Interannual and Decadal Changes in Tropospheric Ozone in China and the Associated Chemistry–Climate Interactions: A Review

China has been experiencing widespread air pollution due to rapid industrialization and urbanization in recent decades.The two major concerns of ambient air quality in China are particulate matter(PM) and tropospheric ozone(O_3). With the implementation of air pollution prevention and control actions in the last five years, the PM pollution in China has been substantially reduced. In contrast, under the conditions of the urban air pollution complex, the elevated O_3 levels in city clusters of eastern China, especially in warm seasons, have drawn increasing attention. Emissions of air pollutants and their precursors not only contribute to regional air quality, but also alter climate. Climate change in turn can change chemical processes, long-range transport, and local meteorology that influence air pollution. Compared to PM, less is known about O_3 pollution and its climate effects over China. Here, we present a review of the main findings from the literature over the period 2011–18 with regard to the characteristics of O_3 concentrations in China and the mechanisms that drive its interannual to decadal variations, aiming to identify robust conclusions that may guide decision-making for emissions control and to highlight critical knowledge gaps. We also review regional and global modeling studies that have investigated the impacts of tropospheric O_3 on climate, as well as the projections of future tropospheric O_3 owing to climate and/or emission changes.     

What Causes the Springtime Tropospheric Ozone Maximum over Northeast Asia？

Scientists have long debated the relative importance of tropospheric photochemical production versus stratospheric influx as causes of the springtime tropospheric ozone maximum over northern mid-latitudes. This paper investigates whether or not stratospheric intrusion and photochemistry play a significant role in the springtime ozone maximum over Northeast Asia,where ozone measurements are sparse.We examine how tropospheric ozone seasonalities over Naha(26°N,128°E),Kagoshima(31°N,131°E),and Pohang(36°N,129°E),which are located on the same meridional line,are related to the timing and location of the jet stream.The ozone seasonality shows a gradual increase from January to the maximum ozone month,which corresponds to April at Naha,May at Kagoshima,and June at Pohang.In order to examine the occurrence of stratospheric intrusion,we analyze a correlation between jet stream activity and tropospheric ozone seasonality.From these analyses,we did not find any favorable evidence supporting the hypothesis that the springtime enhancement may result from stratospheric intrusion.According to trajectory analysis for vertical and horizontal origins of the airmass,a gradual increasing tendency in ozone amounts from January until the onset of monsoon was similar to the increasing ozone formation tendency from winter to spring over mainland China,which has been observed during the build-up of tropospheric ozone over Central Europe in the winter-spring transition period due to photochemistry.Overall,the analyses suggest that photochemistry is the most important contributor to observed ozone seasonality over Northeast Asia.     

Trends and Variability in Total Ozone from a Mid-Latitude Southern Hemisphere Site: The Melbourne Dobson Record 1978–2012

Abstract

The Australian Bureau of Meteorology maintains a number of long-running Dobson measurement programs, among the few in southern hemisphere mid-latitudes. Data from the Melbourne site (the Melbourne/Airport World Ozone and Ultraviolet Radiation Data Centre (WOUDC) station was originally located at Aspendale, then moved to the city centre, and finally to Melbourne Airport) from 1978 to 2012 have recently been reviewed and re-evaluated. These data are analyzed using multi-linear regression and also by application of an 11-year running mean. Satellite data from the Merged Ozone Dataset are also used for comparison with the Dobson results. We show that the Quasi-Biennial Oscillation (QBO) plays a major role in winter and spring once phase is taken into account by month. We also show that the three so-called “classical” proxies (QBO, solar cycle, and Equivalent Effective Stratospheric Chlorine (EESC)) alone are able to give a good fit to ozone for Melbourne and, more generally, the southern mid-latitudes for most months of the year, in contrast with the case in the northern hemisphere where dynamical variation plays a much more important role. Correspondingly, the smoothed Melbourne Dobson time series shows a high correlation to EESC.     

Comparison of the Bright Band Characteristics Measured by Micro Rain Radar （MRR） at a Mountain and a Coastal Site in South Korea

Data from a long term measurement of Micro Rain Radar (MRR) at a mountain site (Daegwallyeong,DG, one year period of 2005) and a coastal site (Haenam, HN, three years 2004–2006) in South Korea were analyzed to compare the MRR measured bright band characteristics of stratiform precipitation at the two sites. On average, the bright band was somewhat thicker and the sharpness (average gradient of reflectivity above and below the reflectivity peak) was slightly weaker at DG, compared to those values at HN. The ...     

Role of Ozone in the Sodium and Hydroxyl Nightglow

One-dimensional photochemical diffusion model which includes oxygen-hydrogen-sodium atmosphere has been used to examine the relation between sodium and hydroxyl nightglow and the role of ozone in it. It is found that both emissions can be obtained on the basis of photochemistry. The following reactionsNa + O3→jNaO + O2and H + O3→OH*+O2play key role in sodium and hydroxyl emission respectively. Further it is found that variations in both emissions are controlled by the variation in the concentration of ozone.     

The Surface Friction and the Flow over Mountain

The flow over mountain is quite complicated. There are a lot of papers on this problem and a lot of progresses have been made. However, in the most of these papers, just the dynamics contributions of mountain have been analysed; the effect of the friction is often neglected. Since the frictional effect is always associated with flow, especially when it flows over the mountain. The study shows that the friction is small in the magnitude but it is not a negligible effect because it changes the features of the flow. In the case of super-or sub-critical flow, there are two extremes: one maximum, one minimum of the fluid surface on the lee-side of the mountain, while in the inviscid fluid, there is just one extreme. The frictional effect should neither be too strong nor too weak to make the situation happened according to the investigation of this paper.     

Air–Sea Interaction Features in the Baltic Sea and at a Pacific Trade-Wind Site: An Inter-comparison Study

A systematic comparison of wind profiles and momentum exchange at a trade wind site outside Oahu, Hawaii and corresponding data from the Baltic Sea is presented. The trade wind data are to a very high degree swell dominated, whereas the Baltic Sea data include a more varied assortment of wave conditions, ranging from a pure growing sea to swell. In the trade wind region swell waves travel predominantly in the wind direction, while in the Baltic, significant cross-wind swells are also present. Showing the drag coefficient as a function of the 10-m wind speed demonstrates striking differences for unstable conditions with swell for the wind-speed range 2 m s^?1 < U ₁₀ < 7 m s^?1, where the trade-wind site drag values are significantly larger than the corresponding Baltic Sea values. In striking contrast to this disagreement, other features studied are surprisingly similar between the two sites. Thus, exactly as found previously in Baltic Sea studies during unstable conditions and swell, the wind profile in light winds (3 m s^?1) shows a wind maximum at around 7–8 m above the water, with close to constant wind speed above. Also, for slightly higher wind speeds (4 m s^?1 < U ₁₀ < 7 m s^?1), the similarity between wind profiles is striking, with a strong wind-speed increase below a height of about 7–8 m followed by a layer of virtually constant wind speed above. A consequence of these wind-profile features is that Monin–Obukhov similarity is no longer valid. At the trade-wind site this was observed to be the case even for wind speeds as high as 10 m s^?1. The turbulence kinetic energy budget was evaluated for four cases of 8–16 30- min periods at the trade-wind site, giving results that agree very well with corresponding figures from the Baltic Sea.     

The Measurement and Analysis of Antarctic Ozone at Zhongshan Station of 1993

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Tropospheric adjustment to increasing CO2: its timescale and the role of land–sea contrast

Physical processes responsible for tropospheric adjustment to increasing carbon dioxide concentration are investigated using abrupt CO₂ quadrupling experiments of a general circulation model (GCM) called the model for interdisciplinary research on climate version 5 with several configurations including a coupled atmosphere–ocean GCM, atmospheric GCM, and aqua-planet model. A similar experiment was performed in weather forecast mode to explore timescales of the tropospheric adjustment. We found that the shortwave component of the cloud radiative effect (SWcld) reaches its equilibrium within 2 days of the abrupt CO₂ increase. The change in SWcld is positive, associated with reduced clouds in the lower troposphere due to warming and drying by instantaneous radiative forcing. A reduction in surface turbulent heat fluxes and increase of the near-surface stability result in shoaling of the marine boundary layer, which shifts the cloud layer downward. These changes are common to all experiments regardless of model configuration, indicating that the cloud adjustment is primarily independent of air–sea coupling and land–sea thermal contrast. The role of land in cloud adjustment is further examined by a series of idealized aqua-planet experiments, with a rectangular continent of varying width. Land surface warming from quadrupled CO₂ induces anomalous upward motion, which increases high cloud and associated negative SWcld over land. The geographic distribution of continents regulates the spatial pattern of the cloud adjustment. A larger continent produces more negative SWcld, which partly compensates for a positive SWcld over the ocean. The land-induced negative adjustment is a factor but not necessary requirement for the tropospheric adjustment.     

HCl Quasi-Biennial Oscillation in the Stratosphere and a Comparison with Ozone QBO

1. Introduction The quasi-biennial oscillation (QBO) of the mean zonal wind in the equatorial stratosphere was discov- ered by Reed et al. (1961) and Veryard and Ebdon (1961). Later, Funk and Garnham (1962) and Ra- manathan (1963) were the first to descri…     

The Ozone, Aerosol Depletion and Condensation Nuclei Events in the Stratosphere

Recently, the depletion in ozone and aerosol extinctions inside Antarctic Spring westerly vortex and condensation nuclei enhancement events in the mid latitudes stratosphere were related to downward transport of aerosols by subsidence and sedimentation. However, the problems associated with such hypothesis would keep a constraint on photochemical theories on ozone hole and stratospheric condensation nuclei (CN) events. Alternately, the gross features of aerosol hole are better explicable assuming a reversed residual circulation. This opens a path for combined operation on ozone by both photochemistry and dynamics in the same space domain.Independently, we relate the CN events to the growth and transport of negative ion complexes above the Peak of Junge Layer (PJL) without invoking photochemistry in order to be consistant with the observed interhemispheric differences in the planetary wave activity and CN concentration.     

Products and Mechanism of the Gas Phase Reaction of Ozone with β-Pinene

Gas phase ozonolysis of -pinene was performedin a 570 l static reactor at 730 Torr and 296 K insynthetic air and the products were analysed by acombination of gas phase FTIR spectroscopy, HPLC andIC analyses of gas phase and aerosol samples,respectively. The reaction mechanism was investigatedby adding HCHO, HCOOH and H₂O as Criegeeintermediate scavenger and cyclohexane as OH radicalscavenger. Main identified products (yields inparentheses) in the presence of cyclohexane as OHradical scavenger were HCHO (0.65 ± 0.04),nopinone (0.16 ± 0.04), 3-hydroxy-nopinone (0.15± 0.05), CO₂ (0.20 ± 0.04), CO (0.030± 0.002), HCOOH (0.020 ± 0.002), the secondaryozonide of -pinene (0.16 ± 0.05), andcis-pinic acid (0.02 ± 0.01). The decompositionof the primary ozonide was found to yieldpredominantly the excited C₉-Criegee intermediateand HCHO (0.84 ± 0.04) and to a minor extent theexcited CH₂OO intermediate and nopinone (0.16± 0.04). Roughly 40% of the excitedC₉-Criegee intermediate becomes stabilised andcould be shown to react with HCHO, HCOOH and H₂O. The atmospherically important reaction of thestabilised C₉-Criegee intermediate with H₂Owas found to result in a nopinone increase of (0.35± 0.05) and in the formation of H₂O₂(0.24 ± 0.03). Based on the observed products,the unimolecular decomposition/isomerisationchannels of the C₉-Criegee intermediate arediscussed in terms of the hydroperoxide and esterchannels. Subsequent reactions of the nopinonylradical, formed in the hydroperoxide channel, lead tomajor products like 3-hydroxy-nopinone but also tominor products like cis-pinic acid. A mechanismfor the formation of this dicarboxylic acid isproposed and its possible role in aerosol formationprocesses discussed.     

Comparison between measured and modelled cloudless‐sky solar irradiances at the surface and at the top of the atmosphere

Abstract

Cloudless‐sky solar fluxes calculated by the radiative transfer algorithm used in the Canadian Climate Centre's general circulation climate model are compared with measurements of upwelling radiation at the top of the atmosphere (TOA) and downwelling radiation at the surface. The 12‐layer model partitions the solar spectrum into two broad wavebands (0.25–0.68 and 0.68–4.00 μm). The comparison utilized TOA fluxes estimated from Nimbus‐ 7 measurements and measured downwelling fluxes at the surface for Kalgoorlie, West Australia, and downwelling fluxes at the surface for Woodbridge, Ontario. Model estimates and measurements agreed to within experimental error for most solar zenith angles. Estimates improved, especially at Woodbridge, when aerosol effects were included. The mean bias error was less than 4% for surface irradiance and less than 6% for upwelling TOA irradiance, which produces a TOA albedo error of about 0.01.     

Gas and Particle Products Distribution from the Reaction of β-Caryophyllene with Ozone

Gas and particulate reaction products from the ozonolysis of -caryophyllene (I) in the presence of atmospheric air were investigated using a combination of gas chromatography-mass spectrometry (GC-MS) and high performance liquid chromatography (HPLC). A Scanning Mobility Particle Sizer system (3936, TSI) and a Condensation Particle Counter (3025A, TSI) were used to study secondary organic aerosol formation. The nighttime oxidation was carried out in a large outdoor smog chamber (190 m³). A wide range of ring retaining and ring opening products in the gas and particle phase are reported over the course of the reaction. On average, measured gas and particle phase products accounted for 64% of the reacted -caryophyllene (I) carbon. Measurements show that a number of reaction products with low vapor pressure (e.g., -caryophyllone aldehyde (IV), -norcaryophyllone aldehyde (V), -caryophyllonic acid (VIII), -14-hydroxycaryophyllonic acid (XIV)) were found in the sample taken during the first 20 min of the reaction and may play an important role in the early formation of secondary organic aerosol. A detailed mechanism is proposed to account for most products observed in this investigation.     

Climate Responses to Direct Radiative Forcing of Anthropogenic Aerosols,Tropospheric Ozone,and Long-Lived Greenhouse Gases in Eastern China over 1951–2000

A unified chemistry-aerosol-climate model is applied in this work to compare climate responses to chang- ing concentrations of long-lived greenhouse gases(GHGs,CO2,CH4,N2O),tropospheric O3,and aerosols during the years 1951–2000.Concentrations of sulfate,nitrate,primary organic carbon(POA),secondary organic carbon(SOA),black carbon(BC)aerosols,and tropospheric O3 for the years 1950 and 2000 are obtained a priori by coupled chemistry-aerosol-GCM simulations,and then monthly concentrations are in- terpolated ...     

The Energy Budget of Snow and Ice at Breidamerkurjökull, Vatnajökull, Iceland

Measurements of the energy and mass budgets have beenmade at the equilibrium line ofBreidamerkurjökull, a southern outlet glacier ofVatnajökull, Iceland. The glacier's surface wasmelting for most of the measurement period, whichallowed for a reliable closure of the energy budget.Sensitivity studies focussed mainly on potentialeffects of measurement errors, site-specificmicrometeorological conditions, surface developmentand different parameterization of the turbulentfluxes. Although the high stability and a roughnessdisturbance imposed certain restrictions, thesestudies confirmed the applicability of theMonin–Obukhov framework for the evaluation of turbulentfluxes.The characteristics of the energy and mass budgets arediscussed with respect to various time scales andsignificant weather conditions. Due to the maskingglacial boundary layer, warm fronts appearedcomparatively weak compared to the more vigorous coldfronts. The latter were often associated with leeeffects and give striking signals in the turbulent fluxes.Transition from snow to ice induced a distinct changein the regime because of related albedo and roughnesseffects.A compilation of the major energy budget components atglaciers all over the world confirms the maritimeregime at Vatnajökull.     

Climate change and the Water Framework Directive: cost effectiveness and policy design for water management in the Swedish Mälar region

This paper calculates the impacts of climatic change on cost effective nutrient management under the Water Framework Directive (WFD) for the eutrophic Mälar lake and Stockholm archipelago in south-eastern Sweden. This is carried out for two types of targets: actual nutrient reduction targets and water quality targets as suggested by WFD. Stochastic programming is applied where climatic changes are modelled as impacts on the mean and variability in nutrient loads and water quality. The results indicate significant impacts on abatement costs and associated nutrient policy design for both targets. Climatic change may under favourable conditions ‘solve’ the water quality problem by achieving the predetermined target without any need for policy instruments, but can also generate large increases in cleaning costs and required charge/subsidy schemes for the same target. The results also point to the importance of target setting, where water quality targets are more robust than nutrient reduction targets with respect to achievement under different climate change impacts.     

Retrieval of Tropospheric CO Profiles Using Correlation Radiometer.Ⅱ: Effects of Other Gases and the Retrieval in Cloudy Atmosphere

l.Intr0ducti0nAschemeforretrievingCOprofilesinthetroPOspherehasbeendiscussedinthepreviousPartI(WuandGille,partI)foragascorrelationradiometerMeasurementsofPollutionintheTroPOsphere(M0PITT)workingatthe4.6pmwaveband.Thebasicequationshavebeendiscussed.TheuseofthewidebandsignalforprovidingthesurfacetemPeratureandanaddi-tionalchannelforthecolumnarC0amounttoimprovetheretrievalinthenearsurfacelayerhasbeentested.Itisfoundthaterrorsinthetemperatureprofilemayincreaseerrorsinthere-trievedprofiles…     

Numerical Simulation Study on the Impacts of Tropospheric and CO_2 Concentration Changes on Winter Wheat. Part I: Model Description

Ozone is well documented as the air pollutant most damaging to agricultural crops and other plants. It is reported that tropospheric O3 concentration increases rapidly in recent 20 years. Evaluating and predicting impacts of ozone concentration changes on crops are drawing great attention in the scientific community. In China, main study method about this filed is controlled experiments, for example, Open Top Chambers. But numerical simulation study about impacts of ozone on crops with crop model was developed slowly, what is more, the study about combined impacts of ozone and carbon dioxide has not been reported. The improved agroecosystem model is presented to evaluate simultaneously impacts of tropospheric O3 and CO2 concentration changes on crops in the paper by integrating algorithms about impacts of ozone on photosynthesis with an existing agroecosystem biogeochemical model (named as DNDC). The main physiological processes of crop growth (phenology, leaf area index, photosynthesis, respiration, assimilated allocation and so on) in the former DNDC are kept. The algorithms about impacts of ozone on photosynthesis and winter wheat leaf are added in the modified DNDC model in order to reveal impacts of ozone and carbon dioxide on growth, development, and yield formation of winter wheat by coupling the simulation about impacts of carbon dioxide on photosynthesis of winter wheat which exists in the former DNDC. In the paper, firstly assimilate allocation algorithms and some genetic parameters (such as daily thermal time of every development stage) were modified in order that DNDC can be applicable in North China. Secondly impacts of ozone on crops were simulated with two different methods- one was impacts of ozone on light use efficiency, and the other was direct effects of ozone on leaves photosynthesis. The latter simulated results are closer to experiment measurements through comparing their simulating results. At last the method of direct impacts of ozone on leaf growth is adopted and the coefficients about impacts of ozone on leaf growth and death are ascertained. Effects of climate changes, increasing ozone, and carbon dioxide concentration on agroecosystem are tried to be simulated numerically in the study which is considered to be advanced and credible.