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- ItemCharging of mesospheric aerosol particles: The role of photodetachment and photoionization from meteoric smoke and ice particles(Göttingen : Copernicus, 2009) Rapp, M.Time constants for photodetachment, photoemission, and electron capture are considered for two classes of mesospheric aerosol particles, i.e., meteor smoke particles (MSPs) and pure water ice particles. Assuming that MSPs consist of metal oxides like Fe2O3 or SiO, we find that during daytime conditions photodetachment by solar photons is up to 4 orders of magnitude faster than electron attachment such that MSPs cannot be negatively charged in the presence of sunlight. Rather, even photoemission can compete with electron capture unless the electron density becomes very large (≫1000 cm-3) such that MSPs should either be positively charged or neutral in the case of large electron densities. For pure water ice particles, however, both photodetachment and photoemission are negligible due to the wavelength characteristics of its absorption cross section and because the flux of solar photons has already dropped significantly at such short wavelengths. This means that water ice particles should normally be negatively charged. Hence, our results can readily explain the repeated observation of the coexistence of positive and negative aerosol particles in the polar summer mesopause, i.e., small MSPs should be positively charged and ice particles should be negatively charged. These results have further important implications for our understanding of the nucleation of mesospheric ice particles as well as for the interpretation of incoherent scatter radar observations of MSPs. © 2009 Author(s).
- ItemDust mass, cloud condensation nuclei, and ice-nucleating particle profiling with polarization lidar: Updated POLIPHON conversion factors from global AERONET analysis(Göttingen : Copernicus GmbH, 2019) Ansmann, A.; Mamouri, R.-E.; Hofer, J.; Baars, H.; Althausen, D.; Abdullaev, S.F.The POLIPHON (Polarization Lidar Photometer Networking) method permits the retrieval of particle number, surface area, and volume concentration for dust and non-dust aerosol components. The obtained microphysical properties are used to estimate height profiles of particle mass, cloud condensation nucleus (CCN) and ice-nucleating particle (INP) concentrations. The conversion of aerosol-type-dependent particle extinction coefficients, derived from polarization lidar observations, into the aerosol microphysical properties (number, surface area, volume) forms the central part of the POLIPHON computations. The conversion parameters are determined from Aerosol Robotic Network (AERONET) aerosol climatologies of optical and microphysical properties. In this article, we focus on the dust-related POLIPHON retrieval products and present an extended set of dust conversion factors considering all relevant deserts around the globe. We apply the new conversion factor set to a dust measurement with polarization lidar in Dushanbe, Tajikistan, in central Asia. Strong aerosol layering was observed with mineral dust advected from Kazakhstan (0-2km height), Iran (2-5km), the Arabian peninsula (5-7km), and the Sahara (8-10km). POLIPHON results obtained with different sets of conversion parameters were contrasted in this central Asian case study and permitted an estimation of the conversion uncertainties.
- ItemNano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) for investigating hygroscopic properties of sub-10nm aerosol nanoparticles(Katlenburg-Lindau : Copernicus, 2020) Lei, Ting; Ma, Nan; Hong, Juan; Tuch, Thomas; Wang, Xin; Wang, Zhibin; Pöhlker, Mira; Ge, Maofa; Wang, Weigang; Mikhailov, Eugene; Hoffmann, Thorsten; Pöschl, Ulrich; Su, Hang; Wiedensohler, Alfred; Cheng, YafangInteractions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physicochemical properties of nanoparticles, however, is restricted by the limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Besides maintaining accurate and stable sheath and aerosol flow rates (1 %), high accuracy of the differential mobility analyzer (DMA) voltage (0:1 %) in the range of 0-50V is crucial for achieving accurate sizing and small sizing offsets between the two DMAs (1:4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (0:1 K). We also tested and discussed different ways of preventing predeliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size effect on the deliquescence and efflorescence relative humidity (DRH and ERH, respectively) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size dependence of DRH and ERH between 20 and 6 nm nanoparticles. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
- Item3+2 + X : what is the most useful depolarization input for retrieving microphysical properties of non-spherical particles from lidar measurements using the spheroid model of Dubovik et al. (2006)?(Katlenburg-Lindau : Copernicus, 2019) Tesche, Matthias; Kolgotin, Alexei; Haarig, Moritz; Burton, Sharon P.; Ferrare, Richard A.; Hostetler, Chris A.; Müller, DetlefThe typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β) at 355, 532, and 1064 nm and two extinction coefficients (α) at 355 and 532 nm. This data combination is referred to as a 3β C 2α or 3 + 2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter for the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of d that exceed 0.10 at 532 nm, i.e. in the presence of nonspherical particles such as desert dust, volcanic ash, and, under special circumstances, biomass-burning smoke. We use experimental data collected with instruments that are capable of measuring d at all three lidar wavelengths with an inversion routine that applies the spheroidal light-scattering model of Dubovik et al. (2006) with a fixed axis-ratio distribution to replicate scattering properties of non-spherical particles. The inversion gives the fraction of spheroids required to replicate the optical data as an additional output parameter. This is the first systematic test of the effect of using all theoretically possible combinations of d taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information of at least one wavelength already provides useful information for the inversion of optical data that have been collected in the presence of non-spherical mineral dust particles. However, any choice of d will give lower values of the single-scattering albedo than the traditional 3 + 2 data set. We find that input data sets that include d355 give a spheroid fraction that closely resembles the dust ratio we obtain from using β532 and d532 in a methodology applied in aerosol-type separation. The use of d355 in data sets of two or three d? reduces the spheroid fraction that is retrieved when using d532 and d1064. Use of the latter two parameters without accounting for d355 generally leads to high spheroid fractions that we consider not trustworthy. The use of three d instead of two δ, including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3 + 2 + d355 for the observations with varying contributions of mineral dust considered here. However, additional measurements at wavelengths different from 355 nm would be desirable for application to a wider range of aerosol scenarios that may include non-spherical smoke particles, which can have values of d355 that are indistinguishable from those found for mineral dust. We therefore conclude that - depending on measurement capability - the future standard input for inversion of lidar data taken in the presence of mineral dust particles and using the spheroid model of Dubovik et al. (2006) might be 3+2Cδ355 or 3 + 2 + δ355 + δ532. © 2019 The Author(s).
- ItemA phenomenology of new particle formation (NPF) at 13 European sites(Katlenburg-Lindau : European Geosciences Union, 2021) Bousiotis, Dimitrios; Pope, Francis D.; Beddows, David C. S.; Dall'Osto, Manuel; Massling, Andreas; Nøjgaard, Jakob Klenø; Nordstrøm, Claus; Niemi, Jarkko V.; Portin, Harri; Petäjä, Tuukka; Perez, Noemi; Alastuey, Andrés; Querol, Xavier; Kouvarakis, Giorgos; Mihalopoulos, Nikos; Vratolis, Stergios; Eleftheriadis, Konstantinos; Wiedensohler, Alfred; Weinhold, Kay; Merkel, Maik; Tuch, Thomas; Harrison, Roy M.New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (<ĝ€¯200ĝ€¯km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400ĝ€¯% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions. © Author(s) 2021.
- ItemSmall-scale mixing processes enhancing troposphere-to-stratosphere transport by pyro-cumulonimbus storms(Göttingen : Copernicus GmbH, 2007) Luderer, G.; Trentmann, J.; Hungershöfer, K.; Herzog, M.; Fromm, M.; Andreae, M.O.Deep convection induced by large forest fires is an efficient mechanism for transport of aerosol particles and trace gases into the upper troposphere and lower stratosphere (UT/LS). For many pyro-cumulonimbus clouds (pyroCbs) as well as other cases of severe convection without fire forcing, radiometric observations of cloud tops in the thermal infrared (IR) reveal characteristic structures, featuring a region of relatively high brightness temperatures (warm center) surrounded by a U-shaped region of low brightness temperatures. We performed a numerical simulation of a specific case study of pyroCb using a non-hydrostatic cloud resolving model with a two-moment cloud microphysics parameterization and a prognostic turbulence scheme. The model is able to reproduce the thermal IR structure as observed from satellite radiometry. Our findings establish a close link between the observed temperature pattern and small-scale mixing processes atop and downwind of the overshooting dome of the pyroCb. Such small-scale mixing processes are strongly enhanced by the formation and breaking of a stationary gravity wave induced by the overshoot. They are found to increase the stratospheric penetration of the smoke by up to almost 30 K and thus are of major significance for irreversible transport of forest fire smoke into the lower stratosphere.
- ItemAerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters(Katlenburg-Lindau : EGU, 2016) Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ∼ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.
- ItemYear-round stratospheric aerosol backscatter ratios calculated from lidar measurements above northern Norway(Göttingen : Copernicus GmbH, 2019) Langenbach, A.; Baumgarten, G.; Fiedler, J.; Lübken, F.-J.; Von Savigny, C.; Zalach, J.We present a new method for calculating backscatter ratios of the stratospheric sulfate aerosol (SSA) layer from daytime and nighttime lidar measurements. Using this new method we show a first year-round dataset of stratospheric aerosol backscatter ratios at high latitudes. The SSA layer is located at altitudes between the tropopause and about 30 km. It is of fundamental importance for the radiative balance of the atmosphere. We use a state-of-the-art Rayleigh-Mie-Raman lidar at the Arctic Lidar Observatory for Middle Atmosphere Research (ALOMAR) station located in northern Norway (69N, 16E; 380ma.s.l.). For nighttime measurements the aerosol backscatter ratios are derived using elastic and inelastic backscatter of the emitted laser wavelengths 355, 532 and 1064nm. The setup of the lidar allows measurements with a resolution of about 5 min in time and 150 m in altitude to be performed in high quality, which enables the identification of multiple sub-layers in the stratospheric aerosol layer of less than 1 km vertical thickness. We introduce a method to extend the dataset throughout the summer when measurements need to be performed under permanent daytime conditions. For that purpose we approximate the backscatter ratios from color ratios of elastic scattering and apply a correction function. We calculate the correction function using the average backscatter ratio profile at 355nm from about 1700 h of nighttime measurements from the years 2000 to 2018. Using the new method we finally present a year-round dataset based on about 4100 h of measurements during the years 2014 to 2017. © Author(s) 2019.
- ItemVAHCOLI, a new concept for lidars: technical setup, science applications, and first measurements(Katlenburg-Lindau : European Geosciences Union, 2021) Lübken, Franz-Josef; Höffner, JosefA new concept for a cluster of compact lidar systems named VAHCOLI (Vertical And Horizontal COverage by LIdars) is presented, which allows for the measurement of temperatures, winds, and aerosols in the middle atmosphere (10 110 km) with high temporal and vertical resolution of minutes and some tens of meters, respectively, simultaneously covering horizontal scales from a few hundred meters to several hundred kilometers ( four-dimensional coverage ). The individual lidars ( units ) being used in VAHCOLI are based on a diode-pumped alexandrite laser, which is currently designed to detect potassium (D 770 nm), and on sophisticated laser spectroscopy measuring all relevant frequencies (seeder laser, power laser, backscattered light) with high temporal resolution (2 ms) and high spectral resolution applying Doppler-free spectroscopy. The frequency of the lasers and the narrowband filter in the receiving system are stabilized to typically 10 100 kHz, which is a factor of roughly 105 smaller than the Doppler-broadened Rayleigh signal. Narrowband filtering allows for the measurement of Rayleigh and/or resonance scattering separately from the aerosol (Mie) signal during both night and day. Lidars used for VAHCOLI are compact (volume: 1m3) and multi-purpose systems which employ contemporary electronic, optical, and mechanical components. The units are designed to autonomously operate under harsh field conditions in remote locations. An error analysis with parameters of the anticipated system demonstrates that temperatures and line-of-sight winds can be measured from the lower stratosphere to the upper mesosphere with an accuracy of (0.1 5)K and (0.1 10)ms1, respectively, increasing with altitude. We demonstrate that some crucial dynamical processes in the middle atmosphere, such as gravity waves and stratified turbulence, can be covered by VAHCOLI with sufficient temporal, vertical, and horizontal sampling and resolution. The four-dimensional capabilities of VAHCOLI allow for the performance of time-dependent analysis of the flow field, for example by employing Helmholtz decomposition, and for carrying out statistical tests regarding, for example, intermittency and helicity. The first test measurements under field conditions with a prototype lidar were performed in January 2020. The lidar operated successfully during a 6-week period (night and day) without any adjustment. The observations covered a height range of 5 100 km and demonstrated the capability and applicability of this unit for the VAHCOLI concept.
- ItemAbsorption instruments inter-comparison campaign at the Arctic Pallas station(Katlenburg-Lindau : European Geosciences Union, 2021) Asmi, Eija; Backman, John; Servomaa, Henri; Virkkula, Aki; Gini, Maria I.; Eleftheriadis, Konstantinos; Müller, Thomas; Ohata, Sho; Kondo, Yutaka; Hyvärinen, AnttiAerosol light absorption was measured during a 1-month field campaign in June-July 2019 at the Pallas Global Atmospheric Watch (GAW) station in northern Finland. Very low aerosol concentrations prevailed during the campaign, which posed a challenge for the instruments' detection capabilities. The campaign provided a real-world test for different absorption measurement techniques supporting the goals of the European Metrology Programme for Innovation and Research (EMPIR) Black Carbon (BC) project in developing aerosol absorption standard and reference methods. In this study we compare the results from five filter-based absorption techniques - aethalometer models AE31 and AE33, a particle soot absorption photometer (PSAP), a multi-angle absorption photometer (MAAP), and a continuous soot monitoring system (COSMOS) - and from one indirect technique called extinction minus scattering (EMS). The ability of the filter-based techniques was shown to be adequate to measure aerosol light absorption coefficients down to around 0.01g¯Mm-1 levels when data were averaged to 1-2g¯h. The hourly averaged atmospheric absorption measured by the reference MAAP was 0.09g¯Mm-1 (at a wavelength of 637g¯nm). When data were averaged for >1g¯h, the filter-based methods agreed to around 40g¯%. COSMOS systematically measured the lowest absorption coefficient values, which was expected due to the sample pre-treatment in the COSMOS inlet. PSAP showed the best linear correlation with MAAP (slopeCombining double low line0.95, R2Combining double low line0.78), followed by AE31 (slopeCombining double low line0.93). A scattering correction applied to PSAP data improved the data accuracy despite the added noise. However, at very high scattering values the correction led to an underestimation of the absorption. The AE31 data had the highest noise and the correlation with MAAP was the lowest (R2Combining double low line0.65). Statistically the best linear correlations with MAAP were obtained for AE33 and COSMOS (R2 close to 1), but the biases at around the zero values led to slopes clearly below 1. The sample pre-treatment in the COSMOS instrument resulted in the lowest fitted slope. In contrast to the filter-based techniques, the indirect EMS method was not adequate to measure the low absorption values found at the Pallas site. The lowest absorption at which the EMS signal could be distinguished from the noise was >0.1g¯Mm-1 at 1-2g¯h averaging times. The mass absorption cross section (MAC) value measured at a range 0-0.3g¯Mm-1 was calculated using the MAAP and a single particle soot photometer (SP2), resulting in a MAC value of 16.0±5.7g¯m2g-1. Overall, our results demonstrate the challenges encountered in the aerosol absorption measurements in pristine environments and provide some useful guidelines for instrument selection and measurement practices. We highlight the need for a calibrated transfer standard for better inter-comparability of the absorption results. © Author(s) 2021.