborne measurements via level‐leg flights in the atmospheric boundary layer, lower, and upper free troposphere and vertical profiles spanning these altitudes. We also merged various airborne in situ measurements onto a common standard sampling interval, which brings coherence to the data, creates geolocated data products, and makes it much easier for the users to perform holistic analysis of the ACT‐America data products. Here, we report on detailed information of data sets collected, the workflow for data sets including storage and processing of the quality controlled and quality assured harmonized observations, and their archival and formatting for users. Finally, we provide some important information on the dissemination of data products including metadata and highlights of applications of ACT‐America data sets.

Aerosol Layering in the Free Troposphere over the Industrial City of Raciborz in Southwest Poland and Its Influence on Surface UV Radiation

Atmospheric aerosol and ultraviolet index (UVI) measurements performed in Racibórz (50.08° N, 18.19° E) were analyzed for the period June–September 2019. Results of the following observations were taken into account: columnar characteristics of the aerosols (aerosol thickness, Angstrom exponent, single scattering albedo, asymmetry factor) obtained from standard CIMEL sun-photometer observations and parameters of aerosol layers (ALs) in the free troposphere (the number of layers and altitudes of the base and top) derived from continuous monitoring by a CHM-15k ceilometer. Three categories of ALs were defined: residues from the daily evolution of the planetary boundary layer (PBL) aerosols, from the PBL-adjacent layer, and from the elevated layer above the PBL. Total column ozone measurements taken by the Ozone-Monitoring Instrument on board NASA’s Aura satellite completed the list of variables used to model UVI variability under clear-sky conditions. The aim was to present a hybrid model (radiative transfer model combined with a regression model) for determining ALs’ impact on the observed UVI series. First, a radiative transfer model, the Tropospheric Ultraviolet–Visible (TUV) model, which uses typical columnar characteristics to describe UV attenuation in the atmosphere, was applied to calculate hypothetical surface UVI values under clear-sky conditions. These modeled values were used to normalize the measured UVI data obtained during cloudless conditions. Next, a regression of the normalized UVI values was made using the AL characteristics. Random forest (RF) regression was chosen to search for an AL signal in the measured data. This explained about 55% of the variance in the normalized UVI series under clear-sky conditions. Finally, the UVI values were calculated as the product of the RF regression and the relevant UVIs by the columnar TUV model. The root mean square error and mean absolute error of the hybrid model were 1.86% and 1.25%, respectively, about 1 percentage point lower than corresponding values derived from the columnar TUV model. The 5th–95th percentile ranges of the observation/model differences were [−2.5%, 2.8%] and [−3.0%, 5.3%] for the hybrid model and columnar TUV model, respectively. Therefore, the impact of ALs on measured surface UV radiation could be demonstrated using the proposed AL characteristics. The statistical analysis of the UVI differences between the models allowed us to identify specific AL configuration responsible for these differences.

Estimating Mass Concentration Using a Low-cost Portable Particle Counter Based on Full-year Observations: Issues to Obtain Reliable Atmospheric PM2.5 Data

Expanding the use of a recently introduced low-cost particle monitor (DC1700 Dylos Air Quality Monitor) for sensing atmospheric PM2.5 requires comparison with data obtained using a certified method for PM2.5 based on appropriate atmospheric observations. Full-year measurements of atmospheric aerosols were taken in Nagoya, Japan during March 2017-March 2018 using the DC1700 to measure the particle number concentrations of >0.5 and >2.5 μm diameter particles and to measure the PM2.5 mass concentration (Mdry, PM2.5) using an automated β attenuation mass monitor (PM712). The number-size distribution was measured using an optical particle counter (KC01D). The dried mass concentration of 0.5–2.5 μm particles (Mdry, 0.5–2.5) was estimated from the ambient relative humidity and the DC1700 number concentration. The values of Mdry, 0.5–2.5 were invariably less than those of Mdry, PM2.5. The coefficient of determination and slope of Mdry, 0.5–2.5 to Mdry, PM2.5 for the year were, respectively, 0.68 and 0.40. Slope values changed seasonally from 0.24 in July and August 2017 to 0.55 in May and April 2017. Light absorbing particles, smaller-fine particles, and the estimation method of Mdry, 0.5–2.5 were inferred as causes of the difference between Mdry, 0.5–2.5 and Mdry, PM2.5. Especially, we estimated a large contribution (ca. 54% underestimation of Mdry, 0.5–2.5 into Mdry, PM2.5) of particles smaller than the minimum detection diameter of DC1700. The seasonal variation of Mdry, 0.5–2.5/Mdry, PM2.5 was related to the volume fraction of particles smaller than 0.5 μm. Good correlation of Mdry, 0.5–2.5 to Mdry, PM2.5 suggests that data obtained using DC1700 with a correction factor are useful as a rough proxy of atmospheric PM2.5 within a season. However, precise estimation of PM2.5 from the DC1700 number concentrations should include appropriate corrections of the size distribution, not only hygroscopicity.

Demonstration of a combined differential absorption and high spectral resolution lidar for profiling atmospheric temperature.

This work presents the first demonstration of atmospheric temperature measurement using the differential absorption lidar (DIAL) technique. While DIAL is routinely used to measure atmospheric gases such as ozone and water vapor, almost no success has been found in using DIAL to measure atmospheric temperature. Attempts to measure temperature using a well-mixed gas like oxygen (O2) have largely failed based on a need for quantitative ancillary measurements of water vapor and atmospheric aerosols. Here, a lidar is described and demonstrated that simultaneously measures O2 absorption, water vapor number density, and aerosol backscatter ratio. This combination of measurements allows for the first measurements of atmospheric temperature with useful accuracy. DIAL temperature measurements are presented to an altitude of 4 km with 225 m and 30 min resolution with accuracy better than 3K. DIAL temperature data is compared to a co-located Raman lidar system and radiosondes to evaluate the system's performance. Finally, an analysis of current performance characteristics is presented, which highlights pathways for future improvement of this proof-of-concept instrument.

White LED light source radar system for multi-wavelength remote sensing measurement ofatmospheric aerosols.

A Mie scattering radar system with a white light-emitting diode (LED) light source is proposed for the multi-wavelength detection of atmospheric aerosols. By splitting the continuous spectrum, the multi-wavelength echo signals are extracted to achieve multi-wavelength real-time detection of atmospheric aerosols. The white LED spectrum characteristics are analyzed, and four detection wavelengths are set at 450, 525, 600, and 661 nm. The composition and detection principles of a white LED light source radar system are expounded, the design of each system part is described in detail, and the system parameters and data inversion algorithm are presented. We built a white LED light source radar system and conducted preliminary observation experiments. The results show that radar can achieve multi-wavelength real-time detection of atmospheric aerosols within a 300 m height, which can provide effective data for further study of aerosol particle distribution and lay a foundation for further studies of aerosol characteristics at special wavelengths.

DISCRIMINATION AEROSOL FORM CLOUDS USING CATS-ISS LIDAR OBSERVATIONS BASED ON RANDOM FOREST AND SVM ALGORITHMS OVER THE EASTERN PART OF MIDDLE EAST

Abstract. Aerosols and Clouds play an important role in the Earth's environment, climate change and climate models. The Cloud-Aerosol Transport System (CATS) as a lidar remote sensing instrument, from the International Space Station (ISS), provides range-resolved profile measurements of atmospheric aerosols and clouds. Discrimination aerosols from clouds have always been a challenges task in the classification of space-born lidars. In this study, two algorithms including Random Forest (RF) and Support Vector Machine (SVM) were used to tackle the problem in a nighttime lidar data from 18 October 2016 which passes form the western part of Iran. The procedure includes 3 stages preprocessing (improving the signal to noise, generating features, taking training sample), classification (implementing RF and SVM), and postprocessing (correcting misleading classification). Finally, the result of classifications of the two algorithms (RF-SVM) were compared against ground truth samples and Vertical Feature Mask (VFM) of CATS product indicated 0.96–0.94 and 0.88–0.88 respectively. Also, it should be mentioned that a kappa accuracy 0.88 was acquired when we compared VFM against our ground truth samples. Moreover, a visual comparison with Moderate Resolution Imaging Spectroradiometer (MODIS) AOD and RGB products demonstrating that clouds and aerosol can be well detected and discriminated. The experimental results elucidated that the proposed method for classification of space borne lidar observation leads to higher accuracy compared to PDFs based algorithms.

An extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles

Abstract. Real-time, online measurements of atmospheric organic aerosol (OA) composition are an essential tool for determining the emissions sources and physicochemical processes governing aerosol effects on climate and health. However, the reliance of current techniques on thermal desorption, hard ionization, and/or separated collection/analysis stages introduces significant uncertainties into OA composition measurements, hindering progress towards these goals. To address this gap, we present a novel, field-deployable extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which provides online, near-molecular (i.e., molecular formula) OA measurements at atmospherically relevant concentrations without analyte fragmentation or decomposition. Aerosol particles are continuously sampled into the EESI-TOF, where they intersect a spray of charged droplets generated by a conventional electrospray probe. Soluble components are extracted and then ionized as the droplets are evaporated. The EESI-TOF achieves a linear response to mass, with detection limits on the order of 1 to 10 ng m−3 in 5 s for typical atmospherically relevant compounds. In contrast to conventional electrospray systems, the EESI-TOF response is not significantly affected by a changing OA matrix for the systems investigated. A slight decrease in sensitivity in response to increasing absolute humidity is observed for some ions. Although the relative sensitivities to a variety of commercially available organic standards vary by more than a factor of 30, the bulk sensitivity to secondary organic aerosol generated from individual precursor gases varies by only a factor of 15. Further, the ratio of compound-by-compound sensitivities between the EESI-TOF and an iodide adduct FIGAERO-I-CIMS varies by only ±50 %, suggesting that EESI-TOF mass spectra indeed reflect the actual distribution of detectable compounds in the particle phase. Successful deployments of the EESI-TOF for laboratory environmental chamber measurements, ground-based ambient sampling, and proof-of-concept measurements aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.