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Atmospheric waves as scaling, turbulent phenomena

It is paradoxical that, while atmospheric dynamics are highly nonlinear and turbulent, atmospheric waves are commonly modelled by linear or weakly nonlinear theories. We postulate that the laws governing atmospheric waves are in fact high-Reynolds-number (Re), emergent laws so that – in common with the emergent high-Re turbulent laws – they are also constrained by scaling symmetries. We propose an effective turbulence–wave propagator which corresponds to a fractional and anisotropic extension of the classical wave equation propagator, with dispersion relations similar to those of inertial gravity waves (and Kelvin waves) yet with an anomalous (fractional) order Hwav/2. Using geostationary IR radiances, we estimate the parameters, finding that Hwav ≈ 0.17 ± 0.04 (the classical value = 2).
Arctic stratospheric dehydration – Part 2: Microphysical modeling

Large areas of synoptic-scale ice PSCs (polar stratospheric clouds) distinguished the Arctic winter 2009/2010 from other years and revealed unprecedented evidence of water redistribution in the stratosphere. A unique snapshot of water vapor repartitioning into ice particles was obtained under extremely cold Arctic conditions with temperatures around 183 K. Balloon-borne, aircraft and satellite-based measurements suggest that synoptic-scale ice PSCs and concurrent reductions and enhancements in water vapor are tightly linked with the observed de- and rehydration signatures, respectively. In a companion paper (Part 1), water vapor and aerosol backscatter measurements from the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) and LAPBIAT-II (Lapland Atmosphere–Biosphere Facility) field campaigns have been analyzed in detail. This paper uses a column version of the Zurich Optical and Microphysical box Model (ZOMM) including newly developed NAT (nitric acid trihydrate) and ice nucleation parameterizations. Particle sedimentation is calculated in order to simulate the vertical redistribution of chemical species such as water and nitric acid. Despite limitations given by wind shear and uncertainties in the initial water vapor profile, the column modeling unequivocally shows that (1) accounting for small-scale temperature fluctuations along the trajectories is essential in order to reach agreement between simulated optical cloud properties and observations, and (2) the use of recently developed heterogeneous ice nucleation parameterizations allows the reproduction of the observed signatures of de- and rehydration. Conversely, the vertical redistribution of water measured cannot be explained in terms of homogeneous nucleation of ice clouds, whose particle radii remain too small to cause significant dehydration.
Global lightning NOx production estimated by an assimilation of multiple satellite data sets

The global source of lightning-produced NOx (LNOx) is estimated by assimilating observations of NO2, O3, HNO3, and CO measured by multiple satellite measurements into a chemical transport model. Included are observations from the Ozone Monitoring Instrument (OMI), Microwave Limb Sounder (MLS), Tropospheric Emission Spectrometer (TES), and Measurements of Pollution in the Troposphere (MOPITT) instruments. The assimilation of multiple chemical data sets with different vertical sensitivity profiles provides comprehensive constraints on the global LNOx source while improving the representations of the entire chemical system affecting atmospheric NOx, including surface emissions and inflows from the stratosphere. The annual global LNOx source amount and NO production efficiency are estimated at 6.3 Tg N yr−1 and 310 mol NO flash−1, respectively. Sensitivity studies with perturbed satellite data sets, model and data assimilation settings lead to an error estimate of about 1.4 Tg N yr−1 on this global LNOx source. These estimates are significantly different from those estimated from a parameter inversion that optimizes only the LNOx source from NO2 observations alone, which may lead to an overestimate of the source adjustment. The total LNOx source is predominantly corrected by the assimilation of OMI NO2 observations, while TES and MLS observations add important constraints on the vertical source profile. The results indicate that the widely used lightning parameterization based on the C-shape assumption underestimates the source in the upper troposphere and overestimates the peak source height by up to about 1 km over land and the tropical western Pacific. Adjustments are larger over ocean than over land, suggesting that the cloud height dependence is too weak over the ocean in the Price and Rind (1992) approach. The significantly improved agreement between the analyzed ozone fields and independent observations gives confidence in the performance of the LNOx source estimation.
Chemical ozone loss and ozone mini-hole event during the Arctic winter 2010/2011 as observed by SCIAMACHY and GOME-2

Record breaking loss of ozone (O3) in the Arctic stratosphere has been reported in winter–spring 2010/2011. We examine in detail the composition and transformations occurring in the Arctic polar vortex using total column and vertical profile data products for O3, bromine oxide (BrO), nitrogen dioxide (NO2), chlorine dioxide (OClO), and polar stratospheric clouds (PSC) retrieved from measurements made by SCIAMACHY (Scanning Imaging Absorption SpectroMeter for Atmospheric CHartography) on-board Envisat (Environmental Satellite), as well as total column ozone amount, retrieved from the measurements of GOME-2 (Global Ozone Monitoring Experiment) on MetOp-A (Meteorological Experimental Satellite). Similarly we use the retrieved data from DOAS (Differential Optical Absorption Spectroscopy) measurements made in Ny-Ålesund (78.55° N, 11.55° E). A chemical transport model (CTM) has been used to relate and compare Arctic winter–spring conditions in 2011 with those in the previous year. In late winter–spring 2010/2011 the chemical ozone loss in the polar vortex derived from SCIAMACHY observations confirms findings reported elsewhere. More than 70% of O3 was depleted by halogen catalytic cycles between the 425 and 525 K isentropic surfaces, i.e. in the altitude range ~16–20 km. In contrast, during the same period in the previous winter 2009/2010, a typical warm Arctic winter, only slightly more than 20% depletion occurred below 20 km, while 40% of O3 was removed above the 575 K isentrope (~23 km). This loss above 575 K is explained by the catalytic destruction by NOx descending from the mesosphere. In both Arctic winters 2009/2010 and 2010/2011, calculated O3 losses from the CTM are in good agreement to our observations and other model studies. The mid-winter 2011 conditions, prior to the catalytic cycles being fully effective, are also investigated. Surprisingly, a significant loss of O3 around 60%, previously not discussed in detail, is observed in mid-January 2011 below 500 K (~19 km) and sustained for approximately 1 week. The low O3 region had an exceptionally large spatial extent. The situation was caused by two independently evolving tropopause elevations over the Asian continent. Induced adiabatic cooling of the stratosphere favoured the formation of PSC, increased the amount of active chlorine for a short time, and potentially contributed to higher polar ozone loss later in spring.
Numerical simulation of "an American haboob"

A dust storm of fearful proportions hit Phoenix in the early evening hours of 5 July 2011. This storm, an American haboob, was predicted hours in advance because numerical, land–atmosphere modeling, computing power and remote sensing of dust events have improved greatly over the past decade. High-resolution numerical models are required for accurate simulation of the small scales of the haboob process, with high velocity surface winds produced by strong convection and severe downbursts. Dust productive areas in this region consist mainly of agricultural fields, with soil surfaces disturbed by plowing and tracks of land in the high Sonoran Desert laid barren by ongoing draught. Model simulation of the 5 July 2011 dust storm uses the coupled atmospheric-dust model NMME–DREAM (Non-hydrostatic Mesoscale Model on E grid, Janjic et al., 2001; Dust REgional Atmospheric Model, Nickovic et al., 2001; Pérez et al., 2006) with 4 km horizontal resolution. A mask of the potentially dust productive regions is obtained from the land cover and the normalized difference vegetation index (NDVI) data from the Moderate Resolution Imaging Spectroradiometer (MODIS). The scope of this paper is validation of the dust model performance, and not use of the model as a tool to investigate mechanisms related to the storm. Results demonstrate the potential technical capacity and availability of the relevant data to build an operational system for dust storm forecasting as a part of a warning system. Model results are compared with radar and other satellite-based images and surface meteorological and PM10 observations. The atmospheric model successfully hindcasted the position of the front in space and time, with about 1 h late arrival in Phoenix. The dust model predicted the rapid uptake of dust and high values of dust concentration in the ensuing storm. South of Phoenix, over the closest source regions (~25 km), the model PM10 surface dust concentration reached ~2500 μg m−3, but underestimated the values measured by the PM10 stations within the city. Model results are also validated by the MODIS aerosol optical depth (AOD), employing deep blue (DB) algorithms for aerosol loadings. Model validation included Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), equipped with the lidar instrument, to disclose the vertical structure of dust aerosols as well as aerosol subtypes. Promising results encourage further research and application of high-resolution modeling and satellite-based remote sensing to warn of approaching severe dust events and reduce risks for safety and health.
Source apportionment of PM10 in a north-western Europe regional urban background site (Lens, France) using positive matrix factorization and including primary biogenic emissions

In this work, the source of ambient particulate matter (PM10) collected over a one-year period at an urban background site in Lens (France) was determined and investigated using a positive matrix factorization receptor model (US EPA PMF v3.0). In addition, a potential source contribution function (PSCF) was performed by means of the Hybrid Single-Particle Lagrangian Integrated Trajectory (Hysplit) v4.9 model to assess prevailing geographical origins of the identified sources. A selective iteration process was followed for the qualification of the more robust and meaningful PMF solution. Components measured and used in the PMF included inorganic and organic species: soluble ionic species, trace elements, elemental carbon (EC), sugar alcohols, sugar anhydride, and organic carbon (OC). The mean PM10 concentration measured from March 2011 to March 2012 was about 21 μg m−3 with typically OM, nitrate and sulfate contributing to most of the mass and accounting respectively for 5.8, 4.5 and 2.3 μg m−3 on a yearly basis. Accordingly, PMF outputs showed that the main emission sources were (in decreasing order of contribution) secondary inorganic aerosols (28% of the total PM10 mass), aged marine emissions (19%), with probably predominant contribution of shipping activities, biomass burning (13%), mineral dust (13%), primary biogenic emissions (9%), fresh sea salts (8%), primary traffic emissions (6%) and heavy oil combustion (4%). Significant temporal variations were observed for most of the identified sources. In particular, biomass burning emissions were negligible in summer but responsible for about 25% of total PM10 and 50% of total OC in wintertime. Conversely, primary biogenic emissions were found to be negligible in winter but to represent about 20% of total PM10 and 40% of total OC in summer. The latter result calls for more investigations of primary biogenic aerosols using source apportionment studies, which quite usually disregard this type of source. This study further underlines the major influence of secondary processes during daily threshold exceedances. Finally, apparent discrepancies that could be generally observed between filter-based studies (such as the present one) and aerosol mass spectrometer-based PMF analyses (organic fractions) are also discussed.
Wind extraction potential from 4D-Var assimilation of stratospheric O3, N2O, and H2O using a global shallow water model

The wind extraction due to assimilation of stratospheric trace gas (tracer) data is examined using a 4D-Var (four-dimensional variational) data assimilation system based on the shallow water equations coupled to the tracer continuity equation. The procedure is outlined as follows. First, a nature run is created, simulating middle stratospheric winter conditions. Second, ozone (O3), nitrous oxide (N2O), and water vapor (H2O) (treated in this study as passive tracers) are initialized using Aura Microwave Limb Sounder (MLS) mixing ratios at 850 K potential temperature and are advected by the nature run winds. Third, the initial dynamical conditions are perturbed by using a 6 h offset. Fourth, simulated hourly tracer observations on the full model grid are assimilated with a 4D-Var system in which tracer and winds are coupled via the adjoint of the tracer continuity equation. Multiple assimilation experiments are performed by varying the amount of random observation error added to the simulated measurements. Finally, the wind extraction potential (WEP) is calculated as the reduction of the vector wind root mean square error (RMSE) relative to the maximum possible reduction. For a single 6 h assimilation cycle with the smallest observation error, WEP values are ~60% for all three tracers, while 10-day multi-cycle simulations result in WEP of ~90%, wind errors of ~0.3 m s−1, and height errors of ~13 m. There is therefore sufficient information in the tracer fields to almost completely constrain the dynamics, even without direct assimilation of dynamical information. When realistic observation error is added (based on MLS precisions at 10 hPa), the WEP after 10 days is 90% for O3, 87% for N2O, and 72% for H2O. O3 and N2O provide more wind information than H2O due to stronger background gradients relative to the MLS precisions. The RMSE for wind reach a minimum level of ~0.3–0.9 m s−1 for the MLS precisions, suggesting a limit to which realistic tracers could constrain the winds, given complete global cover age. With higher observation noise levels, the WEP values decrease, but the impact on the winds is still positive up to noise levels of 100% (relative to the global mean value) when compared to the case of no data assimilation.
Analysis of the PKT correction for direct CO2 flux measurements over the ocean

Eddy covariance measurements of air–sea CO2 fluxes can be affected by cross-sensitivities of the CO2 measurement to water vapour, resulting in order-of-magnitude biases. Well-established causes for these biases are (i) cross-sensitivity of the broadband non-dispersive infrared sensors due to band-broadening and spectral overlap (commercial sensors typically correct for this) and (ii) the effect of air density fluctuations (removed by determining the dry air CO2 mixing ratio). Another bias related to water vapour fluctuations has recently been observed with open-path sensors, attributed to sea salt build-up and water films on sensor optics. Two very different approaches have been used to deal with these water vapour-related biases. Miller et al. (2010) employed a membrane drier to physically eliminate 97% of the water vapour fluctuations in the sample air before it entered a closed-path gas analyser. Prytherch et al. (2010a) employed the empirical (Peter K. Taylor, PKT) post-processing correction to correct open-path sensor data. In this paper, we test these methods side by side using data from the Surface Ocean Aerosol Production (SOAP) experiment in the Southern Ocean. The air–sea CO2 flux was directly measured with four closed-path analysers, two of which were positioned down-stream of a membrane dryer. The CO2 fluxes from the two dried gas analysers matched each other and were in general agreement with common parameterisations. The flux estimates from the un-dried sensors agreed with the dried sensors only during periods with low latent heat flux (&leq;7 W m−2). When latent heat flux was higher, CO2 flux estimates from the un-dried sensors exhibited large scatter and an order-of-magnitude bias. Applying the PKT correction to the flux data from the un-dried analysers did not remove the bias when compared to the data from the dried gas analyser. The results of this study demonstrate the validity of measuring CO2 fluxes using a pre-dried air stream and show that the PKT correction is not valid for the correction of CO2 fluxes.
On the temperature dependence of organic reactivity, nitrogen oxides, ozone production, and the impact of emission controls in San Joaquin Valley, California

The San Joaquin Valley (SJV) experiences some of the worst ozone air quality in the US, frequently exceeding the California 8 h standard of 70.4 ppb. To improve our understanding of trends in the number of ozone violations in the SJV, we analyze observed relationships between organic reactivity, nitrogen oxides (NOx), and daily maximum temperature in the southern SJV using measurements made as part of California at the Nexus of Air Quality and Climate Change in 2010 (CalNex-SJV). We find the daytime speciated organic reactivity with respect to OH during CalNex-SJV has a temperature-independent portion with molecules typically associated with motor vehicles being the major component. At high temperatures, characteristic of days with high ozone, the largest portion of the total organic reactivity increases exponentially with temperature and is dominated by small, oxygenated organics and molecules that are unidentified. We use this simple temperature classification to consider changes in organic emissions over the last and next decade. With the CalNex-SJV observations as constraints, we examine the sensitivity of ozone production (PO3) to future NOx and organic reactivity controls. We find that PO3 is NOx-limited at all temperatures on weekends and on weekdays when daily maximum temperatures are greater than 29 °C. As a consequence, NOx reductions are the most effective control option for reducing the frequency of future ozone violations in the southern SJV.
Chlorine as a primary radical: evaluation of methods to understand its role in initiation of oxidative cycles

The role of chlorine atoms (Cl) in atmospheric oxidation has been traditionally thought to be limited to the marine boundary layer, where they are produced through heterogeneous reactions involving sea salt. However, recent observation of photolytic Cl precursors (ClNO2 and Cl2) formed from anthropogenic pollution has expanded the potential importance of Cl to include coastal and continental urban areas. Measurements of ClNO2 in Los Angeles during CalNex (California Nexus – Research at the Nexus of Air Quality and Climate Change) showed it to be an important primary (first generation) radical source. Evolution of ratios of volatile organic compounds (VOCs) has been proposed as a method to quantify Cl oxidation, but we find no evidence from this approach for a significant role of Cl oxidation in Los Angeles. We use a box model with the Master Chemical Mechanism (MCM v3.2) chemistry scheme, constrained by observations in Los Angeles, to examine the Cl sensitivity of commonly used VOC ratios as a function of NOx and secondary radical production. Model results indicate VOC tracer ratios could not detect the influence of Cl unless the ratio of [OH] to [Cl] was less than 200 for at least a day. However, the model results also show that secondary (second generation) OH production resulting from Cl oxidation of VOCs is strongly influenced by NOx, and that this effect obscures the importance of Cl as a primary oxidant. Calculated concentrations of Cl showed a maximum in mid-morning due to a photolytic source from ClNO2 and loss primarily to reactions with VOCs. The [OH] to [Cl] ratio was below 200 for approximately 3 h in the morning, but Cl oxidation was not evident from the measured ratios of VOCs. Instead, model simulations show that secondary OH production causes VOC ratio evolution to follow that expected for OH oxidation, despite the significant input of primary Cl from ClNO2 photolysis in the morning. Even though OH is by far the dominant oxidant in Los Angeles, Cl atoms do play an important role in photochemistry there, constituting 9% of the primary radical source. Furthermore, Cl–VOC reactivity differs from that of OH, being more than an order of magnitude larger and dominated by VOCs, such as alkanes, that are less reactive toward OH. Primary Cl is also slightly more effective as a radical source than primary OH due to its greater propensity to initiate radical propagation chains via VOC reactions relative to chain termination via reaction with nitrogen oxides.