First-Order Chemistry in the Surface-Flux Layer

We have discussed the behavior of a non-conserved scalar in the stationary, horizontally homogeneous, neutral surface-flux layer and, on the basis of conventional second-order closure, derived analytic expressions for flux and for mean concentration of a gas, subjected to a first-order removal process. The analytic flux solution showed a clear deviation from the constant flux, characterizing a conserved scalar in the surface-flux layer. It decreases with height and is reduced by an order of magnitude of the surface flux at a height equal to about the typical mean distance a molecule can travel before destruction. The predicted mean concentration profile, however, shows only a small deviation from the logarithmic behavior of a conserved scalar. The solution is consistent with assuming a flux-gradient relationship with a turbulent diffusivity corrected by the Damköhler ratio, the ratio of a characteristic turbulent time scale and the scalar mean lifetime. We show that if we use only first-order closure and neglect the effect of the Damköhler ratio on the turbulent diffusivity we obtain another analytic solution for the profiles of the flux and the mean concentration which, from an experimental point of view, is indistinguishable from the first analytic solution. We have discussed two cases where the model should apply, namely NO which, by night, is irreversibly destroyed by interaction with mainly O₃ and the radioactive ²²⁰Rn. Only in the last case was it possible to find data to shed light on the validity of our predictions. The agreement seemed such that a falsification of our model was impossible. It is shown how the model can be used to predict the surface flux of ²²⁰Rn from measured concentration profiles.     

Kinetics of the Gas-Phase Reactions of OH Radicals, NO3 Radicals and O3 with Three C7-Carbonyls Formed From The Atmospheric Reactions of Myrcene, Ocimene and Terpinolene

Rate constants for the gas-phase reactions of OH radicals, NO₃ radicals and O₃ with the C₇-carbonyl compounds 4-methylenehex-5-enal [CH₂=CHC(=CH₂)CH₂CH₂CHO], (3Z)- and (3E)-4-methylhexa-3,5-dienal [CH₂=CHC(CH₃)=CHCH₂CHO] and 4-methylcyclohex-3-en-1-one, which are products of the atmospheric degradations of myrcene, Z- and E-ocimene and terpinolene, respectively, have been measured at 296 ± 2 K and atmospheric pressure of air using relative rate methods. The rate constants obtained (in cm³ molecule^–1 s^–1 units) were: for 4-methylenehex-5-enal, (1.55 ± 0.15) × 10^–10, (4.75 ± 0.35) × 10^–13 and (1.46 ± 0.12) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively; for (3Z)-4-methylhexa-3,5-dienal: (1.61 ± 0.35) × 10^–10, (2.17 ± 0.30) × 10^–12, and (4.13 ± 0.81) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively; for (3E)-4-methylhexa-3,5-dienal: (2.52 ± 0.65) × 10^–10, (1.75 ± 0.27) × 10^–12, and (5.36 ± 0.28) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively; and for 4-methylcyclohex-3-en-1-one: (1.10 ± 0.19) × 10^–10, (1.81 ± 0.35) × 10^–12, and (6.98 ± 0.40) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively. These carbonyl compounds are all reactive in the troposphere, with daytime reaction with the OH radical and nighttime reaction with the NO₃ radical being predicted to dominate as loss processes and with estimated lifetimes of about an hour or less.     

An Algorithm for the Determination of All Significant Pathways in Chemical Reaction Systems

When the output of a complex chemical model is analysed, a typical topic isthe determination of pathways, i.e., reaction sequences, that produce ordestroy a chemical species of interest.A representative example is the investigation of catalytic ozone destruction cycles in the stratosphere.An algorithm for the automatic determination of pathways in any given reactionsystem is presented. Under the assumption that reaction rates are known, it finds all significant pathways, i.e., all pathways with a rate above a prescribed threshold.The algorithm forms pathways step by step, starting from single reactions.The chemical species in the system are consecutively considered as `branching points'.For every branching-point species, each pathway producing it is connected witheach pathway consuming it.Rates proportional to `branching probabilities' are calculated.Pathways with a rate that is smaller than a prescribed threshold arediscarded.If a newly formed pathway contains sub-pathways, e.g., null cycles, it is split into these simpler pathways.In order to demonstrate the performance of the algorithm, it has been applied to the determination of catalytic ozone destruction cycles and methaneoxidation pathways in the stratosphere.     

A Review of Research on Human Activity Induced Climate ChangeⅠ. Greenhouse Gases and Aerosols

Extensive research on the sources and sinks of greenhouse gases, carbon cycle modeling, and the characterization of atmospheric aerosols has been carried out in China during the last 10 years or so. This paper presents the major achievements in the fields of emissions of greenhouse gases from agricultural lands, carbon cycle modeling, the characterization of Asian mineral dust, source identification of the precursors of the tropospheric ozone, and observations of the concentrations of atmospheric organic compounds. Special, more detailed Information on the emissions of methane from rice fields and the physical and chemical characteristics of mineral aerosols are presented.     

An asynchronous Geoprocessing Workflow and its application to an Antarctic ozone monitoring and mapping service

The integration of Sensor Web Enablement services with other Open Geospatial Consortium (OGC) Web Services as Geospatial Processing Workflows (GPW) is essential for future Sensor Web application scenarios. With the help of GPW technology, distributed and heterogeneous OGC Web Services can be organized and integrated as compound Web Service applications that can direct complicated earth observation tasks. Under the Sensor Web environment, asynchronous communications between Sensor Web Services are common. We have proposed an asynchronous GPW architecture for the integration of Sensor Web Services into a Web Service Business Process Execution Language workflow technology. We designed a Sensor Information Accessing and Processing workflow, an asynchronous GPW instance, to take an experiment of observing and mapping ozone over Antarctica. Based on our results, our proposed asynchronous workflow method shows the advantages of taking environmental monitoring and mapping tasks.     

A modeling study of effective radiative forcing and climate response due to tropospheric ozone

This study simulates the effective radiative forcing(ERF) of tropospheric ozone from 1850 to 2013 and its effects on global climate using an aerosol–climate coupled model, BCC AGCM2.0.1 CUACE/Aero, in combination with OMI(Ozone Monitoring Instrument) satellite ozone data. According to the OMI observations, the global annual mean tropospheric column ozone(TCO) was 33.9 DU in 2013, and the largest TCO was distributed in the belts between 30°N and 45°N and at approximately 30°S; the annual mean TCO was higher in the Northern Hemisphere than that in the Southern Hemisphere;and in boreal summer and autumn, the global mean TCO was higher than in winter and spring. The simulated ERF due to the change in tropospheric ozone concentration from 1850 to 2013 was 0.46 W m~(-2), thereby causing an increase in the global annual mean surface temperature by 0.36℃, and precipitation by 0.02 mm d~(-1)(the increase of surface temperature had a significance level above 95%). The surface temperature was increased more obviously over the high latitudes in both hemispheres, with the maximum exceeding 1.4?C in Siberia. There were opposite changes in precipitation near the equator,with an increase of 0.5 mm d~(-1)near the Hawaiian Islands and a decrease of about-0.6 mm d~(-1)near the middle of the Indian Ocean.     

卫星臭氧资料的发展与应用

随着卫星探测技术的进步、天气学和气候学理论的不断完善,以及高性能计算机广泛应用,卫星臭氧资料的种类得到极大丰富并被应用到多个研究领域中,取得了一系列重要成果。文中介绍了主要星载臭氧探测仪的发展概况,回顾了卫星臭氧资料在气象领域的应用研究成果,主要包括卫星臭氧资料在气旋或低压过程中、全球或区域臭氧的气候分布及变化特征、高原臭氧分布及变化特点、数值应用等方面的应用研究,并展望了卫星臭氧资料研究的未来发展趋势。      

The global search and commercialization of alternatives and substitutes for ozone-depleting substances

The Montreal Protocol has halted 99% of global production of chemical substances that deplete stratospheric ozone, which protects life on earth from the harmful effects of ultraviolet (UVB) radiation. UVB causes skin cancer and cataracts, suppresses the human immune system, destroys plastics, and damages agricultural crops and natural ecosystems. Because ozone-depleting substances (ODSs) are powerful greenhouse gases, the Montreal Protocol also protects climate. From the authors’ perspectives in multiple roles as environmental entrepreneurs, practitioners, and authorities, this paper explains how individuals, companies, and military organizations researched, developed, commercialized and implemented alternatives to ODSs that are also safer for climate. With the benefit of hindsight, the authors reflect on what was neglected or done badly under the Montreal Protocol and present lessons learned on how Montreal Protocol institutions can be renewed and revitalized to phase down hydrofluorocarbons (HFCs).     

Twenty-five years of spectral UV-B measurements over Canada,Europe and Japan: Trends and effects from changes in ozone,aerosols, clouds,and surface reflectivity

Spectral UV records of solar irradiance at stations over Europe, Canada, and Japan were used to study long-term trends at 307.5 nm for a 25-year period, from 1992 to 2016. Ground-based measurements of total ozone, as well as satellite measurements of the Aerosol Index, the Total Cloud Cover and the surface reflectivity were also used in order to attribute the estimated changes of the UV to the corresponding changes of these factors. The present study shows that over the Northern Hemisphere, the long-term changes in UV-B radiation reaching the Earth's surface vary significantly over different locations, and that the main drivers of these variations are changes in aerosols and total ozone. At high latitudes, part of the observed changes may also be attributed to changes in the surface reflectivity. Over Japan, the UV-B irradiance at 307.5 nm has increased significantly by ∼3%/decade during the past 25 years, possibly due to the corresponding significant decrease of its absorption by aerosols. It was found that the greatest part of this increase took place before the mid-2000s. The only European station, over which UV radiation increases significantly, is that of Thessaloniki, Greece. Analysis of the clear-sky irradiance for the particular station shows increasing irradiance at 307.5 nm by ∼3.5%/decade during the entire period of study, with an increasing rate of change during the last decade, possibly again due to the decreasing absorption by aerosols.     

The cause of the spring strengthening of the Antarctic polar vortex

The stratospheric polar vortex strengthening from late winter to spring plays a crucial role in polar ozone depletion. The Arctic polar vortex reaches its peak intensity in mid-winter, whereas the Antarctic vortex usually strengthens in early spring. As a result, the strong ozone depletion is observed every year over the Antarctic, while over the Arctic short-term ozone loss occasionally occurs in late winter or early spring. However, the cause of such a difference in the life cycles of the Arctic and Antarctic polar vortices is still not completely clear. Based on the ERA-Interim reanalysis data, we show a high agreement between the seasonal variations of temperature in the subtropical lower stratosphere and zonal wind in the subpolar and polar lower stratosphere in the Southern Hemisphere. Thus, the spring strengthening of the Antarctic polar vortex can occur due to the seasonal temperature increase in the subtropical lower stratosphere in this period.