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Measuring the specific surface area of snow with X-ray tomography and gas adsorption: comparison and implications for surface smoothness

Chemical and physical processes, such as heterogeneous chemical reactions, light scattering, and metamorphism occur in the natural snowpack. To model these processes in the snowpack, the specific surface area (SSA) is a key parameter. In this study, two methods, computed tomography and methane adsorption, which have intrinsically different effective resolutions – molecular and 30 μm, respectively – were used to determine the SSA of similar natural snow samples. Except for very fresh snow, the two methods give identical results, with an uncertainty of 3%. This implies that the surface of aged natural snow is smooth up to a scale of about 30 μm and that if smaller structures are present they do not contribute significantly to the overall SSA. It furthermore implies that for optical methods a voxel size of 10 μm is sufficient to capture all structural features of this type of snow; however, fresh precipitation appears to contain small features that cause an under-estimation of SSA with tomography at this resolution. The methane adsorption method is therefore superior to computed tomography for very fresh snow having high SSA. Nonetheless, in addition to SSA determination, tomography provides full geometric information about the ice matrix. It can also be advantageously used to investigate layered snow packs, as it allows measuring SSA in layers of less than 1 mm.
Cloud type comparisons of AIRS, CloudSat, and CALIPSO cloud height and amount

The precision of the two-layer cloud height fields derived from the Atmospheric Infrared Sounder (AIRS) is explored and quantified for a five-day set of observations. Coincident profiles of vertical cloud structure by CloudSat, a 94 GHz profiling radar, and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), are compared to AIRS for a wide range of cloud types. Bias and variability in cloud height differences are shown to have dependence on cloud type, height, and amount, as well as whether CloudSat or CALIPSO is used as the comparison standard. The CloudSat-AIRS biases and variability range from −4.3 to 0.5±1.2–3.6 km for all cloud types. Likewise, the CALIPSO-AIRS biases range from 0.6–3.0±1.2–3.6 km (−5.8 to −0.2±0.5–2.7 km) for clouds ≥7 km (<7 km). The upper layer of AIRS has the greatest sensitivity to Altocumulus, Altostratus, Cirrus, Cumulonimbus, and Nimbostratus, whereas the lower layer has the greatest sensitivity to Cumulus and Stratocumulus. Although the bias and variability generally decrease with increasing cloud amount, the ability of AIRS to constrain cloud occurrence, height, and amount is demonstrated across all cloud types for many geophysical conditions. In particular, skill is demonstrated for thin Cirrus, as well as some Cumulus and Stratocumulus, cloud types infrared sounders typically struggle to quantify. Furthermore, some improvements in the AIRS Version 5 operational retrieval algorithm are demonstrated. However, limitations in AIRS cloud retrievals are also revealed, including the existence of spurious Cirrus near the tropopause and low cloud layers within Cumulonimbus and Nimbostratus clouds. Likely causes of spurious clouds are identified and the potential for further improvement is discussed.
Clouds and aerosols in Puerto Rico – a new evaluation

The influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and behaviour of clouds and their influence on climate. In an attempt to better understand warm cloud formation in a tropical marine environment, a period of intensive measurements took place in December 2004 in Puerto Rico, using some of the latest developments in online instrumentation such as aerosol mass spectrometers, cloud condensation nuclei counters and a hygroscopicity tandem differential mobility analyser. Simultaneous online measurements of aerosol size distributions, composition, hygroscopicity and optical properties were made near the lighthouse of Cape San Juan in the north-eastern corner of the island and at the top of East Peak mountain (1040 m a.s.l.), the two sites separated by 17 km. Additional measurements of the cloud droplet residual and interstitial aerosol properties were made at the mountain site, accompanied by measurements of cloud droplet size distributions, liquid water content and the chemical composition of cloud and rain water samples. Both aerosol composition and cloud properties were found to be sensitive to wind sector. Air from the east-northeast (ENE) was mostly free of anthropogenic influences, the submicron fraction being mainly composed of non-sea salt sulphate, while that from the east-southeast (ESE) was found to be moderately influenced by populated islands upwind, adding smaller (<100 nm), externally mixed, carbonaceous particles to the aerosol that increased the number concentrations by over a factor of 3. This change in composition was also accompanied with a reduction in the measured hygroscopicity and fractional cloud activation potential of the aerosol. At the mountain site, the average cloud droplet concentrations increased from 193 to 519 cm−3, median volume diameter decreased from 20 to 14 μm and the liquid water content increased from 0.24 to 0.31 g m−3 when the winds shifted from the ENE to ESE. Larger numbers of interstitial particles were recorded, most notably at sizes greater than 100 nm, which were absent during clean conditions. The average size of the residual particles and concentrations of cloudwater nitrate, sulphate and insoluble material increased during polluted conditions. Previous studies in Puerto Rico had reported the presence of a significant non-anthropogenic organic fraction in the aerosols measured and concluded that this was a factor controlling the in situ cloud properties. However, this was not observed in our case. In contrast to the 1.00±0.14 μg m−3 of organic carbon measured in 1992 and 1995, the organic matter measured in the current study of 0.17±0.35 μg m−3 is many times lower, most of which can be attributed to anthropogenic sources. During clean conditions, the submicron aerosol was observed to be almost entirely inorganic, an observation supported by the hygroscopicity measurements. This suggests that organic aerosols from marine sources may not be completely ubiquitous (either spatially or temporally) in this environment and requires further investigation to quantify their true extent and implications, with more extensive, longer-term sampling in conjunction with wind field analyses.
Global isoprene emissions estimated using MEGAN, ECMWF analyses and a detailed canopy environment model

The global emissions of isoprene are calculated at 0.5° resolution for each year between 1995 and 2006, based on the MEGAN (Model of Emissions of Gases and Aerosols from Nature) version 2 model (Guenther et al., 2006) and a detailed multi-layer canopy environment model for the calculation of leaf temperature and visible radiation fluxes. The calculation is driven by meteorological fields – air temperature, cloud cover, downward solar irradiance, windspeed, volumetric soil moisture in 4 soil layers – provided by analyses of the European Centre for Medium-Range Weather Forecasts (ECMWF). The estimated annual global isoprene emission ranges between 374 Tg (in 1996) and 449 Tg (in 1998 and 2005), for an average of ca. 410 Tg/year over the whole period, i.e. about 30% less than the standard MEGAN estimate (Guenther et al., 2006). This difference is due, to a large extent, to the impact of the soil moisture stress factor, which is found here to decrease the global emissions by more than 20%. In qualitative agreement with past studies, high annual emissions are found to be generally associated with El Niño events. The emission inventory is evaluated against flux measurement campaigns at Harvard forest (Massachussets) and Tapajós in Amazonia, showing that the model can capture quite well the short-term variability of emissions, but that it fails to reproduce the observed seasonal variation at the tropical rainforest site, with largely overestimated wet season fluxes. The comparison of the HCHO vertical columns calculated by a chemistry and transport model (CTM) with HCHO distributions retrieved from space provides useful insights on tropical isoprene emissions. For example, the relatively low emissions calculated over Western Amazonia (compared to the corresponding estimates in the inventory of Guenther et al., 1995) are validated by the excellent agreement found between the CTM and HCHO data over this region. The parameterized impact of the soil moisture stress on isoprene emissions is found to reduce the model/data bias over Australia, but it leads to underestimated emissions near the end of the dry season over subtropical Africa.
Modelling sea salt aerosol and its direct and indirect effects on climate

A size-dependent sea salt aerosol parameterization was developed based on the piecewise log-normal approximation (PLA) for aerosol size distributions. Results of this parameterization from simulations with a global climate model produce good agreement with observations at the surface and for vertically-integrated volume size distributions. The global and annual mean of the sea salt burden is 10.1 mg m−2. The direct radiative forcing is calculated to be −1.52 and −0.60 W m−2 for clear sky and all sky, respectively. The first indirect radiative forcing is about twice as large as the direct forcing for all-sky (−1.34 W m−2). The results also show that the total indirect forcing of sea salt is −2.9 W m−2 if climatic feedbacks are taken into account. The sensitivity of the forcings to changes in the burdens and sizes of sea salt particles was also investigated based on additional simulations with a different sea salt source function.
Hydrogen isotope fractionation in the photolysis of formaldehyde

Experiments investigating the isotopic fractionation in the formation of H2 by the photolysis of CH2O under tropospheric conditions are reported and discussed. The deuterium (D) depletion in the H2 produced is 500(±20)&permil; with respect to the parent CH2O. We also observed that complete photolysis of CH2O under atmospheric conditions produces H2 that has virtually the same isotope ratio as that of the parent CH2O. These findings imply that there must be a very strong concomitant isotopic enrichment in the radical channel (CH2O+hν → CHO+H) as compared to the molecular channel (CH2O+hν → H2+CO) of the photolysis of CH2O in order to balance the relatively small isotopic fractionation in the competing reaction of CH2O with OH. Using a 1-box photochemistry model we calculated the isotopic fractionation factor for the radical channel to be 0.22(±0.08), which is equivalent to a 780(±80)&permil; enrichment in D of the remaining CH2O. When CH2O is in photochemical steady state, the isotope ratio of the H2 produced is determined not only by the isotopic fractionation occurring during the photolytical production of H2 (αm) but also by overall fractionation for the removal processes of CH2O (αf), and is represented by the ratio of αm/αf. Applying the isotopic fractionation factors relevant to CH2O photolysis obtained in the present study to the troposphere, the ratio of αm/αf varies from ~0.8 to ~1.2 depending on the fraction of CH2O that reacts with OH and that produces H2. This range of αm/αf can render the H2 produced from the photochemical oxidation of CH4 to be enriched in D (with respect to the original CH4) by the factor of 1.2–1.3 as anticipated in the literature.
Trends and variability of midlatitude stratospheric water vapour deduced from the re-evaluated Boulder balloon series and HALOE

This paper presents an updated trend analysis of water vapour in the lower midlatitude stratosphere from the Boulder balloon-borne NOAA frostpoint hygrometer measurements and from the Halogen Occulation Experiment (HALOE). Two corrections for instrumental bias are applied to homogenise the frostpoint data series, and a quality assessment of all soundings after 1991 is presented. Linear trend estimates based on the corrected data for the period 1980–2000 are up to 40% lower than previously reported. Vertically resolved trends and variability are calculated with a multi regression analysis including the quasi-biennal oscillation and equivalent latitude as explanatory variables. In the range of 380 to 640 K potential temperature (≈14 to 25 km), the frostpoint data from 1981 to 2006 show positive linear trends between 0.3±0.3 and 0.7±0.1%/yr. The same dataset shows trends between −0.2±0.3 and 1.0±0.3%/yr for the period 1992 to 2005. HALOE data over the same time period suggest negative trends ranging from −1.1±0.2 to −0.1±0.1%/yr. In the lower stratosphere, a rapid drop of water vapour is observed in 2000/2001 with little change since. At higher altitudes, the transition is more gradual, with slowly decreasing concentrations between 2001 and 2007. This pattern is consistent with a change induced by a drop of water concentrations at entry into the stratosphere. Previously noted differences in trends and variability between frostpoint and HALOE remain for the homogenised data. Due to uncertainties in reanalysis temperatures and stratospheric transport combined with uncertainties in observations, no quantitative inference about changes of water entering the stratosphere in the tropics could be made with the mid latitude measurements analysed here.
Applications of lagrangian dispersion modeling to the analysis of changes in the specific absorption of elemental carbon

We use a Lagrangian dispersion model driven by a mesoscale model with four-dimensional data assimilation to simulate the dispersion of elemental carbon (EC) over a region encompassing Mexico City and its surroundings. The region was the study domain for the 2006 MAX-MEX experiment, which was a component of the MILAGRO campaign. The results are used to identify periods when biomass burning was likely to have had a significant impact on the concentrations of elemental carbon at two sites, T1 and T2, downwind of the city, and when emissions from the Mexico City Metropolitan Area (MCMA) were likely to have been more important. They are also used to estimate the median ages of EC affecting the specific absorption of light, αABS, at 870 nm as well as to identify periods when the urban plume from the MCMA was likely to have been advected over T1 and T2. Median EC ages at T1 and T2 are substantially larger during the day than at night. Values of αABS at T1, the nearer of the two sites to Mexico City, were smaller at night and increased rapidly after mid-morning, peaking in the mid-afternoon. The behavior is attributed to the coating of aerosols with substances such as sulfate or organic carbon during daylight hours, but such coating appears to be limited or absent at night. Evidence for this is provided by scanning electron microscopy images of aerosols collected at the sampling sites. During daylight hours the values of αABS did not increase with aerosol age for median ages in the range of 1–4 h. There is some evidence for absorption increasing as aerosols were advected from T1 to T2 but the statistical significance of that result is not strong.
A long-term comparison of wind and tide measurements in the upper mesosphere recorded with an imaging Doppler interferometer and SuperDARN radar at Halley, Antarctica

Data from a near co-located imaging Doppler interferometer (IDI) and SuperDARN radar recorded since 1996 have been analysed in a consistent manner to compare the derived mean winds and tides in the upper mesosphere. By comparing only days when both techniques were recording good quality meridional wind data it is shown that the SuperDARN radar winds and tides correlate best with the IDI height bin 90–95 km. On timescales of one hour the winds derived from the IDI have a much greater associated variance and correlate poorly with the SuperDARN winds. Regression analysis reveals that the observed SuperDARN daily mean meridional wind strength is approximately 65% that recorded by the IDI, in good quantitative agreement with previous studies which have shown contamination to SuperDARN derived winds due to the significant back lobe of the radar radiation pattern. Climatologically the two techniques observe similar monthly mean winds with the SuperDARN meridional winds suppressed compared to the IDI which tends to record winds more poleward than those derived by the SuperDARN radar during the summer months, and to be slightly more equatorward during the winter. The 12-h tidal amplitude and phase derived from both techniques are in good agreement, whereas the 24-h tides are seen much more strongly in the SuperDARN radar, especially in wintertime, with poor phase agreement. Long term comparison of the two techniques reveals a tendency for the IDI meridional winds to be more poleward during solar maximum especially during summer time; an effect which is not reproduced in the meridional winds derived from the SuperDARN radar. These results are discussed in the context of previous studies to independently determine the veracity of each technique, and to highlight the circumstances where data derived from these two techniques can be used to draw reliable conclusions from comparative studies based on geographically distributed pairs of instruments.
Seasonal and diurnal variations of Hg° over New England

Factors influencing diurnal to interannual variability in Hg° over New England were investigated using multi-year measurements conducted by AIRMAP at the Thompson Farm (TF) coastal site, an inland elevated site at Pac Monadnock (PM), and two month measurements on Appledore Island (AI) in the Gulf of Maine. Mixing ratios of Hg° at TF showed distinct seasonality with maxima in March and minima in October. Hg° at AI tracked the trend at TF but with higher minima, while at PM the diurnal and annual cycles were dampened. In winter, Hg° was correlated most strongly with CO and NOy, indicative of anthropogenic emissions as their primary source. Our analysis indicates that Hg° had a regional background level of ~160 fmol/mol in winter, a dry deposition velocity of ~0.20 cm s−1 with a ~16 day lifetime in the coastal boundary layer in summer. The influence of oceanic emissions on ambient Hg° levels was identified using the Hg°-CHBr3 correlation at both TF and AI. Moreover, the lower Hg° levels and steeper decreasing warm season trend at TF (0.5–0.6 fmol/mol d−1) compared to PM (0.2–0.3 fmol/mol d−1) likely reflected the impact of marine halogen chemistry. Large interannual variability in warm season Hg° levels in 2004 versus 2005/2006 may be due to the role of precipitation patterns in influencing surface evasion of Hg°. In contrast, changes in wintertime maximum levels of Hg° were small compared to drastic reductions in CO, CO2, NOy, and SO2 from 2004/2005 to 2006/2007. These trends could be explained by a homogeneous distribution of Hg° over North American in winter due to its long lifetime and/or rapid removal of reactive mercury from anthropogenic sources. We caution that during warmer winters, the Hg°-CO slope possibly reflects Hg° loss relative to changes in CO more than their emission ratio.