Observations of nitric acid perturbations in the winter Arctic stratosphere: Evidence for PSC sedimentation

Gaseous nitric acid (HNO3) and hydrogene fluoride (HF) have been measured in the winter Arctic stratosphere using balloon- and aircraft-based Ion Molecule Reaction Mass Spectrometry (IMRMS) instruments. Strong HNO3 perturbations were found in 1993 and 1995 which may indicate nitrification around 11-13 km and denitrification around 20 km altitude. Most likely these perturbations were caused by sedimentation of HNO3 containing aerosols followed by aerosol evaporation at lower altitudes.     

A review of global stratospheric aerosol: Measurements, importance, life cycle, and local stratospheric aerosol

Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm^− 3), increasing by factors of 2–4 (10–10³) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO₂, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO₂ have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.     

Extremely low temperatures in the stratosphore and very low total ozone amount above northern and central Europe during winter 1989

On 1 February 1989, -83.5°C was recorded in 27.8 hPa over Hohenpeißenberg, the lowest temperature in the 22-year series. This was measured together with a very low total ozone amount of 266 DU. This may be compared with nearly twice this amount on 27 February 1989. The situation was very unusual: following an extremely cold winter in the Arctic stratosphere, the stratospheric cold pole was located over southern Scandinavia on 1 February in a very southerly position. The analyzed temperatures of -92 °C in 30 hPa were also unusual. Even though the low ozone amounts over Hohenpeißenberg were probably dynamically caused, an additional very small ozone decrease due to heterogeneous reactions in altitudes from 23–28 km, where the temperatures lie below -80 °C, cannot be ruled out. Extinction measurements by the orbitting SAGE II instrument indeed show polar stratospheric clouds over Europe near 50° N during the period 31 January–2 February. Also, polar stratospheric clouds were previously observed over Kiruna at similarly low temperatures and signs of a corresponding small ozone decrease were noted there.     

On the effect of the chemical composition of atmospheric aerosol particles on nucleation scavenging and the formation of a cloud interstitial aerosol

Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation.     

2019-2020冬季北半球超强极涡事件

2019-2020冬季北极平流层极涡异常并且持续的偏强,偏冷.利用NCEP再数据和OMI臭氧数据,本文分析了此次强极涡事件中平流层极涡的动力场演变及其对地面暖冬天气和臭氧低值的影响.此次强极涡的形成是由于上传行星波不活跃.持续的强极涡使得2020年春季的最后增温出现时间偏晚.平流层正NAM指数向下传播到地面,与地面AO...     

Interannual variability of the winter stratospheric polar vortex in the Northern Hemisphere and their relations to QBO and ENSO

We investigated the interannual variations of the winter stratospheric polar vortex in this paper. EOF analysis shows that two modes of variability dominate the stratospheric polar vortex on interannual timescales. The leading mode (EOF1) reflects the intensity variation of the polar vortex and is characterized by a geopotential height seesaw between the polar region and the mid-latitudes. The second one (EOF2) exhibits variation in the zonal asymmetric part of the polar vortex, which mainly describes the stationary planetary wave activity. As the strongest interannual variation signal in the atmosphere, the QBO has been shown to influence mainly the strength of the polar vortex. On the other hand, the ENSO cycle, as the strongest interannual variation signal in the ocean, has been shown to be mainly associated with the variation of stationary planetary wave activity in the stratosphere. Possible influences of the stratospheric polar vortex on the tropospheric circulation are also discussed in this paper.     

HNO3 and PSC Measurements from the Transall: Sequestering of HNO3 in the Winter of 1994/95

In the winter of 1994/95 the TRANSALL research aircraft performed several flights in the region of the Arctic vortex during the period of low stratospheric temperatures. The results of simultaneous measurements of HNO3 column amounts by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and of aerosol backscatter profiles by the Ozone Lidar EXperiment (OLEX) are presented for two typical flight scenarios across the polar vortex boundary on December 17, 1994 and January 11/12, 1995. On December 17 and January 12, the column amounts of gaseous HNO3 decreased significantly in regions with low stratospheric temperatures. This decrease was correlated with the extent of the polar stratospheric clouds. Depolarisation measurements showed that type Ib PSCs were observed primarily, but equilibrium calculations for H2SO4/HNO3/H2O aerosols seem to underestimate the observed HNO3 sequestering.     

Nitrosyl and Nitryl Chloride Formation in H2SO4/HNO3/H2O/HCl Solutions at 200 K

Infrared spectroscopy has been used to measure the vapor pressure of chlorine containing species generated from H2SO4/HNO3/H2O/HCl solutions at 200 K. The vapor pressure was observed to be a function of solution composition. Two solution compositions were investigated. One solution remained a liquid whereas the second solution was a mixed liquid and solid phase (an ice slurry). The liquid solution had a composition of 64.6 wt.% H2SO4/4.8 wt.% HNO3/30.1 wt.% H2O/0.5 wt.% HCl and produced only vapor phase HCl. The ice slurry solution had a composition of 76.6 wt.% H2SO4/3.0 wt.% HNO3/20.1 wt.% H2O/0.3 wt.% HCl and produced HCl, ClNO, and ClNO2 vapor phase components. The sulfuric acid, nitric acid, and water content of these solutions are representative of those present in polar stratospheric clouds (PSCs), however the HCl concentrations are much higher than present within these clouds. The partitioning of chlorine between vapor phase HCl (50%) and ClNO/ClNO2 (50%) for the ice slurry solution suggests a possible mechanism of halogen activation within PSCs. A reaction mechanism to model the observed chemistry is proposed.     

On the diffusivity of trace gases under stratospheric conditions

Transport of trace gases within the gas phase to a cloud or a sulphate aerosol droplet proceeds by molecular diffusion at the gas-liquid interface. An accurate determination of the molecular diffusion coefficient has a direct bearing on estimates of trace gas uptake and scavenging. A literature search revealed that this parameter is often chosen rather arbitrarily and the choice of a particular value is constrained by the availability of experimental data which are usually available at one atmospheric pressure under laboratory conditions. Since the process of trace gas transport to droplets occur at heights much above the ground level, it is important to determine an accurate value of the diffusion coefficient at varying levels in the atmosphere. This was achieved theoretically by estimating diffusivities for some important trace gases under stratospheric conditions by a Lennard-Jones method. Molecular diffusivity of 22 trace gases (including ClONO₂, HNO₃, SO₂ and H₂O₂ which may lead to heterogeneous reactions on various surfaces) have been estimated which can be used by modellers for improved scavenging estimates.     

北半球平流层极涡崩溃早晚的环流特征及其对5月南亚降水的影响

本文采用1979—2014年NCEP/NCAR月平均再分析资料、CMAP和GPCP月平均降水资料,分析了北半球平流层极涡崩溃早晚的环流特征及其与南亚降水的关系。结果表明,北半球平流层极涡崩溃时间存在明显的年际变化特征。极涡崩溃偏早(偏晚)年,自3月开始异常信号从平流层向下传播,之后的4月,从平流层到对流层高层极区温度异常偏高(偏低),极涡异常偏弱(偏强),极夜急流异常偏弱(偏强)。结果还表明,5月南亚降水异常与平流层极涡崩溃时间的早晚存在显著相关,5月南亚降水异常与平流层极涡崩溃早晚年平流层异常信号的下传有关。当平流层极涡崩溃偏晚年,4月平流层极区表现为位势高度异常偏低,而中纬度则位势高度场异常偏高,并伴随位势高度异常场的向下传播,5月该位势高度异常场下传至阿拉伯海北部大陆上空对流层顶,形成有利于降水的环流场,导致南亚降水偏多。反之,则相反。     

Cluster Ion Reactions: Insights into Processes of Atmospheric Significance

Experimental results of ion cluster reactions withatmospherically relevant species are considered hereinto provide a unified overview of the current state ofunderstanding brought about through experimentalstudies of cluster ion reactions. This isaccomplished by first outlining the atmospheric issuesaddressed by cluster ion studies and then, summarizingthe results of numerous studies. The recent, as wellas previously published studies of cluster ionreactions, are considered in the context of gainingnew insights into the molecular details ofheterogeneous processes involving the interactions ofelectrolytes with cloud droplets, ice crystals andaerosol particles. In addition to elucidating themechanisms of these and other selected reactions andtransformations of atmospheric significance, thefindings of the uptake of acid molecules in waterclusters are shown to lead to the suggestion of a newmodel that accounts for the formation of reactioncenters involving charged sites at aqueous surfaces.     

平流层大气环流的典型系统及变化特征综述

随着大气探测技术以及计算机性能的不断提高,近年来平流层探测数据日渐丰富,中层大气模式也得到了快速发展,平流层中一些重要的物理、化学以及动力过程得以深入研究,对平流层大气环流的认识也进一步加深。本文分析了平流层准2 a振荡（Quasi-Biennial Oscillation,QBO）、平流层残余（Brewer-Dobson,BD）环流和平流层极地环流等主要的平流层大气环流系统和信号的气候态特征、形成机制、年际变率以及长期趋势等,阐述了它们的主要影响因子和过程,讨论并展望了与平流层环流有关的一些主要科学问题。     

基于静稳天气下气球探空实验的中国沙漠地区沙尘气溶胶的垂直分布（英文）

塔克拉玛干沙漠是亚洲沙尘气溶胶的重要源地。为探讨塔克拉玛干地区沙尘气溶胶的理化特性与时空变化,研究其环境与气候效应,本文分析了四个季节在中国敦煌(塔克拉玛干沙漠内)取得的探空气球观测数据,包括气溶胶的数浓度、粒径分布、质量浓度及在西风主导下的水平输送通量。气溶胶数浓度的垂直廓线显示,来自沙漠地区的矿物粒子对局地环境与气候有重要影响,且所有季节都存在长距离输送。粒子谱分布显示局地有大量粗粒子输入。结果说明,源于塔克拉玛干沙漠的沙尘气溶胶的背景输送有着重要的科学意义,需进一步研究其对东亚和西太平洋地区环境与气候的影响。     

Relationship of heterogeneous nucleation and condensational growth on aerosol nanoparticles

Heterogeneous nucleation and condensation of dibutylphthalate, octadecane, octadecanol, and octadecanoic acid vapors at various pressures on insoluble AgCl and Ag nanoparticles in a turbulent mixing condensation nuclei counter (TMCNC) have been studied theoretically. A method to interpret the particle size distributions measured with a DMA and estimate the parameters for nucleation on single particles is proposed. Based on this semi-empirical method, the Gibbs free energy is calculated and a rate of heterogeneous nucleation on single particles is estimated directly from the experimental “condensation spectra” of inactive and active CN using the DMA data. In some cases, the dependence of the Gibbs nucleation energy on the vapor supersaturation had two maximums and one minimum, instead of one maximum as described by Gibbs' classical thermodynamics of phase transitions. This phenomenon, called “double barrier nucleation” (DBN) is caused by the surface heterogeneity of nano-CN; this is first experimental verification of DBN that had been previously predicted theoretically. Two types of heterogeneity may be present: topographic or energetic. Focusing on energetic heterogeneity, a theoretical model of DBN for spherical geometry is developed. The surface heterogeneity for insoluble nano-sized CN is shown to be critical to explaining the unusual transformation of a monomodal size distribution of inactive CN into a bimodal distribution of activated CN when coagulation is excluded. Future studies will be directed toward more data for further refining the theory and developing a model that simultaneously accounts for both types of surface heterogeneity of nano-CN.     

Seasonality of the Lagged Relationship between ENSO and the Northern Hemispheric Polar Vortex Variability

This paper reports the seasonal feature of the relationship between ENSO and the stratospheric Polar Vortex Oscillation (PVO) variability in the Northern Hemisphere.It is shown that the lagged ENSO-PVO coupling relationship exhibits distinct seasonal feature,due to the strong seasonality of PVO and ENSO.Specifically,the PVO variability not only during winter,but also in autumn and spring months,is significantly correlated with ENSO anomalies leading by seasons;however,no significant effect of ENSO is found on the PVO variability in winter months of November and February.Although a significant ENSO effect is primarily observed when ENSO leads PVO by about one year,a significant correlation is also found between PVO in the following spring months (M +1 A +1) and ENSO anomalies in the previous autumn (A-1 S-1 O- 1 N -1) when ENSO anomalies lead by about 18 months.The significant correlation between PVO in various seasons and the corresponding ENSO anomalies leading by seasons could be explicitly verified in most of the individual years,confirming that the lagged ENSO effect can largely modulate the seasonal timescale variability of PVO.Moreover,the composite spatial patterns of the zonal-mean temperature anomalies further show that the ENSO effect on the PVO in various seasons is related to the interannual variability of the seasonal timescale PVO events.     

On the nonlinear response of lower stratospheric ozone to NOx and ClOx perturbations for different CH4 sources

The impact of sulfate aerosol, ClOx and NOx perturbations for two different magnitudes of CH4 sources on lower stratospheric ozone is studied by using a heterogeneous chemical system that consists of 19 species belonging to 5 chemical families （oxygen, hydrogen, nitrogen, chlorine and carbon）. The results show that the present modeled photochemical system can present several different solutions, for instance, periodic states and multi-equilibrium states appearing in turn under certain parameter domains, through chlorine chemistry and nitrogen chemistry together with sulfate aerosol as well as the increasing magnitude of CH4 sources. The existence of catastrophic transitions could produce a dramatic reduction in the ozone concentration with the increase of external sources.     

两个大气环流模式SAMIL和BCC_AGCM对北半球冬季极涡振荡的模拟对比

基于与NCEP再分析资料的比较, 本文利用大气环流模式SAMIL和北京气候中心大气环流模式BCC_AGCM的1950～1999年的AMIP试验模拟数据, 对北半球冬季环流及平流层极涡振荡的模拟性能进行了评估分析。结果表明两个模式都可以再现北半球环流基本型以及环流振荡的主导模态。对冬季气候平均态的模拟, 两个模式模拟的热带—热带外温度梯度均偏大, 极夜急流偏强, 极涡偏冷偏强;100～20 hPa平均位势高度场谐波分析表明两个模式模 拟的行星波偏弱;气候平均的10 hPa极夜急流均存在1个月的季节漂移, 200 hPa副热带西风急流较NCEP偏弱。两个模式模拟的环流变化的主导模态均代表极涡振荡, SAMIL极涡振荡的强度大于BCC_AGCM, BCC_AGCM极涡振荡的频率要高于SAMIL。连续功率谱分析表明, NCEP资料中极涡振荡存在4.6个月的显著周期, 相应地, SAMIL中为5.5个月的显著周期, BCC_AGCM中为4.8个月。NCEP资料中的极涡振荡主要发生在12～3月, SAMIL模拟的极涡振荡主要发生在2～3月, BCC_AGCM模拟的极涡振荡主要发生在2～4月。