We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from −0.58 to −0.02 Wm−2, with a mean of −0.27 Wm−2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of −0.35 Wm−2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results

Abstract. The formation of secondary organic aerosol (SOA) from the oxidation of β-pinene via nitrate radicals is investigated in the Georgia Tech Environmental Chamber (GTEC) facility. Aerosol yields are determined for experiments performed under both dry (relative humidity (RH) < 2 %) and humid (RH = 50 % and RH = 70 %) conditions. To probe the effects of peroxy radical (RO2) fate on aerosol formation, "RO2 + NO3 dominant" and "RO2 + HO2 dominant" experiments are performed. Gas-phase organic nitrate species (with molecular weights of 215, 229, 231, and 245 amu, which likely correspond to molecular formulas of C10H17NO4, C10H15NO5, C10H17NO5, and C10H15NO6, respectively) are detected by chemical ionization mass spectrometry (CIMS) and their formation mechanisms are proposed. The NO+ (at m/z 30) and NO2+ (at m/z 46) ions contribute about 11 % to the combined organics and nitrate signals in the typical aerosol mass spectrum, with the NO+ : NO2+ ratio ranging from 4.8 to 10.2 in all experiments conducted. The SOA yields in the "RO2 + NO3 dominant" and "RO2 + HO2 dominant" experiments are comparable. For a wide range of organic mass loadings (5.1–216.1 μg m−3), the aerosol mass yield is calculated to be 27.0–104.1 %. Although humidity does not appear to affect SOA yields, there is evidence of particle-phase hydrolysis of organic nitrates, which are estimated to compose 45–74 % of the organic aerosol. The extent of organic nitrate hydrolysis is significantly lower than that observed in previous studies on photooxidation of volatile organic compounds in the presence of NOx. It is estimated that about 90 and 10 % of the organic nitrates formed from the β-pinene+NO3 reaction are primary organic nitrates and tertiary organic nitrates, respectively. While the primary organic nitrates do not appear to hydrolyze, the tertiary organic nitrates undergo hydrolysis with a lifetime of 3–4.5 h. Results from this laboratory chamber study provide the fundamental data to evaluate the contributions of monoterpene + NO3 reaction to ambient organic aerosol measured in the southeastern United States, including the Southern Oxidant and Aerosol Study (SOAS) and the Southeastern Center for Air Pollution and Epidemiology (SCAPE) study.

Abstract.We examine the formation of nitrate and ammonium on five types of externally mixed pre-existing aerosols using the hybrid dynamic method in a global chemistry transport model. The model developed here predicts a similar spatial pattern of total aerosol nitrate and ammonium to that of several pioneering studies, but separates the effects of nitrate and ammonium on pure sulfate, biomass burning, fossil fuel, dust and sea salt aerosols. Nitrate and ammonium boost the scattering efficiency of sulfate and organic matter but lower the extinction of sea salt particles since the hygroscopicity of a mixed nitrate-ammonium-sea salt particle is less than that of pure sea salt. The direct anthropogenic forcing of particulate nitrate and ammonium at the top of the atmosphere (TOA) is estimated to be −0.12 W m −2 . Nitrate, ammonium and nitric acid gas also affect aerosol activation and the reflectivity of clouds. The first aerosol indirect forcing by anthropogenic nitrate (gas plus aerosol) and ammonium is estimated to be −0.09 W m −2 at the TOA, almost all of which is due to condensation of nitric acid gas onto growing droplets (−0.08 W m −2 ).

Organic aerosols (OA) play an important role in climate change. However, very few calculations of global OA radiative forcing include secondary organic aerosol (SOA) or the light-absorbing part of OA (brown carbon). Here we use a global model to assess the radiative forcing associated with the change in primary organic aerosol (POA) and SOA between present-day and preindustrial conditions in both the atmosphere and the land snow/sea ice. Anthropogenic emissions are shown to substantially influence the SOA formation rate, causing it to increase by 29 Tg/yr (93%) since preindustrial times. We examine the effects of varying the refractive indices, size distributions for POA and SOA, and brown carbon fraction in SOA. The increase of SOA exerts a direct forcing ranging from À0.12 to À0.31 W m À2 and a first indirect forcing in warm-phase clouds ranging from À0.22 to À0.29 W m À2, with the range due to different assumed SOA size distributions and refractive indices. The increase of POA since preindustrial times causes a direct forcing varying from À0.06 to À0.11 W m À2, when strongly and weakly absorbing refractive indices for brown carbon are used. The change in the total OA exerts a direct forcing ranging from À0.14 to À0.40 W m À2 . The atmospheric absorption from brown carbon ranges from +0.22 to +0.57 W m À2 , which corresponds to 27%~70% of the black carbon (BC) absorption predicted in the model. The radiative forcing of OA deposited in land snow and sea ice ranges from +0.0011 to +0.0031 W m À2 or as large as 24% of the forcing caused by BC in snow and ice simulated by the model.

[1] Seasonal variations of snow cover fraction (SFC) over the Tibet Plateau (TP) are examined using the data acquired from the Moderate Resolution Imaging Spectroradiometer (MODIS) on the Terra spacecraft. In this study, we first evaluate the accuracy of the MODIS high-resolution snow cover data by comparing the data with in-situ Chinese snow observations. Results show that overall accuracy of MODIS snow data is about 90% over the TP area. Statistical analysis is then performed over the MODIS snow data during 2000 -2006. It is found that the most persistent snow cover is located in the southern and western edges of the TP within large mountain ridges and western part of Yarlung Zangbo valley. The higher SCFs are mostly concentrated in the regions where the elevation is higher than 6000 m. The duration for snow persistence varies in different elevation ranges and generally becomes longer with increases in the terrain elevation. Citation: Pu, Z., L. Xu, and V. V.Salomonson (2007), MODIS/Terra observed seasonal variations of snow cover over the Tibetan Plateau, Geophys. Res. Lett., 34, L06706,

We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 15 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 15 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from &minus;0.58 to &minus;0.02 W m^&minus;2, with a mean of &minus;0.30 W m^&minus;2 for the 15 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of &minus;0.39 W m^&minus;2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results

Satellite-based estimates of the aerosol indirect effect (AIE) are consistently smaller than the estimates from global aerosol models, and, partly as a result of these differences, the assessment of this climate forcing includes large uncertainties. Satellite estimates typically use the present-day (PD) relationship between observed cloud drop number concentrations (N c ) and aerosol optical depths (AODs) to determine the preindustrial (PI) values of N c . These values are then used to determine the PD and PI cloud albedos and, thus, the effect of anthropogenic aerosols on top of the atmosphere radiative fluxes. Here, we use a model with realistic aerosol and cloud processes to show that empirical relationships for lnðN c Þ versus lnðAODÞ derived from PD results do not represent the atmospheric perturbation caused by the addition of anthropogenic aerosols to the preindustrial atmosphere. As a result, the model estimates based on satellite methods of the AIE are between a factor of 3 to more than a factor of 6 smaller than model estimates based on actual PD and PI values for N c . Using lnðN c Þ versus lnðAIÞ (Aerosol Index, or the optical depth times angstrom exponent) to estimate preindustrial values for N c provides estimates for N c and forcing that are closer to the values predicted by the model. Nevertheless, the AIE using lnðN c Þ versus lnðAIÞ may be substantially incorrect on a regional basis and may underestimate or overestimate the global average forcing by 25 to 35%.A n increase in aerosol concentrations leads to an increase in cloud droplet number concentration (N c ) for a cloud with a constant cloud liquid water content. The increase in N c implies a decrease in the cloud droplet effective radius, which leads to an increase in cloud optical depth and an increase in cloud reflectivity (1); this climate forcing is known as the first aerosol indirect effect (AIE).Satellite measurements of N c versus aerosol optical depth (AOD) have been used to estimate the effect of changes in clouds due to anthropogenic aerosols. The estimated changes to clouds from preindustrial (PI) to present-day (PD) conditions gives an AIE that ranges from −0.2 Wm −2 to −0.5 Wm −2 at the top of the atmosphere (TOA) (2, 3). In contrast, model results that rely on mechanistic descriptions of the relationship between aerosols and cloud drop number concentrations give an AIE that ranges from −0.5 to −2.03 Wm −2 (4, 5).Satellite-based estimates rely on a linear fit to the spatial variation of lnðN c Þ versus lnðAODÞ in the PD to determine PI values for N c , rather than temporal variations induced by actual changes between PD and PI aerosol concentrations. Improved estimates from satellites are expected if measurements of N c versus AI (where AI is the Aerosol Index, or the angstrom exponent times AOD) are used rather than N c versus AOD, because AI is a better measure of aerosol number concentration (6), but can still give values smaller than process-based models. Previous studies have attempted to combine satellite data with model...

Wearable biosensors as a user-friendly measurement platform have become a rapidly growing field of interests due to their possibility in integrating traditional medical diagnostics and healthcare management into miniature lab-on-body analytic devices. This paper demonstrates a flexible and skin-mounted band that combines superhydrophobic-superhydrophilic microarrays with nanodendritic colorimetric biosensors toward in situ sweat sampling and analysis. Particularly, on the superwettable bands, the superhydrophobic background could confine microdroplets into superhydrophilic microwells. On-body investigations further reveal that the secreted sweat is repelled by the superhydrophobic silica coating and precisely collected and sampled onto the superhydrophilic micropatterns with negligible lateral spreading, which provides an independent “vessel” toward cellphone-based sweat biodetection (pH, chloride, glucose and calcium). Such wearable, superwettable band-based biosensors with improved interface controllability could significantly enhance epidemical sweat sampling in well-defined sites, holding a great promise for facile and noninvasive biofluids analysis.