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We derive the tropical modal age of air from an analysis of the water vapor tape recorder. We combine the observationally derived modal age with mean age of air from CO<sub>2</sub> and SF<sub>6</sub> to create diagnostics for the independent evaluation of the vertical transport rate and horizontal recirculation into the tropics between 16–32 km. These diagnostics are applied to two Global Modeling Initiative (GMI) chemistry and transport model (CTM) age tracer simulations to give new insights into the tropical transport characteristics of the meteorological fields from the GEOS4-GCM and the GEOS4-DAS. Both simulations are found to have modal ages that are in reasonable agreement with the empirically derived age (i.e., transit times) over the entire altitude range. Both simulations show too little horizontal recirculation into the tropics above 22 km, with the GEOS4-DAS fields having greater recirculation. Using CH<sub>4</sub> as a proxy for mean age, comparisons between HALOE and model CH<sub>4</sub> in the Antarctic demonstrate how the strength of tropical recirculation affects polar composition in both CTM experiments. Better tropical recirculation tends to improve the CH<sub>4</sub> simulation in the Antarctic. However, mean age in the Antarctic lower stratosphere can be compromised by poor representation of tropical ascent, tropical recirculation, or vortex barrier strength. The connection between polar and tropical composition shown in this study demonstrates the importance of diagnosing each of these processes separately in order to verify the adequate representation of the processes contributing to polar composition in models.
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A mineral dust module is developed and implemented into the global aerosol microphysics model, GISS-TOMAS. The model is evaluated against long-term measurements of dust surface mass concentrations and deposition fluxes. Predicted mass concentrations and deposition fluxes are in error on average by a factor of 3 and 5, respectively. The comparison shows that the model performs better near the dust source regions but underestimates surface concentrations and deposition fluxes in more remote regions. Including only sites with measured dust concentrations of at least 0.5 μg m<sup>−3</sup>, the model prediction agrees with observations to within a factor of 2. It was hypothesized that the lifetime of dust, 2.6 days in our base case, is too short and causes the underestimation in remote areas. However, a sensitivity simulation with smaller dust particles and increased lifetime, 3.7 days, does not significantly improve the comparison. These results suggest that the underestimation of mineral dust in remote areas may result from local factors/sources not well described by the global dust source function used here or the GCM meteorology. The effect of dust aerosols on CCN(0.2%) concentrations is negligible in most regions of the globe; however, CCN(0.2%) concentrations change decrease by 10–20% in dusty regions the impact of dust on CCN(0.2%) concentrations in dusty regions is very sensitive to the assumed size distribution of emissions. If emissions are predominantly in the coarse mode, CCN(0.2%) decreases in dusty regions up to 10–20% because dust competes for condensable H<sub>2</sub>SO<sub>4</sub>, reducing the condensational growth of ultrafine mode particles to CCN sizes. With significant fine mode emissions, however, CCN(0.2%) doubles in Saharan source regions because the direct emission of dust particles outweighs any microphysical feedbacks. The impact of dust on CCN concentrations active at various water supersaturations is also investigated. Below 0.1%, CCN concentrations increase significantly in dusty regions due to the presence of coarse dust particles. Above 0.2%, CCN concentrations show a similar behavior as CCN(0.2%).
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We propose a new technique that overcomes the obstacles of the existing methods for monitoring near-surface water vapour, by estimating humidity from data collected through existing wireless communication networks. <br><br> Weather conditions and atmospheric phenomena affect the electromagnetic channel, causing attenuations to the radio signals. Thus, wireless communication networks are in effect built-in environmental monitoring facilities. The wireless microwave links, used in these networks, are widely deployed by cellular providers for backhaul communication between base stations, a few tens of meters above ground level. As a result, if all available measurements are used, the proposed method can provide moisture observations with high spatial resolution and potentially high temporal resolution. Further, the implementation cost is minimal, since the data used are already collected and saved by the cellular operators. In addition – many of these links are installed in areas where access is difficult such as orographic terrain and complex topography. As such, our method enables measurements in places that have been hard to measure in the past, or have never been measured before. The technique is restricted to weather conditions which exclude rain, fog or clouds along the propagation path. Strong winds that may cause movement of the link transmitter or receiver (or both) may also interfere with the ability to conduct accurate measurements. <br><br> We present results from real-data measurements taken from two microwave links used in a backhaul cellular network that show convincing correlation to surface station humidity measurements. The measurements were taken daily in two sites, one in northern Israel (28 measurements), the other in central Israel (29 measurements). The correlation between the microwave link measurements and the humidity gauges were 0.9 and 0.82 for the north and central sites, respectively. The Root Mean Square Differences (RMSD) were 1.8 g/m<sup>3</sup> and 3.4 g/m<sup>3</sup> for the northern and central site measurements, respectively.
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The influence of smoke on the aerosol loading in the free troposphere over Thessaloniki, Greece is examined in this paper. Ten cases during 2001–2005 were identified when very high aerosol optical depth values in the free troposphere were observed with a UV-Raman lidar. Particle dispersion modeling (FLEXPART) and satellite hot spot fire detection (ATSR) showed that these high free tropospheric aerosol optical depths are mainly attributed to the advection of smoke plumes from biomass burning regions over Thessaloniki. The biomass burning regions were found to extend across Russia in the latitudinal belt between 45° N–55° N, as well as in Eastern Europe (Baltic countries, Western Russia, Belarus, and the Ukraine). The highest frequency of agricultural fires occurred during the summer season (mainly in August). The data collected allowed the optical characterization of the smoke aerosols that arrived over Greece, where limited information has so far been available. Two-wavelength backscatter lidar measurements showed that the backscatter-related Ångström exponent ranged between 0.5 and 2.4 indicating a variety of particle sizes. UV-Raman lidar measurements showed that for smoke particles the extinction to backscatter ratios (so-called lidar ratios) varied between 40 sr for small particles to 100 sr for large particles. Dispersion model estimations of the carbon monoxide tracer concentration profiles for smoke particles indicate that the variability of the optical parameters is a function of the age of the smoke plumes. This information could be useful on the lidar community for reducing uncertainty in the aerosol backscatter coefficient determination due to the lidar ratio assumption, starting from a simply elastic backscatter lidar as the first satellite-borne lidar CALIPSO.
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Observations at a mountain-top site within the Mexico City basin are used to characterize ozone production and destruction, nitrogen oxide speciation and chemistry, and the radical budget, with an emphasis on a stagnant air mass observed on one afternoon. The observations compare well with the results of recent photochemical models. An ozone production rate of ~50 ppbv/h was observed in a stagnant air mass during the afternoon of 12 March 2006, which is among the highest observed anywhere in the world. Approximately half of the ozone destruction was due to the oxidation of NO<sub>2</sub>. During this time period ozone production was VOC-limited, deduced by a comparison of the radical production rates and the formation rate of NO<sub>x</sub> oxidation products (NO<sub>z</sub>). For [NO<sub>x</sub>]/[NO<sub>y</sub>] values between 0.2 and 0.8, gas-phase HNO<sub>3</sub> typically accounted for less than 10% of NO<sub>z</sub> and accumulation-mode particulate nitrate (NO<sub>3(PM1)</sub><sup>−</sup>) accounted for 20%–70% of NO<sub>z</sub>, consistent with high ambient NH<sub>3</sub> concentrations. The fraction of NO<sub>z</sub> accounted for by the sum of HNO<sub>3(g)</sub> and NO<sub>3(PM1)</sub><sup>−</sup> decreased with photochemical processing. This decrease is apparent even when dry deposition of HNO<sub>3</sub> is accounted for, and indicates that HNO<sub>3</sub> formation decreased relative to other NO<sub>x</sub> "sink" processes during the first 12 h of photochemistry and/or a significant fraction of the nitrate was associated with the coarse aerosol size mode. The ozone production efficiency of NO<sub>x</sub> on 11 and 12 March 2006 was approximately 7 on a time scale of one day. A new metric for ozone production efficiency that relates the dilution-adjusted ozone mixing ratio to cumulative OH exposure is proposed.
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Wet deposition is an important removal mechanism for atmospheric organic matter, and a potentially important input for receiving ecosystems, yet less than 50% of rainwater organic matter is considered chemically characterized. Precipitation samples collected in New Jersey, USA, were analyzed by negative ion ultra-high resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Elemental compositions of 552 unique molecular species were determined in the mass range 50–500 Da in the rainwater. Four main groups of organic compounds were identified: compounds containing carbon, hydrogen, and oxygen (CHO) only, sulfur (S) containing CHOS compounds, nitrogen (N) containing CHON compounds, and S- and N- containing CHONS compounds. Organic acids commonly identified in precipitation were detected in the rainwater. Within the four main groups of compounds detected in the rainwater, oligomers, organosulfates, and nitrooxy-organosulfates were assigned based on elemental formula comparisons. The majority of the compounds identified are products of atmospheric reactions and are known contributors to secondary organic aerosol (SOA) formed from gas phase, aerosol phase, and in-cloud reactions in the atmosphere. It is suggested that the large uncharacterized component of SOA is the main contributor to the large uncharacterized component of rainwater organic matter.
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Dust and black carbon aerosol have long been known to exert potentially important and diverse impacts on cloud droplet formation. Most studies to date focus on the soluble fraction of these particles, and overlook interactions of the insoluble fraction with water vapor (even if known to be hydrophilic). To address this gap, we developed a new parameterization that considers cloud droplet formation within an ascending air parcel containing insoluble (but wettable) particles externally mixed with aerosol containing an appreciable soluble fraction. Activation of particles with a soluble fraction is described through well-established Köhler theory, while the activation of hydrophilic insoluble particles is treated by "adsorption-activation" theory. In the latter, water vapor is adsorbed onto insoluble particles, the activity of which is described by a multilayer Frenkel-Halsey-Hill (FHH) adsorption isotherm modified to account for particle curvature. We further develop FHH activation theory to <i>i</i>) find combinations of the adsorption parameters <i>A</i><sub>FHH</sub>, <i>B</i><sub>FHH</sub> which yield atmospherically-relevant behavior, and, <i>ii</i>) express activation properties (critical supersaturation) that follow a simple power law with respect to dry particle diameter. <br><br> The new parameterization is tested by comparing the parameterized cloud droplet number concentration against predictions with a detailed numerical cloud model, considering a wide range of particle populations, cloud updraft conditions, water vapor condensation coefficient and FHH adsorption isotherm characteristics. The agreement between parameterization and parcel model is excellent, with an average error of 10% and <i>R</i><sup>2</sup>~0.98. A preliminary sensitivity study suggests that the sublinear response of droplet number to Köhler particle concentration is not as strong for FHH particles.
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Boreal spring climate is uniquely susceptible to solar warming mechanisms because it has expansive snow cover and receives relatively strong insolation. Carbonaceous particles can influence snow coverage by warming the atmosphere, reducing surface-incident solar energy (<i>dimming</i>), and reducing snow reflectance after deposition (<i>darkening</i>). We apply a range of models and observations to explore impacts of these processes on springtime climate, drawing several conclusions: 1) Nearly all atmospheric particles (those with visible-band single-scatter albedo less than 0.999), including all mixtures of black carbon (BC) and organic matter (OM), increase net solar heating of the atmosphere-snow column. 2) Darkening caused by small concentrations of particles within snow exceeds the loss of absorbed energy from concurrent dimming, thus increasing solar heating of snowpack as well (positive net surface forcing). Over global snow, we estimate 6-fold greater surface forcing from darkening than dimming, caused by BC+OM. 3) Equilibrium climate experiments suggest that fossil fuel and biofuel emissions of BC+OM induce 95% as much springtime snow cover loss over Eurasia as anthropogenic carbon dioxide, a consequence of strong snow-albedo feedback and large BC+OM emissions from Asia. 4) Of 22 climate models contributing to the IPCC Fourth Assessment Report, 21 underpredict the rapid warming (0.64°C decade<sup>−1</sup>) observed over springtime Eurasia since 1979. Darkening from natural and anthropogenic sources of BC and mineral dust exerts 3-fold greater forcing on springtime snow over Eurasia (3.9 W m<sup>−2</sup>) than North America (1.2 W m<sup>−2</sup>). Inclusion of this forcing significantly improves simulated continental warming trends, but does not reconcile the low bias in rate of Eurasian spring snow cover decline exhibited by all models, likely because BC deposition trends are negative or near-neutral over much of Eurasia. Improved Eurasian warming may therefore relate more to darkening-induced reduction in mean snow cover.
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We have conducted the first airborne hygroscopic growth closure study to utilize data from an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) coupled with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) measurements from the differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP). These data were collected off the coast of Central California during seven of the 16 flights carried out during the MASE-II field campaign in July 2007. Two of the seven flights were conducted in airmasses characterized by continental origin. These flights exhibited elevated organic volume fractions (VF<sub>organic</sub>=0.56±0.19, as opposed to 0.39±0.20 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61±0.14 at 92% RH, as compared with 1.91±0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53±0.10 at 85%, compared with 1.58±0.08 for all other flights), and no measurable GF suppression at low RH (1.31±0.06 at 74%, compared with 1.31±0.07 for all other flights). Organic loadings were slightly elevated in above-cloud aerosols, as compared with below-cloud aerosols, and corresponded to a similar trend of significantly suppressed GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided good agreement with DASH-SP measurements (<i>R</i><sup>2</sup>=0.78). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.22, 1.45, and 1.48 at 74, 85, and 92% RH, respectively. These values agree with previously reported values for water-soluble organics such as dicarboxylic and multifunctional acids, and correspond to a highly oxidized, presumably water-soluble, organic fraction (mission-averaged O:C=0.92±0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is VF<sub>organic</sub>, indicating that a simple emperical model relating GF, RH, and the relative abundance of organic material can provide accurate predictions (<i>R</i><sup>2</sup>=0.77) of hygroscopic growth for the California coast.
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Lagrangian particle dispersion models (LPDMs) are powerful and popular tools used for the analysis of atmospheric trace gas measurements. However, it can be difficult to determine the transport pathway of emissions from their source to a receptor using the standard gridded model output, particularly during complex meteorological scenarios. In this paper we present a method to clearly and easily identify the pathway taken by only those emissions that arrive at a receptor at a particular time, by combining the standard gridded output from forward (e.g., concentration) and backward (e.g., residence time) LPDM simulations. By comparing the pathway determined from this method with particle trajectories from both the forward and backward models, we show that this method successfully restores much of the Lagrangian information that is lost when the data are gridded. A sample analysis is presented, demonstrating that the source-to-receptor pathway determined from this method is more accurate and easier to use than existing methods using standard LPDM products (gridded fields of, e.g., concentrations and residence time). As demonstrated in an evaluation and an example application, the method requires agreement between the transport described by the forward and backward simulations and thus provides a means to assess the quality and reversibility of the simulation. Finally, we discuss the potential for combining the backward LPDM simulation with gridded data from other sources (e.g., chemical transport models) to obtain a Lagrangian sampling of the air that will eventually arrive at a receptor. Based on the advantages presented here, this new method can complement or even replace many of the standard uses of backward LPDM simulations.
