Beryllium-7 Deposition and Its Relation to Sulfate Deposition

Deposition of ⁷Be, a cosmogenic radionuclide, was observed at the Meteorological Research Institute in Tsukuba, Japan from 1986 to 1993 and compared with those of several chemical species observed in Tsukuba over the same period. We found a correlation between the monthly depositions of ⁷ Be and SO ₄ ² -, a major acidic species. The correlation was especially strong for late spring and fall, when both species had high depositional fluxes. This correlation was also observed in precipitation samples collected daily in 1992 at the same site. The cause of this correlation is discussed in connection with the fact that the stratospheric aerosol is composed largely of SO ₄ ² -. ⁷ Be is produced in the upper atmosphere, and detection of ⁷Be, especially in spring and fall in Japan, can be regarded as detection of stratospheric aerosol. However, we conclude that the bulk of the SO ₄ ² - observed did not have a stratospheric or an upper tropospheric origin. The correlation, therefore, may present a new question regarding acidic deposition: Why does the deposition of stratospheric aerosol in Japan coincide with that of nss-SO ₄ ² - originally from anthropogenic sources on the Earth's surface?     

Latitudinal variation of measured O3 photolysis frequencies J(O1D) and primary OH production rates over the Atlantic Ocean between 50° N and 30° S

The latitudinal variation of the photolysis frequency of ozone to O(¹D) atoms, J(O¹D), was measured using a filter radiometer during the cruise ANT VII/1 of the research vessel Polarstern in September/October 1988. The J(O¹D) noon values exhibited a maximum of 3.6×10^-5 s^-1 (2 sr) at the equator and decreased strongly towards higher latitudes. J(O¹D) reached highest values for clean marine background air with low aerosol load and almost cloudless sky. The J(O¹D) data, measured under these conditions and a temperature of 295 K, can be expressed by: % MathType!MTEF!2!1!+-% feaafiart1ev1aaatCvAUfeBSjuyZL2yd9gzLbvyNv2CaerbuLwBLn% hiov2DGi1BTfMBaeXatLxBI9gBaerbd9wDYLwzYbItLDharqqtubsr% 4rNCHbGeaGqiVu0Je9sqqrpepC0xbbL8F4rqqrFfpeea0xe9Lq-Jc9% vqaqpepm0xbba9pwe9Q8fs0-yqaqpepae9pg0FirpepeKkFr0xfr-x% fr-xb9adbaqaaeGaciGaaiaabeqaamaabaabaaGcbaGaamOsaiaacI% cacaqGpbWaaWbaaSqabeaaiiaacqWF8baFaaGccaqGebGaaeykaiaa% bccacqWF9aqpcaqGGaGaaeyzaiaabIhacaqGWbGaaeiiaiaabUhacq% GHsislcaaI4aGaaiOlaiaaicdacaaIYaGaeyOeI0IaaGioaiaac6ca% caaI4aGaaiiEaiaaigdacaaIWaWaaWbaaSqabeaacqGHsislcaaIZa% aaaOGaaeiiaiaabIhacaqGGaGaam4uaiabgUcaRiaaiodacaGGUaGa% aGinaiaacIhacaaIXaGaaGimamaaCaaaleqabaGaeyOeI0IaaGOnaa% aakiaadofadaahaaWcbeqaaiaaikdaaaGccaGG9bGaaeikaiaaboha% daahaaWcbeqaaiabgkHiTiaaigdaaaGccaGGPaaaaa!5EE9!\[J({\text{O}}^| {\text{D) }} = {\text{ exp \{ }} - 8.02 - 8.8x10^{ - 3} {\text{ x }}S + 3.4x10^{ - 6} S^2 \} {\text{(s}}^{ - 1} )\] where S represents the product of the overhead ozone column (DU) and the secant of the solar zenith angle. The meridional profile of the primary OH radical production rate P(OH) was calculated from the J(O¹D) measurements and simultaneously recorded O₃ and H₂O mixing ratios. While the latitudinal distribution of J(O¹D) and water vapour was nearly symmetric to the equator, high tropospheric ozone levels up to 40 ppb were observed in the Southern Hemisphere, SH, resulting in higher P(OH) in the SH.     

A global three-dimensional model of the tropospheric sulfur cycle

The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO₂ and SO₄ ^2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr^–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO₂, and SO₄ ^2– respectively.     

山西省城市大气CO2本底筛分对比及特征分析

基于典型城市站太原站2018年3月—2019年2月的大气CO₂在线观测资料,利用筛分法(Meteorological filtering method, MET)和黑碳示踪法(Black Carbon tracer, BC)进行本底/非本底的筛分,得到了本底浓度的变化特征。结果表明,太原大气CO₂浓度季均值冬季最高,夏季最低;不同季节呈“单峰型”日变化特征,日振幅均在26.0×10^-6以上;4个季节CO₂浓度与地面风速存在显著负相关关系;CO₂浓度抬升区域主要受当地工业布局的影响,最大抬升幅度在秋季达17.4×10^-6;使用气象筛分法(MET)得到年均本底浓度为(431.4±19.9)×10^-6,人为排放等对其影响为23.5×10^-6,年振幅比同纬度其它本底站大,为34.5×10^-6;黑碳示踪法(BC)得到冬季季均本底浓度为(445.0±22.9)×10^-6,比MET筛...     

Laboratory Study of O(1S) Formation Process in the Photolysis of O3 and its Atmospheric Implications

A high-sensitive technique to detect O(¹S) atoms using vacuum ultraviolet laser-induced fluorescence (VUV-LIF) spectroscopy has been applied to study the O(¹S) production process from the UV photodissociation of O₃, N₂O, and H₂O₂. The quantum yields for O(¹S) formation from O₃ photolysis at 215 and 220 nm are determined to be (1.4 ± 0.4) × 10⁻⁴ and (5 ± 3) × 10⁻⁵, respectively. Based on thermochemical considerations, the O(¹S) formation from O₃ photolysis at 215 and 220 nm is attributed to a spin-forbidden process of O(¹S)+O₂(X³Σ_g ⁻). Analysis of the Doppler profile of O(¹S) produced from O₃ photolysis at 193 nm also indicates that the O(¹S) atoms are produced from the spin-forbidden process. In the photolysis of N₂O and H₂O₂ at 193 nm, no discernible signal of O(¹S) atoms has been detected. The upper limit values of the quantum yields for O(¹S) production from N₂O and H₂O₂ photolysis at 193 nm are estimated to be 8 × 10⁻⁵ and 3 × 10⁻⁵, respectively. Using the experimental results, the impact of the O(¹S) formation from O₃ photolysis on the atmospheric OH radical formation through the reaction of O(¹S)+H₂O has been estimated. The calculated results show that the contribution of the O(¹S)+H₂O reaction to the OH production rate is ∼2% of that of the O(¹D)+H₂O reaction at 30 km altitude in mid-latitude. Implications of the present laboratory experimental results for the terrestrial airglow of O(¹S) at 557.7 nm have also been discussed.     

Adsorption and reaction of trichlorofluoromethane on various particles

As a possible tropospheric sink of trichlorofluoromethane (CCl₃F), its adsorption and reaction on solid particles were studied with or without UV light longer than 310 nm. The adsorption and photodesorption occurred for most of the particles examined. The amounts depended not only on the BET surface area but also on the chemical property of the particles. The reaction rates were less than 0.1% h^-1. The surface induced degradation of CCl₃F in air was confirmed under photoirradiation at room temperature by the detection of Cl^- or F^- on some metal oxides. When the particles were pretreated with heat and evacuation, the reaction rate became larger and disproportionation of CCl₃F took place. The tropospheric lifetime of CCl₃F was reevaluated based on a reported model. It is suggested that the heterogeneous reaction of CCl₃F on particles may be a possible tropospheric sink.     

Satellite Measurements of Tropospheric Column O<Subscript>3</Subscript> and NO<Subscript>2</Subscript> in Eastern and Southeastern Asia: Comparison with a Global Model (MOZART-2)

Satellite measurements of tropospheric column O₃ and NO₂ in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O₃ is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO₂ is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O₃ and NO₂ fields. The analysis of the model results show that the industrial emission of NO_x (NO + NO₂) contributes about 50%–80% to tropospheric column NO₂ in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NO_x to tropospheric column O₃ ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NO_x emissions have a small effect on tropospheric O₃ in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NO_x on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.     

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 ...     

西太平洋地区大气边界层内臭氧的季节变化及其影响因子分析

利用臭氧探空资料,分析了西太平洋地区香港(Hong Kong)、那霸(Naha)和札幌(Sapporo)三个站点2000~2010年期间大气边界层内臭氧(O₃)的季节分布和年变化趋势。结果表明,三个站点O₃的季节分布存在明显的差异。其中,那霸和香港大气边界层内O₃季节平均呈双峰值分布,其峰值分别出现在春季和秋季;而札幌站为单峰分布,峰值出现在春季。造成季节分布差异的主要原因包括人为污染源和自然因素如气象条件。另外,三个站点大气边界层内O₃均呈上升趋势。其中札幌、那霸上升最快,分别达0.80 ppb a-1和0.77 ppb a-1。(ppb表示10-9,下同)香港的年际增长较不明显,但秋季增长却非常明显,高达1.21 ppb a-1。结合GOME (Global Ozone Monitoring Experiment) 和SCIAMACHY (Scanning Imaging Absorption Spectro Meter for Atmospheric Chartography)卫星反演的NO₂数据发现,过去10年中国京津唐和东北地区的对流层内NO₂柱总量增加极为迅速。这些O₃前体物通过远距离输送是导致札幌、那霸O₃浓度增加的主要原因之一。珠江三角洲人为污染源的增加及偏北气流的影响,是导致香港地区秋季O₃增加的主要原因。     

A sensitive method for measuring atmospheric concentrations of sulfur dioxide

A new sensitive method for measuring atmospheric concentrations of sulfur dioxide is presented. Samples are obtained using the mist chamber, which collects highly water-soluble gases with high efficiency, and concentrates them in a small volume of water. Particles are removed from the sampled air stream with a teflon filter, before it enters the mist chamber. After collection, the pH of the water is raised above pH 10 using sodium carbonate, then hydrogen peroxide (H₂O₂) is added to oxidize sulfur that may be present in the sulfur (IV) oxidation state, to sulfate. After a reaction time of at least 16 hours, the sulfate concentration is measured by ion chromatography. From the sulfate concentration, the water volume used in the mist chamber, and the volume of air sampled, the atmospheric concentration of SO₂ is computed. The method is not sensitive to other atmospheric sulfur gases such as DMS, SC₂, H₂S, COS, or MSH. The estimated overall precision of the method is 10%. The detection limit at the present stage of technique development is approximately 20 ppt (parts per trillion, or 10^-12 mol · mol^-1) for a 45 minute sampling time, with lower concentrations being detectable with lower precision.     

Kinetics of the Reactions of IO with HO2 and O(3P)

A discharge-flow tube coupled with resonance fluorescence and chemiluminescence detection has been used to investigate the reactions IO + HO₂ products (1) and IO + O(³P) I + O₂(2), at T = 296 ± 1 K and P = 1.7 - 2 Torr. The rate constants k_-1 and k₂ have been found to be (7.1 ± 1.6) × 10^-11 cm³ molecule^-1 s^-1 and (1.35 ± 0.15) × 10^-10 cm³ molecule^-1 s^-1, respectively.     

Characteristics of ionic components in precipitation in Kitakyushu City,Japan

Precipitation samples were collected by filtrating bulk sampler in Kitakyushu City, Japan, from January 1988 to December 1990. Volume weighted annual mean of pH was 4.93, but the pH distribution indicated that most probable value lay in the range pH 6.0–6.4. Volume weighted annual mean concentrations of major ionic components were as follows; SO ₄ ^2– : 84.2, NO ₃ ^– : 28.1, Cl^–: 86.3, NH ₄ ⁺ : 45.5, Ca²⁺: 63.3, Mg²⁺: 27.0, K⁺: 3.4, Na⁺: 69.0 µ eq l^–1. The highest concentrations of these ionic components were observed in winter and the lowest occurred in the rainy season. The ratio of ex-SO ₄ ^2– /NO ₃ ^– exhibited the lowest ratio in summer, and the highest ratio in winter. Good correlations were obtained between Cl^– and Na⁺, ex-SO ₄ ²⁺ and ex-Ca²⁺, NO ₃ ^– and ex-Ca²⁺, and NH ₄ ⁺ and ex-SO ₄ ^2– , respectively. However, no correlation between Cl^– and Na⁺ with Ca²⁺ was observed. The relationship of H⁺ with (ex-SO ₄ ^2– + NO ₃ ^– ) - (ex-Ca²⁺ + NH ₄ ⁺ ) indicated positive correlation.     

香河地区冬季NO2光解速率的变化特征及其估算方法的建立

NO₂的光解速率j(NO₂)是对流层化学研究中的一个重要的参数，它是对流层臭氧（O₃）和OH自由基的形成关键影响因子之一。本文利用香河站2017年11月至2018年1月的观测资料对NO₂的光解速率j(NO₂)、太阳辐射的变化特征，及光解速率与分波段辐射相关性进行分析，在此基础上建立了一套适合于构建香河地区j(NO₂)的参数化方案。结果表明，香河地区的j(NO₂)与太阳辐射的变化趋势基本一致，日变化均呈正午高、早晚低的单峰型。香河地区冬季j(NO₂)的变化范围是0.00046～0.0044 s-1，平均值为0.0029 s-1。j(NO₂)与晴空指数（K_S）和定义的紫外辐射晴空指数（K_UV）存在很好的相关性，因此，利用j(NO₂)与大气质量数和晴空指数的相互依赖关系，基于K_UV构建了适合于香河地区j(NO₂) 的估算方程。由于总辐射是气象站的常规观测要素，晴空指数K_S更容易获取，继而建立了通过K_S参数化计算j(NO₂)的估算方程。利用K_UV和K_S建立的j(NO₂)估算方程的瞬时估算值与观测值的平均相对误差分别为6.5%和13.9%，均方根误差分别为0.00029和0.00051。     

Production of N2O,CH4, and CO2 from soils in the tropical savanna during the dry season

Emissions of N₂O, CH₄, and CO₂ from soils at two sites in the tropical savanna of central Venezuela were determined during the dry season in February 1987. Measured arithmetic mean fluxes of N₂O, CH₄, and CO₂ from undisturbed soil plots to the atmosphere were 2.5×10⁹, 4.3×10¹⁰, and 3.0×10¹³ molecules cm^-2 s^-1, respectively. These fluxes were not significantly affected by burning the grass layer. Emissions of N₂O increased fourfold after simulated rainfall, suggesting that production of N₂O in savanna soils during the rainy season may be an important source for atmospheric N₂O. The CH₄ flux measurements indicate that these savanna soils were not a sink, but a small source, for atmospheric methane. Fluxes of CO₂ from savanna soils increased ninefold two hours after simulated rainfall, and remained three times higher than normal after 16 hours. More research is needed to clarify the significance of savannas in the global cycles of N₂O, CH₄, CO₂, and other trace gases, especially during the rainy season.     

Measurement of the photodissociation coefficient of NO2 in the atmosphere: II,stratospheric measurements

The photodissociation coefficient of NO₂, J _{NO 2}, has been measured from a balloon platform in the stratosphere. Results from two balloon flights are reported. High Sun values of J _{NO 2} measured were 10.5±0.3 and 10.3±0.3×10^-3 s^-1 at 24 and 32 km respectively. The decrease in J _{NO 2} at sunset was monitored in both flights. The measurements are found to be in good agreement with calculations of J _{NO 2} using a simplified isotropic multiple scattering computer routine.     

临安冬夏季SO2、NO2和O3体积分数特征及与气象条件的关系

对临安大气本底站2003-2004年冬、夏季二氧化氮(NO2)、二氧化硫(SO2)、臭氧(O3)进行了分析.结果表明:冬季NO2和SO2平均体积分数分别为19.48×10-9和35.74 x10-9,而夏季的平均体积分数分别为4.81×10-9和8.12×10-9,冬季高于夏季;O3在夏季的平均体积分数为33.55×10-9,略高于冬季的25.44×10-9;夜间NO2和SO2体积分数比白天高,并且NO2呈明显的单峰单谷型分布,O3也呈单峰型但峰值出现在白天.NO2、SO2体积分数存在着明显的“假日效应”,假日比非假日低,周五高于假日和非假日;但O3体积分数没有明显的假日效应.降水对SO2有明显的清除作用,但对NO2的清除作用不明显.与风向对比发现,夏季高体积分数的NO2、SO2都受到NW、WNW风的影响,冬季则分别受NE和SW、SSW风的影响;而O3受风向的影响较复杂,与局地光化学反应有关.     

1980～2013年华东小雨减少及其主要影响因子分析

本文通过对1980～2013年华东区域447站各等级降水的时空分布特征进行分析,从低空气温、水汽、相对湿度入手,采用经验正交函数分析（Empirical Orthogonal Function,简称EOF）、合成分析等诊断方法揭示小雨与低空气温、水汽、相对湿度之间的关系;根据克劳修斯-克拉珀龙（Clausius-Clapeyron）方程,从物理角度对温度和水汽含量变化对小雨减少的相对贡献进行分析,并选取长三角区域利用能见度资料分析小雨减少的特征。研究主要得出以下结论:（1）华东区域1980～2013年总降水日和总降水量分布呈现南多北少随纬度增加递减趋势,总降水日主要以小雨日为主,小雨日占总降水日的71.84%。除暴雨外,其它各等级降水均呈现出减少趋势,以小雨的减少最为显著,小雨日和小雨量区域平均减少趋势为－3.37 d (10 a)-1、－6.52 mm (10 a)-1。小雨日EOF分解的第一模态呈现了华东区域小雨日一致减少的分布特征;第二模态则体现了小雨日变化的不均匀性,具有明显的区域差异。（2）小雨日的减少是伴随着低空增温发生的,低空温度上升了0.32 K (10 a)-1,同时可降水量呈现微弱的减少趋势。小雨日的变化与低空相对湿度有很好的正相关关系,EOF分解结果也揭示了低空相对湿度具有与小雨一致的空间分布特征。合成分析表明低空气温偏高（低）年,小雨日偏少（多）,可降水量偏多（少）年,小雨日偏多（少）,相对湿度偏高（低）年,小雨日偏多（少）。（3）根据Clausius-Clapeyron方程和相对湿度公式,低空增暖使饱和水汽压增加6% K-1～7% K-1,饱和水汽压增加在水汽微弱减少的前提下,导致了低空相对湿度的显著减少,从而导致了小雨的减少。对低空温度,比湿变化对小雨的影响进行分析,发现单纯由温度变化引起的相对湿度减少为－4.83%,而单纯由于比湿变化引起的相对湿度变化为－1.91%,分析表明了低空增暖是引起小雨日减少的主要原因。（4）能见度较差的区域,年均小雨日和小雨量偏少,但是小雨的长期减少趋势主要还是由低空增暖引起的相对湿度的减少导致的。     

Atmospheric chemistry of carbon disulphide

The oxidation of carbon disulphide has been studied under conditions which are likely to pertain in the atmosphere. The quantum yield for direct photo-oxidation of CS₂ in air at 1 atm pressure, using near UV radiation was 0.012, with OCS as a major product. The rate coefficient (k ₁) for the reaction of OH with CS₂, was determined from measurements of OCS formation in the near UV photolysis of HONO?CS₂?O₂?N₂ mixtures. k ₁ was dependent on oxygen concentration rising from ≤4×10^-14 cm³ molecule^-1 s^-1 at O₂≤15 Torr to (2.0±1.0)×10^-12 cm³ molecule^-1 s^-1 at 1 atm air and 300 K. Equimolar amounts of carbonyl sulphide and sulphur dioxide were the major reaction products. The concentration of carbon disulphide in the ambient atmosphere was measured and the concentration to be expected in the background atmosphere was estimated. Rate and concentration data were used to show that carbon disulphide oxidation represents a major source for atmospheric carbonyl sulphide. It can also serve as an alternate source for atmospheric sulphur dioxide in addition to that produced from hydrogen sulphide and dimethyl sulphide. A consideration of atmospheric concentrations and rate data for these trace sulphur gases suggests that the natural sulphur budget is much smaller than the yearly amounts of sulphur dioxide emitted from anthropogenic sources.     

Flow reactor and triple quadrupole mass spectrometer investigations of negative ion reactions involving nitric acid: Implications for atmospheric HNO3 detection by chemical ionization mass spectrometry

Atmospheric nitric acid measurements by ACIMS (Active Chemical Ionization Mass Spectrometry) are based on ion-molecule reactions of CO₃ ^-(H₂O) _n and NO₃ ^-(H₂O) _n with HNO₃. We have studied these reactions in the laboratory using a flow tube apparatus with mass spectrometric detection of reactant and product ions. Both product ion distributions and rate coefficients were measured. All reactions were investigated in an N₂-buffer (1–3 hPa) at room temperature. The reaction rate coefficients of OH^-, O₂ ^-, O₃ ^-, CO₄ ^-, CO₃ ^-, CO₃ ^-H₂O, NO₃ ^-, and NO₃ ^-H₂O were measured relative to the known rate k=3.0×10^-9 cm³ s^-1 for the reaction of O^- with HNO₃. The main product ion of the reaction of CO₃ ^-H₂O with HNO₃ was found to be (CO₃HNO₃)^- supporting a previous suggestion made on the basis of balloon-borne ACIMS measurements. For the reaction of bare CO₃ ^- with HNO₃ three product ions were observed, namely NO₃ ^-, (NO₃OH)^-, and (CO₃HNO₃)^-. The reaction rate coefficients for CO₃ ^-H₂O (1.7×10^-9 cm³ s^-1) and NO₃ ^-H₂O (1.6×10^-9 cm³ s^-1) were found to be close to the collision rate. The measured k values for bare CO₃ ^- (1.3×10^-9 cm³ s^-1) and NO₃ ^- (0.7×10^-9 cm³ s^-1) are somewhat smaller. The collisional dissociations of CO₃ ^-(H₂O) _n , NO₃ ^-(H₂O) _n (n=1, 2), (CO₃HNO₃)^- and (NO₃HNO₃)^-, occasionally influencing ACIMS measurements, were also studied. Fragment ion distributions were measured using a triple quadrupole mass spectrometer. The results showed that previous stratospheric nitric acid measurements were unimpaired from collisional dissociation processes whereas these processes played a major role during previous tropospheric measurements leading to an underestimation of nitric acid concentrations. Previous ACIMS HNO₃ detection was also affected by the conversion of CO₃ ^-(H₂O) _n to NO₃ ^-(H₂O) _n due to ion source-produced neutral radicals. A novel ACIMS ion source was developed in order to avoid these problems and to improve the ACIMS method.