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Assessment of small-scale integrated water vapour variability during HOPE

The spatio-temporal variability of integrated water vapour (IWV) on small scales of less than 10 km and hours is assessed with data from the 2 months of the High Definition Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE). The statistical intercomparison of the unique set of observations during HOPE (microwave radiometer (MWR), Global Positioning System (GPS), sun photometer, radiosondes, Raman lidar, infrared and near-infrared Moderate Resolution Imaging Spectroradiometer (MODIS) on the satellites Aqua and Terra) measuring close together reveals a good agreement in terms of random differences (standard deviation &leq;1 kg m−2) and correlation coefficient (&geq; 0.98). The exception is MODIS, which appears to suffer from insufficient cloud filtering. For a case study during HOPE featuring a typical boundary layer development, the IWV variability in time and space on scales of less than 10 km and less than 1 h is investigated in detail. For this purpose, the measurements are complemented by simulations with the novel ICOsahedral Nonhydrostatic modelling framework (ICON), which for this study has a horizontal resolution of 156 m. These runs show that differences in space of 3–4 km or time of 10–15 min induce IWV variabilities on the order of 0.4 kg m−2. This model finding is confirmed by observed time series from two MWRs approximately 3 km apart with a comparable temporal resolution of a few seconds. Standard deviations of IWV derived from MWR measurements reveal a high variability (> 1 kg m−2) even at very short time scales of a few minutes. These cannot be captured by the temporally lower-resolved instruments and by operational numerical weather prediction models such as COSMO-DE (an application of the Consortium for Small-scale Modelling covering Germany) of Deutscher Wetterdienst, which is included in the comparison. However, for time scales larger than 1 h, a sampling resolution of 15 min is sufficient to capture the mean standard deviation of IWV. The present study shows that instrument sampling plays a major role when climatological information, in particular the mean diurnal cycle of IWV, is determined.
How emissions, climate, and land use change will impact mid-century air quality over the United States: a focus on effects at national parks

We use a global coupled chemistry–climate–land model (CESM) to assess the integrated effect of climate, emissions and land use changes on annual surface O3 and PM2.5 in the United States with a focus on national parks (NPs) and wilderness areas, using the RCP4.5 and RCP8.5 projections. We show that, when stringent domestic emission controls are applied, air quality is predicted to improve across the US, except surface O3 over the western and central US under RCP8.5 conditions, where rising background ozone counteracts domestic emission reductions. Under the RCP4.5 scenario, surface O3 is substantially reduced (about 5 ppb), with daily maximum 8 h averages below the primary US Environmental Protection Agency (EPA) National Ambient Air Quality Standards (NAAQS) of 75 ppb (and even 65 ppb) in all the NPs. PM2.5 is significantly reduced in both scenarios (4 μg m−3; ~50%), with levels below the annual US EPA NAAQS of 12 μg m−3 across all the NPs; visibility is also improved (10–15 dv; >75 km in visibility range), although some western US parks with Class I status (40–74 % of total sites in the US) are still above the 2050 planned target level to reach the goal of natural visibility conditions by 2064. We estimate that climate-driven increases in fire activity may dominate summertime PM2.5 over the western US, potentially offsetting the large PM2.5 reductions from domestic emission controls, and keeping visibility at present-day levels in many parks. Our study indicates that anthropogenic emission patterns will be important for air quality in 2050. However, climate and land use changes alone may lead to a substantial increase in surface O3 (2–3 ppb) with important consequences for O3 air quality and ecosystem degradation at the US NPs. Our study illustrates the need to consider the effects of changes in climate, vegetation, and fires in future air quality management and planning and emission policy making.
Biomass burning related ozone damage on vegetation over the Amazon forest: a model sensitivity study

The HadGEM2 earth system climate model was used to assess the impact of biomass burning on surface ozone concentrations over the Amazon forest and its impact on vegetation, under present-day climate conditions. Here we consider biomass burning emissions from wildfires, deforestation fires, agricultural forest burning, and residential and commercial combustion. Simulated surface ozone concentration is evaluated against observations taken at two sites in the Brazilian Amazon forest for years 2010 to 2012. The model is able to reproduce the observed diurnal cycle of surface ozone mixing ratio at the two sites, but overestimates the magnitude of the monthly averaged hourly measurements by 5–15 ppb for each available month at one of the sites. We vary biomass burning emissions over South America by ±20, 40, 60, 80 and 100% to quantify the modelled impact of biomass burning on surface ozone concentrations and ozone damage on vegetation productivity over the Amazon forest. We used the ozone damage scheme in the "high" sensitivity mode to give an upper limit for this effect. Decreasing South American biomass burning emissions by 100% (i.e. to zero) reduces surface ozone concentrations (by about 15 ppb during the biomass burning season) and suggests a 15% increase in monthly mean net primary productivity averaged over the Amazon forest, with local increases up to 60%. The simulated impact of ozone damage from present-day biomass burning on vegetation productivity is about 230 TgC yr−1. Taking into account that uncertainty in these estimates is substantial, this ozone damage impact over the Amazon forest is of the same order of magnitude as the release of carbon dioxide due to fire in South America; in effect it potentially doubles the impact of biomass burning on the carbon cycle.
A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles

Given significant challenges with available measurements of aerosol acidity, proxy methods are frequently used to estimate the acidity of atmospheric particles. In this study, four of the most common aerosol acidity proxies are evaluated and compared: (1) the ion balance method, (2) the molar ratio method, (3) thermodynamic equilibrium models, and (4) the phase partitioning of ammonia. All methods are evaluated against predictions of thermodynamic models and against direct observations of aerosol–gas equilibrium partitioning acquired in Mexico City during the Megacity Initiative: Local and Global Research Objectives (MILAGRO) study. The ion balance and molar ratio methods assume that any deficit in inorganic cations relative to anions is due to the presence of H+ and that a higher H+ loading and lower cation / anion ratio both correspond to increasingly acidic particles (i.e., lower pH). Based on the MILAGRO measurements, no correlation is observed between H+ levels inferred with the ion balance and aerosol pH predicted by the thermodynamic models and NH3–NH4+ partitioning. Similarly, no relationship is observed between the cation / anion molar ratio and predicted aerosol pH. Using only measured aerosol chemical composition as inputs without any constraint for the gas phase, the E-AIM (Extended Aerosol Inorganics Model) and ISORROPIA-II thermodynamic equilibrium models tend to predict aerosol pH levels that are inconsistent with the observed NH3–NH4+ partitioning. The modeled pH values from both E-AIM and ISORROPIA-II run with gas + aerosol inputs agreed well with the aerosol pH predicted by the phase partitioning of ammonia. It appears that (1) thermodynamic models constrained by gas + aerosol measurements and (2) the phase partitioning of ammonia provide the best available predictions of aerosol pH. Furthermore, neither the ion balance nor the molar ratio can be used as surrogates for aerosol pH, and previously published studies with conclusions based on such acidity proxies may need to be reevaluated. Given the significance of acidity for chemical processes in the atmosphere, the implications of this study are important and far reaching.
Analysis of the ozone profile specifications in the WRF-ARW model and their impact on the simulation of direct solar radiation

Although ozone is an atmospheric gas with high spatial and temporal variability, mesoscale numerical weather prediction (NWP) models simplify the specification of ozone concentrations used in their shortwave schemes by using a few ozone profiles. In this paper, a two-part study is presented: (i) an evaluation of the quality of the ozone profiles provided for use with the shortwave schemes in the Advanced Research version of the Weather Research and Forecasting (WRF-ARW) model and (ii) an assessment of the impact of deficiencies in those profiles on the performance of model simulations of direct solar radiation. The first part compares simplified data sets used to specify the total ozone column in six schemes (i.e., Goddard, New Goddard, RRTMG, CAM, GFDL and Fu–Liou–Gu) with the Multi-Sensor Reanalysis data set during the period 1979–2008 examining the latitudinal, longitudinal and seasonal limitations in the ozone profile specifications of each parameterization. The results indicate that the maximum deviations are over the poles and show prominent longitudinal patterns in the departures due to the lack of representation of the patterns associated with the Brewer–Dobson circulation and the quasi-stationary features forced by the land–sea distribution, respectively. In the second part, the bias in the simulated direct solar radiation due to these deviations from the simplified spatial and temporal representation of the ozone distribution is analyzed for the New Goddard and CAM schemes using the Beer–Lambert–Bouguer law and for the GFDL using empirical equations. For radiative applications those simplifications introduce spatial and temporal biases with near-zero departures over the tropics throughout the year and increasing poleward with a maximum in the high middle latitudes during the winter of each hemisphere.
Sources and fluxes of organic nitrogen in precipitation over the southern East Sea/Sea of Japan

We measured total dissolved reactive nitrogen in precipitation samples collected at Uljin, a Korean coastal site upwind of the southern East Sea/Sea of Japan (EJS), selected as a representative study site of atmospheric deposition over the northwestern Pacific margin. NO3- was found to be the most abundant nitrogen species, followed by NH4+ and dissolved organic nitrogen (DON). Air-mass back-trajectory (AMBT) analysis revealed that a significant fraction of the inorganic nitrogen (NO3- and NH4+) originated from mainland Asia, whereas the DON was primarily derived from Korea. Using varimax-rotated factor analysis in combination with major ions as tracers, agricultural activities in Korea were identified as the primary sources of DON in these samples. In addition, a positive correlation was found at Uljin between the size of organic fraction in total reactive nitrogen and nitrogen to carbon atomic ratio in organic matter. This correlation has also been observed at other locations worldwide, implying the utilization potential of atmospheric organic nitrogen might increase with its proportion in total nitrogen. Combining wet deposition measurements in this study with literature values for dry deposition observed at a remote island in the EJS, the total atmospheric depositional flux of reactive nitrogen was estimated to be 115 mmol N m−2 yr−1 over the southern EJS. Our study sheds new light on the potentially significant contribution to primary productivity of the northwestern Pacific Ocean by atmospheric deposition of nitrogen, especially the organic fraction.
Evidence for tropospheric wind shear excitation of high-phase-speed gravity waves reaching the mesosphere using the ray-tracing technique

Sources and propagation characteristics of high-frequency gravity waves observed in the mesosphere using airglow emissions from Gadanki (13.5° N, 79.2° E) and Hyderabad (17.5° N, 78.5° E) are investigated using reverse ray tracing. Wave amplitudes are also traced back, including both radiative and diffusive damping. The ray tracing is performed using background temperature and wind data obtained from the MSISE-90 and HWM-07 models, respectively. For the Gadanki region, the suitability of these models is tested. Further, a climatological model of the background atmosphere for the Gadanki region has been developed using nearly 30 years of observations available from a variety of ground-based (MST radar, radiosondes, MF radar) and rocket- and satellite-borne measurements. ERA-Interim products are utilized for constructing background parameters corresponding to the meteorological conditions of the observations. With the reverse ray-tracing method, the source locations for nine wave events could be identified to be in the upper troposphere, whereas for five other events the waves terminated in the mesosphere itself. Uncertainty in locating the terminal points of wave events in the horizontal direction is estimated to be within 50–100 km and 150–300 km for Gadanki and Hyderabad wave events, respectively. This uncertainty arises mainly due to non-consideration of the day-to-day variability in the tidal amplitudes. Prevailing conditions at the terminal points for each of the 14 events are provided. As no convection in and around the terminal points is noticed, convection is unlikely to be the source. Interestingly, large (~9 m s−1km−1) vertical shears in the horizontal wind are noticed near the ray terminal points (at 10–12 km altitude) and are thus identified to be the source for generating the observed high-phase-speed, high-frequency gravity waves.
Observations and modeling of air quality trends over 1990–2010 across the Northern Hemisphere: China, the United States and Europe

Trends in air quality across the Northern Hemisphere over a 21-year period (1990–2010) were simulated using the Community Multiscale Air Quality (CMAQ) multiscale chemical transport model driven by meteorology from Weather Research and Forecasting (WRF) simulations and internally consistent historical emission inventories obtained from EDGAR. Thorough comparison with several ground observation networks mostly over Europe and North America was conducted to evaluate the model performance as well as the ability of CMAQ to reproduce the observed trends in air quality over the past 2 decades in three regions: eastern China, the continental United States and Europe. The model successfully reproduced the observed decreasing trends in SO2, NO2, 8 h O3 maxima, SO42− and elemental carbon (EC) in the US and Europe. However, the model fails to reproduce the decreasing trends in NO3− in the US, potentially pointing to uncertainties of NH3 emissions. The model failed to capture the 6-year trends of SO2 and NO2 in CN-API (China – Air Pollution Index) from 2005 to 2010, but reproduced the observed pattern of O3 trends shown in three World Data Centre for Greenhouse Gases (WDCGG) sites over eastern Asia. Due to the coarse spatial resolution employed in these calculations, predicted SO2 and NO2 concentrations are underestimated relative to all urban networks, i.e., US-AQS (US – Air Quality System; normalized mean bias (NMB) = −38% and −48%), EU-AIRBASE (European Air quality data Base; NMB = −18 and −54%) and CN-API (NMB = −36 and −68%). Conversely, at the rural network EU-EMEP (European Monitoring and Evaluation Programme), SO2 is overestimated (NMB from 4 to 150%) while NO2 is simulated well (NMB within ±15%) in all seasons. Correlations between simulated and observed O3 wintertime daily 8 h maxima (DM8) are poor compared to other seasons for all networks. Better correlation between simulated and observed SO42− was found compared to that for SO2. Underestimation of summer SO42− in the US may be associated with the uncertainty in precipitation and associated wet scavenging representation in the model. The model exhibits worse performance for NO3− predictions, particularly in summer, due to high uncertainties in the gas/particle partitioning of NO3− as well as seasonal variations of NH3 emissions. There are high correlations (R > 0.5) between observed and simulated EC, although the model underestimates the EC concentration by 65% due to the coarse grid resolution as well as uncertainties in the PM speciation profile associated with EC emissions. The almost linear response seen in the trajectory of modeled O3 changes in eastern China over the past 2 decades suggests that control strategies that focus on combined control of NOx and volatile organic compound (VOC) emissions with a ratio of 0.46 may provide the most effective means for O3 reductions for the region devoid of nonlinear response potentially associated with NOx or VOC limitation resulting from alternate strategies. The response of O3 is more sensitive to changes in NOx emissions in the eastern US because the relative abundance of biogenic VOC emissions tends to reduce the effectiveness of VOC controls. Increasing NH3 levels offset the relative effectiveness of NOx controls in reducing the relative fraction of aerosol NO3− formed from declining NOx emissions in the eastern US, while the control effectiveness was assured by the simultaneous control of NH3 emission in Europe.
Temperature profiling of the atmospheric boundary layer with rotational Raman lidar during the HD(CP)2 Observational Prototype Experiment

The temperature measurements of the rotational Raman lidar of the University of Hohenheim (UHOH RRL) during the High Definition of Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observation Prototype Experiment (HOPE) in April and May 2013 are discussed. The lidar consists of a frequency-tripled Nd:YAG laser at 355 nm with 10 W average power at 50 Hz, a two-mirror scanner, a 40 cm receiving telescope, and a highly efficient polychromator with cascading interference filters for separating four signals: the elastic backscatter signal, two rotational Raman signals with different temperature dependence, and the vibrational Raman signal of water vapor. The main measurement variable of the UHOH RRL is temperature. For the HOPE campaign, the lidar receiver was optimized for high and low background levels, with a novel switch for the passband of the second rotational Raman channel. The instrument delivers atmospheric profiles of water vapor mixing ratio as well as particle backscatter coefficient and particle extinction coefficient as further products. As examples for the measurement performance, measurements of the temperature gradient and water vapor mixing ratio revealing the development of the atmospheric boundary layer within 25 h are presented. As expected from simulations, a reduction of the measurement uncertainty of 70% during nighttime was achieved with the new low-background setting. A two-mirror scanner allows for measurements in different directions. When pointing the scanner to low elevation, measurements close to the ground become possible which are otherwise impossible due to the non-total overlap of laser beam and receiving telescope field of view in the near range. An example of a low-level temperature measurement is presented which resolves the temperature gradient at the top of the stable nighttime boundary layer 100 m above the ground.
Uplifting of carbon monoxide from biomass burning and anthropogenic sources to the free troposphere in East Asia

East Asia has experienced rapid development with increasing carbon monoxide (CO) emission in the past decades. Therefore, uplifting CO from the boundary layer to the free troposphere in East Asia can have great implications on regional air quality around the world. It can also influence global climate due to the longer lifetime of CO at higher altitudes. In this study, three cases of high CO episodes in the East China Sea and the Sea of Japan from 2003 to 2005 are examined with spaceborne Measurements of Pollution in the Troposphere (MOPITT) data, in combination with aircraft measurements from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. High CO abundances of 300–550 ppbv are observed in MOZAIC data in the free troposphere during these episodes. These are among the highest CO abundances documented at these altitudes. On average, such episodes with CO over 400 ppbv (in the 2003 and 2004 cases) and between 200 and 300 ppbv (in the 2005 case) may occur 2–5 and 10–20% in time, respectively, in the respective altitudes over the region. Correspondingly, elevated CO is shown in MOPITT daytime data in the middle to upper troposphere in the 2003 case, in the lower to middle troposphere in the 2004 case, and in the upper troposphere in the 2005 case. Through analyses of the simulations from a chemical transport model GEOS-Chem and a trajectory dispersion model FLEXPART, we found different CO signatures in the elevated CO and distinct transport pathways and mechanisms for these cases. In the 2003 case, emissions from large forest fires near Lake Baikal dominated the elevated CO, which had been rapidly transported upward by a frontal system from the fire plumes. In the 2004 case, anthropogenic CO from the North China Plain experienced frontal lifting and mostly reached ~ 700 hPa near the East China Sea, while CO from biomass burning over Indochina experienced orographic lifting, lee-side-trough-induced convection, and frontal lifting through two separate transport pathways, leading to two distinct CO enhancements around 700 and 300 hPa. In the 2005 case, the observed CO of ~ 300 ppbv around 300 hPa originated from anthropogenic sources over the Sichuan Basin and the North China Plain and from forest fires over Indochina. The high CO was transported to such altitudes through strong frontal lifting, interacting with convection and orographic lifting. These cases show that topography affects vertical transport of CO in East Asia via different ways, including orographic uplifting over the Hengduan Mountains, assisting frontal lifting in the North China Plain, and facilitating convection in the Sichuan Basin. In particular, topography-induced lee-side troughs over Indochina led to strong convection that assisted CO uplifting to the upper troposphere. This study shows that the new daytime MOPITT near-infrared (NIR) and thermal-infrared (TIR) data (version 5 or above) have enhanced vertical sensitivity in the free troposphere and may help qualitative diagnosis of vertical transport processes in East Asia.