Impact of cloud dynamics on tropospheric chemistry: Advances in modeling the interactions between microphysical and chemical processes

A chemical module describing the tropospheric photochemistry of ozone precursors in both gaseous and aqueous phases for a remote continental atmosphere has been developed within the framework of a two-dimensional cloud model. Dynamical, microphysical and chemical processes are fully interacting in order to study the influence of clouds on ozone chemistry and to quantify the relative importance of the different processes on the budget and evolution of 12 chemical species. Whereas the concentrations of highly soluble species are strongly affected by evaporation and sedimentation, less soluble species are affected primarily by accretion. The model reproduces previously observed chemical phenomena such as the enrichment of formic acid at the top of the cloud.     

回流暴雪过程的诊断分析和数值试验

利用常规观测资料及NCEP/NCAR 1°×1°逐6 h再分析资料,分析了2018年初豫南特大暴雪过程的特征与成因。结果表明：此次特大暴雪过程发生在500 hPa乌拉尔山以东地区阻塞高压稳定维持和中、高纬地区多支短波槽东移并同位相叠加的环流背景下,具有持续时间长、过程降雪量大、降雪强度大、积雪深等特征;强降雪阶段,对流层低层豫南地区同时存在两个水汽来源,一是700 hPa西南急流对孟加拉湾水汽的输送,二是850 hPa东南气流对东海南部水汽的输送;低层较强的水汽输送及辐合、贯穿整个对流层的湿层、维持较高的比湿和整层可降水量对暴雪的形成与持续有一定的指示意义;低空冷垫有利于逆温层之上西南暖湿气流在其上爬升,低空垂直风切变的变化对降雪强度变化有较好的指示意义;高空急流先于低空西南急流而建立,高空急流轴南压使得低空急流发展北上,高低空急流耦合激发次级环流圈上升支,为暴雪发生发展提供了强烈的上升运动;对流层低层700 hPa与850 hPa持续强烈锋生,有利于暴雪加强和持续。

     

Acidic deposition to forests: The 1985 chemistry of high elevation fog (CHEF) project

Abstract

The literature supporting significant water deposition directly from cloud and fog to the earth's surface is reviewed and previous aircraft and surface measurements of the acidity of this water are summarized. An overview of recent work on forest decline is given and an American (Mountain Cloud Chemistry Project) and Canadian (Chemistry of High Elevation Fog) program to look at the chemical deposition by clouds to high elevation forests, is‐described.

Preliminary measurements in late 1985 on two mountains in Quebec indicate that fog (cloud on the mountain) water pH values (≈3.8) near the summits (850–970 m) are much lower than precipitation pH values (≈ 4.3) at the same location; the summits are estimated to be in cloud 44% of the year with lower percentages at lower elevations; an estimate of total annual fog water deposition (77 cm) near the summit is similar to the average annual precipitation in Quebec; the estimated fog water hydrogen ion deposition (135 meq m^?2) is about three times that from the precipitation; the precipitation pH values may be lower (4.1 ver sus 4.3) at lower elevations with precipitation amounts perhaps 50% higher at higher elevations.     

Nocturnal urban heat island in Lisbon (Portugal): main features and modelling attempts

Summary In recent years, several studies have examined the Lisbon urban climate. A central conclusion is the existence of a nocturnal urban heat island (mean ΔT_u−r = 2.5 °C). The aim of this paper is to summarise several attempts carried out in the last decade to interpolate nocturnal air temperatures across Lisbon, in order to be able to draw thermal maps as accurately as possible. This study refers only to clear nights. Stepwise multiple regression and a Geographic Information System were used to model the relation between air temperature and parameters related to land-use and topography. The different regression models (coefficients of determination between 0.68 and 0.92) show that canopy layer air temperature depends on sky-view factor, building height and percentage of built-up area, but also to a great extend on mesoclimatic geographic factors such as altitude, topography and distance from the Tagus River. Examples of four frequently encountered nocturnal air temperature patterns are presented, each corresponds to a different weather type. This method employed could prove useful in drawing climatic maps that may be of use in master plans of urban municipalities.     

The atmospheric chemistry of dimethylsulfoxide (DMSO) kinetics and mechanism of the OH+DMSO reaction

We have employed a pulsed laser photolysis-pulsed laser induced fluorescence technique to study the kinetics and mechanism of the reaction of OH with dimethylsulfoxide and its deuterated analogue. A rate coefficient of (1.0±0.3)×10^-10 cm³ molecule^-1 s^-1 was obtained ar room temperature. The rate coefficient was independent of pressure over the range 25–700 Torr, showed no dependence on the nature of the buffer gas and showed no kinetic isotope effect. A limited study of the temperature dependence indicated that the reaction displays a negative activation energy. The gas phase ultraviolet absorption spectrum was obtained at room temperature and showed a strong absorption feature in the far ultraviolet. The absolute absorption cross-section at 205 nm, the absorption peak, is (1.0±0.3)×10^-17 cm², where the large uncertainty results from experimental difficulties associated with the low vapor pressure and stickiness of DMSO.     

The respective roles of surface temperature driven feedbacks and tropospheric adjustment to CO2 in CMIP5 transient climate simulations

An overview of radiative climate feedbacks and ocean heat uptake efficiency diagnosed from idealized transient climate change experiments of 14 CMIP5 models is presented. Feedbacks explain about two times more variance in transient climate response across the models than ocean heat uptake efficiency. Cloud feedbacks can clearly be identified as the main source of inter-model spread. Models with strong longwave feedbacks in the tropics feature substantial increases in cloud ice around the tropopause suggestive of changes in cloud-top heights. The lifting of the tropical tropopause goes together with a general weakening of the tropical circulation. Distinctive inter-model differences in cloud shortwave feedbacks occur in the subtropics including the equatorward flanks of the storm-tracks. Related cloud fraction changes are not confined to low clouds but comprise middle level clouds as well. A reduction in relative humidity through the lower and mid troposphere can be identified as being the main associated large-scale feature. Experiments with prescribed sea surface temperatures are analyzed in order to investigate whether the diagnosed feedbacks from the transient climate simulations contain a tropospheric adjustment component that is not conveyed through the surface temperature response. The strengths of the climate feedbacks computed from atmosphere-only experiments with prescribed increases in sea surface temperatures, but fixed CO₂ concentrations, are close to the ones derived from the transient experiment. Only the cloud shortwave feedback exhibits discernible differences which, however, can not unequivocally be attributed to tropospheric adjustment to CO₂. Although for some models a tropospheric adjustment component is present in the global mean shortwave cloud feedback, an analysis of spatial patterns does not lend support to the view that cloud feedbacks are dominated by their tropospheric adjustment part. Nevertheless, there is positive correlation between the strength of tropospheric adjustment processes and cloud feedbacks across different climate models.     

The 2nd Aerosol Characterization Experiment (ACE‐2): meteorological and chemical context

A review is given of the climatological and actual meteorological conditions in the sub‐tropical northeast Atlantic, during June–July 1997, when the 2nd Aerosol Characterization Experiment (ACE‐2) took place. Surface pressure maps, trajectory calculations and in‐situ measurements show how the outflow of European pollution into the marine boundary layer of this area is determined by the location of the Azores high pressure cell. Observations during ACE‐2 and 3 preceding summers show that pollution outbreaks both from the Iberian peninsula and from northern or central Europe can occur during such situations. During ACE‐2, an unusually low number of strong North African dust outbreaks were recorded at the free tropospheric station of Izaña (Tenerife, 2360 m asl), although dust was recorded aloft the station.     

Effect of clouds on the photodissociation of NO2: Observations and modelling

The role of clouds in photodissociation is examined by both modelling and observations. It is emphasized that the photodissociation rate is proportional to the actinic flux rather than to the irradiance. The actinic flux concerns the energy that is incident on a molecule, irrespective of the direction of incidence. The irradiance concerns the energy that is incident on a plane.As far as the modelling aspect is concerned, a multi-layer delta-Eddington model is used to calculate irradiances, actinic fluxes, and photodissociation rates of nitrogen dioxide J(NO₂) as a function of height in inhomogeneous atmospheres. For the considered wavelength interval [290–420 nm], Rayleigh scattering, ozone absorption, and Mie scattering and absorption by cloud drops and aerosols should be taken into account.Further, a three-layer model is used to calculate the actinic flux above and below a cloud, relative to the incident flux, in terms of cloud albedo, zenith angle, and the albedo of the underlying and overlying atmosphere. Cloud albedo is mainly determined by cloud optical thickness. An expression for the incloud actinic flux is given as a function of in-cloud optical thickness. The three-layer model seems to be a useful model for the estimation of photodissociation rates in dispersion models.It is stressed that both models in their present form cannot handle partial cloudiness.It is shown that if no clouds are present, the actinic flux depends primarily on solar zenith angle. Further, the incident flux at the top of the atmosphere diminishes downward into the atmosphere due to the increasing effect of scattering. Therefore, the actinic flux usually increases with height, although above clouds the actinic flux sometimes decreases with height due to a large contribution of the upward scattered light.For cloudy atmospheres, another important parameter with respect to the actinic flux is added: cloud optical thickness. Cloud optical thickness determines cloud albedo. It can be shown that incloud characteristics and cloud height are less important while describing the effect of a cloud on the actinic flux (outside the cloud). The in-cloud values of the actinic flux can exceed the values outside the cloud.Finally, using the photostationary state relationship, a comparison is performed between model results and ground-based measurements as well as in-cloud air craft measurements.     

力觉临场感遥操作机器人(1):技术发展与现状

人机交互式机器人作为最具实用价值的特种机器人已成为当前机器人学研究的前沿和热点.临场感(Telepresence)技术是人机交互的核心.首先,回顾了力觉临场感遥操作机器人技术的产生、发展和现状,介绍了力觉临场感遥操作机器人在核领域、空间探测领域与远程医疗领域的应用情况;其次,对力觉临场感遥操作机器人的4大关键技术:传感技术、力反馈与触觉再现技术、大时延控制技术和虚拟预测环境建模技术等进行了综述;还介绍了东南大学仪器科学与工程学院机器人传感与控制研究所近20年来开展临场感遥操作机器人技术研究,以及在核探测、康复医疗领域应用的情况.通过回顾与分析,指出了力觉临场感遥操作机器人技术今后需要研究的几个重点问题.     

Photooxidation of dimethyl sulfide and dimethyl disulfide. I: Mechanism development

Detailed theoretical (Part I, this article) and experimental (Part II) investigations are presented for the mechanism of the atmospheric photooxidation of dimethyl sulfide (CH₃SCH₃) and dimethyl disulfide (CH₃SSCH₃). In this paper, comprehensive mechanisms for the atmospheric chemistry of CH₃SCH₃ and CH₃SSCH₃ are developed based on fundamental considerations of all available kinetic and mechanistic information.     

Pacific Atmospheric Sulfur Experiment (PASE): dynamics and chemistry of the south Pacific tropical trade wind regime

The Pacific Atmospheric Sulfur Experiment (PASE) was a comprehensive airborne study of the chemistry and dynamics of the tropical trade wind regime (TWR) east of the island of Kiritibati (Christmas Island, 157º, 20?? W, 2º 52?? N). Christmas Island is located due south of Hawaii. Geographically it is in the northern hemisphere yet it is 6?C12º south of the intertropical convergence zone (ITCZ) which places it in the southern hemisphere meteorologically. Christmas Island trade winds in August and September are from east south east at 3?C15 ms^?1. Clouds, if present, are fair weather cumulus located in the middle layer of the TWR which is frequently labeled the buffer layer (BuL). PASE provided clear support for the idea that small particles (80 nm) were subsiding into the tropical trade wind regime (TWR) where sulfur chemistry transformed them to larger particles. Sulfur chemistry promoted the growth of some of these particles until they were large enough to activate to cloud drops. This process, promoted by sulfur chemistry, can produce a cooling effect due to the increase in cloud droplet density and changes in cloud droplet size. These increases in particle size observed in PASE promote additional cooling due to direct scattering from the aerosol. These potential impacts on the radiation balance in the TWR are enhanced by the high solar irradiance and ocean albedo of the TWR. Finally because of the large area involved there is a large factional impact on earth??s radiation budget. The TWR region near Christmas Island appears to be similar to the TWR that persists in August and September, from southwest of the Galapagos to at least Christmas Island. Transport in the TWR between the Galapagos and Christmas involves very little precipitation which could have removed the aerosol thus explaining at least in part the high concentrations of CCN (??300 at 0.5% supersaturation) observed in PASE. As expected the chemistry of sulfur in the trade winds was found to be initiated by the emission of DMS into the convective boundary layer (BL, the lowest of three layers). However, the efficiency with which this DMS is converted to SO₂ has been brought into further question by this study. This unusual result has come about as result of our using two totally different approaches for addressing this long standing question. In the first approach, based on accepted kinetic rate constants and detailed steps for the oxidation of DMS reflecting detailed laboratory studies, a DMS to SO₂ conversion efficiency of 60?C73% was determined. This range of values lies well within the uncertainties of previous studies. However, using a completely different approach, involving a budget analysis, a conversion value of 100% was estimated. The latter value, to be consistent with all other sulfur studies, requires the existence of a completely independent sulfur source which would emit into the atmosphere at a source strength approximately half that measured for DMS under tropical Pacific conditions. At this time, however, there is no credible scientific observation that identifies what this source might be. Thus, the current study has opened for future scientific investigation the major question: is there yet another major tropical marine source of sulfur? Of equal importance, then, is the related question, is our global sulfur budget significantly in error due to the existence of an unknown marine source of sulfur? Pivotal to both questions may be gaining greater insight about the intermediate DMS oxidation species, DMSO, for which rather unusual measurements have been reported in previous marine sulfur studies. The 3 pptv bromine deficit observed in PASE must be lost over the lifetime of the aerosol which is a few days. This observation suggests that the primary BrO production rate is very small. However, considering the uncertainties in these observations and the possible importance of secondary production of bromine radicals through aerosol surface reactions, to completely rule out the importance of bromine chemistry under tropical conditions at this time cannot be justified. This point has been brought into focus from prior work that even at levels of 1 pptv, the effect of BrO oxidation on DMS can still be quite significant. Thus, as in the case of DMS conversion to SO₂, future studies will be needed. In the latter case there will need to be a specific focus on halogen chemistry. Such studies clearly must involve specific measurements of radical species such as BrO.     

The Cloud Ice Mountain Experiment (CIME) 1998: experiment overview and modelling of the microphysical processes during the seeding by isentropic gas expansion

The second field campaign of the Cloud Ice Mountain Experiment (CIME) project took place in February 1998 on the mountain Puy de Dôme in the centre of France. The content of residual aerosol particles, of H₂O₂ and NH₃ in cloud droplets was evaluated by evaporating the drops larger than 5 μm in a Counterflow Virtual Impactor (CVI) and by measuring the residual particle concentration and the released gas content. The same trace species were studied behind a round jet impactor for the complementary interstitial aerosol particles smaller than 5 μm diameter. In a second step of experiments, the ambient supercooled cloud was converted to a mixed phase cloud by seeding the cloud with ice particles by the gas release from pressurised gas bottles. A comparison between the physical and chemical characteristics of liquid drops and ice particles allows a study of the fate of the trace constituents during the presence of ice crystals in the cloud.In the present paper, an overview is given of the CIME 98 experiment and the instrumentation deployed. The meteorological situation during the experiment was analysed with the help of a cloud scale model. The microphysics processes and the behaviour of the scavenged aerosol particles before and during seeding are analysed with the detailed microphysical model ExMix. The simulation results agreed well with the observations and confirmed the assumption that the Bergeron–Findeisen process was dominating during seeding and was influencing the partitioning of aerosol particles between drops and ice crystals. The results of the CIME 98 experiment give an insight on microphysical changes, redistribution of aerosol particles and cloud chemistry during the Bergeron–Findeisen process when acting also in natural clouds.     

影响1991年和1994年南海夏季风爆发迟早的物理因子探讨

通过使用美国NCEP/NCAR再分析资料,利用纬向平均的局地经向环流模式成功地模拟了1991年(爆发晚年)和1994年(爆发早年)南海夏季风的建立过程,经过分析发现,虽然南海夏季风爆发时近地面南风均含有由气压梯度力驱动的地转成分和由除了气压梯度力外的所有动力和热力驱动的非地转成分,且与三维温度梯度有关的温度平流和对流均有正贡献作用,但各因子在(这两年对南海夏季风环流建立时起正贡献的)排序上有明显的差异,主要的差异为:对1991年6月7日00UTC而言,引起地转风的气压梯度力和引起非地转风的热力及动力的合力作用相当.在引起地转偏差的因子中,起正贡献作用的主要因子是潜热加热.而对1994年5月2日00UTC而言,气压梯度力作用相对较小,在引起地转偏差的因子中,起正贡献作用的最大因子是平均纬向温度平流.另外,边界效应独自对模拟的南海近地面最大南风的贡献占42%.引起南海近地层非地转南风的热力和动力因子(稳定度)在1994年5月2日00UTC(早年)均比1991年6月7日00UTC(晚年)大(小).     

Spatial modelling of air temperature and precipitation for Andorra (Pyrenees) from daily circulation patterns

Based on the daily sea level pressure (SLP) circulation catalogue obtained by Esteban, Martin-Vide and Mases, Int J Climatol 26:1501–1515, (2006) for Western Europe, high-resolution maps of daily maximum and minimum temperature, mean daily precipitation and daily precipitation probability have been obtained for Andorra (Pyrenees). The 20 daily-circulation patterns cover the period 1960–2001 and were generated using new approaches based on the rotated principal component analysis (PCA) and clustering technique. The final maps of Andorra associated with each circulation pattern have been constructed using altitude, latitude, continentality and solar radiation as multiple regression predictors (Ninyerola, Pons and Roure, Int J Climatol 20:1823–1841, 2000). The daily temperature and rainfall series used from Andorran, French and Catalan/Spanish weather stations have been checked for data quality. The results confirm the complexity of the spatial distribution of meteorological phenomena over mountainous areas such as in Andorra, and show the importance of the Mediterranean and Atlantic influence upon the climate of this country of the Pyrenees. On the other hand, different tests have been made showing that the classification results could improve the resulting interpolated climate maps by the use of the circulation-pattern frequencies.     

Automated mechanism generation. Part 2: application to atmospheric chemistry of alkanes and oxygenates

In this study, an automated mechanism generation framework was applied to atmospheric chemistry of volatile organic compounds (VOCs) and nitrogen oxides (NO _x ). The framework generates reactions with minimal input based on a small set of reaction operators and includes a hierarchy for specifying rate constants for every reaction created. Mechanisms were generated for formaldehyde-air-NO _x , acetaldehyde-formaldehyde-n-octane-air-NO _x , and acetone-air-NO _x , and the model results were compared to experimental data obtained from smog chambers and to the SAPRC-99 lumped models. The models generated captured the experimental data very well, and their mechanistic formulation provided new insights into the controlling reaction pathways to pollutant formation. The approach applied here is sufficiently general that it can be applied to a wide range of alkane and oxygenate mixtures.     

The Assessment of Global Surface Temperature Change from 1850s:The C-LSAT2.0 Ensemble and the CMST-Interim Datasets

Based on C-LSAT2.0,using high-and low-frequency components reconstruction methods,combined with observation constraint masking,a reconstructed C-LSAT2.0 with 756 ensemble members from the 1850s to 2018 has been developed.These ensemble versions have been merged with the ERSSTv5 ensemble dataset,and an upgraded version of the CMSTInterim dataset with 5°×5°resolution has been developed.The CMST-Interim dataset has significantly improved the coverage rate of global surface temperature data.After reconstruction,the data coverage before 1950 increased from 78%?81%of the original CMST to 81%?89%.The total coverage after 1955 reached about 93%,including more than 98%in the Northern Hemisphere and 81%?89%in the Southern Hemisphere.Through the reconstruction ensemble experiments with different parameters,a good basis is provided for more systematic uncertainty assessment of C-LSAT2.0 and CMSTInterim.In comparison with the original CMST,the global mean surface temperatures are estimated to be cooler in the second half of 19th century and warmer during the 21st century,which shows that the global warming trend is further amplified.The global warming trends are updated from 0.085±0.004℃(10 yr)^–1and 0.128±0.006℃(10 yr)^–1to 0.089±0.004℃(10 yr)^–1and 0.137±0.007℃(10 yr)^–1,respectively,since the start and the second half of 20th century.