NIM陆面过程模式的研究Ⅱ：青藏高原夏季陆面过程的数值模拟

采用南京气象学院（NIM）5层陆面过程模式，利用1979年5－8月“青藏高原气象科学实验”资料模拟和分析了夏季青藏高原不同地区的陆面特征和地表能量特征。并将模拟值与根据观测资料计算得到的感热和潜热以及观测得到的净辐射、土壤温度、土壤热通量进行了对比。结果表明，NIM5层陆面过程模式可以模拟青藏高原夏季不同下垫面情形下的能量交换过程。     

典型干旱区陆面模式模拟检验

利用2000年9月至2001年8月"我国西北干旱区陆-气相互作用试验(NWC-ALIEX)"敦煌站的陆面过程观测资料,基于已有的参数化结果,模拟了敦煌主要陆面特征。结果表明:典型干旱区敦煌夏季感热通量与潜热通量差异显著,感热几乎是潜热的4倍,冬季二者都很小。模式对地表温度模拟较好,但高估了浅层土壤湿度峰值;对向上辐射模拟较好,但对净辐射的模拟存在较大偏差;同时高估了地表能量的峰值。模式结果表明参数化方案对干旱区陆面过程模式具有一定的改进作用。     

CoLM模式对青藏高原中部BJ站陆面过程的数值模拟

利用公共陆面模式Common Land Model(CoLM)及"全球协调加强观测计划之亚澳季风青藏高原试验"(CAMP/Tibet)中那曲地区Bujiao(BJ)站2002—2004年的观测资料对该地区进行了单点数值模拟试验。通过比较模拟与观测的地表能量通量,表明CoLM较成功地模拟了该地区的能量分配。模式对向上的短波辐射、向上的长波辐射、净辐射及土壤热通量模拟得较好,但冬季存在偏差。进一步比较了模拟和观测的土壤温度及土壤湿度,发现浅层60 cm土壤温度模拟较好,深层存在偏差,表现为土壤温度变化滞后于实际变化。土壤湿度总体偏小,尤其是冬季冻结期,土壤冻融过程中忽略了土壤液态水在温度0℃以下仍能存在,含冰量模拟偏高。     

SiB2和SiB3对高寒草甸和茶树地表能量通量模拟的比较

运用简单生物圈模式第2版(SiB2)和第3版(SiB3),分别模拟青藏高原两个观测站(那曲、安多)和长江三角洲苏州东山观测站的近地面能量收支,并与相应观测数据进行比较研究,分析SiB2、SiB3模拟结果和观测资料产生差异的原因,以此来认识上述地区地表能量收支特点。结果表明,SiB2和SiB3模拟的近地面能量通量与观测数据有较好的一致性。对感热通量,那曲和安多站SiB3比SiB2模拟的结果更接近观测资料,但苏州站SiB2模拟的结果与观测资料更吻合;对潜热通量,SiB3比SiB2模拟的日变化与观测资料更一致,SiB3的模拟结果与观测资料(除苏州站外)相关系数都在0.8以上;对地表土壤热通量,SiB2和SiB3模拟结果与观测数据相关系数都在0.8以上;对净辐射通量,SiB2和SiB3模拟结果与观测资料相关系数接近1.0。与SiB2相比,SiB3引用通用陆面模式的土壤描述并增加对冠层空间层温度、湿度和痕量气体的预报,使其能够改善潜热通量和土壤热通量的模拟,但对复杂下垫面的感热和净辐射通量模拟能力提高不明显。     

陆面过程模式CoLM和NCAR_CLM3.0对中国典型森林生态系统陆气相互作用的模拟 I. 不同模式模拟结果的初步分析

CoLM(Common Land Model)和NCAR_CLM3.0(NCAR Community Lanol Model 3.0)是目前国际上广为应用的两个发展比较完善的陆面过程模式.本研究利用中国陆地生态系统通量观测研究网络(Chi-naFLUX)在长白山温带混交林和千烟洲亚热带人工针叶林观测站点的长期连续强化观测资料,对这两个模式在上述地区的模拟性能进行了初步评估.同观测资料的对比表明,两个模式均能较好地模拟出观测站点地表能量和水分平衡的基本特征,其中,CoLM对潜热通量的模拟性能更好.以对潜热通量为期1年的日均值的模拟为例,COLM和CLM3.0在长白山观测站模拟值和观测值时间序列的相关系数分别为0.80和0.65,在千烟洲站分别为0.69和0.64,均通过了0.01的信度检验;两个模式对全年平均的模拟与观测日平均值的比值在长白山分别为1.21和0.86,在千烟洲分别为0.83和0.60.研究结果表明,这两个陆面过程模式可以作为研究这两种典型森林生态系统陆气交换的基本工具.同时,对模式模拟性能差异的深入分析将有助于进一步改进陆面模式的参数化过程,为相关研究奠定更坚实的基础.     

青藏高原西部冻融期陆面过程的模拟分析

利用CAMP/Tibet中CEOP-EOP3改则站2002年10月—2003年9月的观测资料作为强迫场,运用陆面过程模式CoLM(Common Land Model),对青藏高原西部陆面特征的模拟研究表明,在高原西部地表能量平衡过程中,冬半年,感热通量占主要地位,潜热通量较小;尤其在冻结期,潜热通量几乎等于零。但在高原西部的融冻期,潜热通量有显著变化。在干季向湿季转化时段的5月中下旬,表层土壤由于融冻而引起的频繁水分相变,使得潜热通量随之变化并开始增加,Bowen比由大变小。地表有效通量的变化与降水及土壤表层频繁的冻结—消融相联系。     

改则地区气候变化对植被生理过程的影响及反馈效应的模拟研究

利用1997年10月1日至1998年9月30日设置在青藏高原西部改则的自动气象站观测资料作为强迫场,采用大气-植被相互作用模式(AVIM)对改则地区气候变化对植被生长过程的影响及反馈效应进行了模拟研究。结果表明,AVIM模式对青藏高原西部陆面过程具有一定模拟能力,能够较真实地模拟出地表特征量的变化特点。通过敏感性试验发现,青藏高原气候变化对植被生理生长过程有明显影响:降水增加有利于植被生长,尤其在雨季最为明显,其他季节无太大变化;气候变暖对植被生理过程的综合作用是植被净光合作用的变化,即春季增强,夏季减弱,秋季和冬季变化不大;"暖湿化"对高原植被生态系统的影响主要是春季和夏季植被活动增强,尤其春季最为明显。植被物理特性参数可以在相当大程度上改变陆面过程,进而导致高原热源发生变化,因此,为准确估计地表能量收支,对模式陆面参数进行深入研究是必要的。     

青藏高原单点地气交换过程的模拟试验

利用GAME-Tibet 1998 IOPs的外场观测资料,采用单点陆面过程气柱模式CLSM对青藏高原的昌都(Amdo)站和改则(Gaize)站的地气交换过程进行了模拟试验,模拟结果与观测分析的对比表明：模式对两个站陆面特征的变化和陆气之间的交换给出了比较合理的模拟结果,模拟结果与观测结果较一致。这在一定程度上表明,CLSM模式具有描述夏季高原地区两种不同下垫面陆面状况基本过程的能力。     

藏北高原地表能量和边界层结构的数值模拟

利用耦合了NCAR LSM陆面过程的中尺度模式MM5V3.7和2002年8月CAMP/Tibet加强期的观测资料,对藏北高原地区地气交换过程进行了48 h模拟研究。模式较好地模拟了该地区的山谷风环流;并将模拟的地表通量在中尺度区域上与NCEP/NCAR全球大气再分析格点资料(NNRP)获得的结果进行了比较,同时也与单站的实测值进行了比较,结果显示:模拟的地表通量与NNRP得到的结果比较吻合,同时可以得到雨季时藏北、藏东地区潜热通量大于感热通量,而高原西部感热通量大于潜热通量,这与观测试验分析结果一致;与单站试验结果比较,模拟的感热通量与实测值一致,潜热通量的模拟值和实测值有一定差别。模拟的边界层位温廓线与实测值比较,模式模拟的对流混合层和夜间残留层都与实测结果吻合,但模拟的混合层高度较实测值高。由此来看,中尺度模式MM5V3.7能够较好地模拟藏北高原的地表能量和边界层结构特征,但还需要进一步完善陆面过程和物理过程参数化方案。     

青藏高原积雪对陆面过程热量输送的影响研究

利用1979-2016年中国区域长时间序列逐日雪深资料,分析了青藏高原积雪深度与积雪日数的分布及变化特征,并将积雪期划分为三个阶段(积累期、鼎盛期和消融期),结合ERA-Interim月平均再分析资料,分析了积雪与地表热状况(气温、地表和土壤温度)和能量输送量(地表净短波辐射、地表净长波辐射、感热通量、潜热通量、地表热通量和土壤热通量)的相关关系,初步探讨了积雪在高原陆面过程中的作用。结果表明:研究时间范围内青藏高原积雪(深度和日数)主要呈减少趋势,仅在黄河源区及高原边缘地区为增加趋势,积雪鼎盛阶段(1-2月)的减少趋势最显著;高原积雪对地表主要起降温作用,深层土壤温度对积雪的响应存在滞后性,积雪的减少抑制了土壤向上的热量输送进而不利于冻土的发育;高原积雪与地表感热和地表热通量主要呈现负相关关系,潜热通量与积雪也呈负相关特征但比感热通量的相关性小。由于ERA-Interim资料对高原积雪深度的描述与本研究使用的卫星遥感积雪深度存在较大偏差(包括空间分布、气候倾向率、年际变化以及绝对大小等),导致本研究中积雪与地表热状况和热通量的相关度不高,需要通过陆面模式模拟做进一步探讨。     

Rate constants for the reactions of the NO3 radical with HCOOH/HCOO− and CH3COOH/CH3COO− in aqueous solution between 278 and 328 K

The kinetics of the aqueous phase reactions of NO₃ radicals with HCOOH/HCOO^– and CH₃COOH/CH₃COO^– have been investigated using a laser photolysis/long-path laser absorption technique. NO₃ was produced via excimer laser photolysis of peroxodisulfate anions (S₂O ₈ ^2– ) at 351 nm followed by the reactions of sulfate radicals (SO ₄ ^– ) with excess nitrate. The time-resolved detection of NO₃ was achieved by long-path laser absorption at 632.8 nm. For the reactions of NO₃ with formic acid (1) and formate (2) rate coefficients ofk ₁=(3.3±1.0)×10⁵ l mol^–1 s^–1 andk ₂=(5.0±0.4)×10⁷ l mol^–1 s^–1 were found atT=298 K andI=0.19 mol/l. The following Arrhenius expressions were derived:k ₁(T)=(3.4±0.3)×10¹⁰ exp[–(3400±600)/T] l mol^–1 s^–1 andk ₂(T)=(8.2±0.8)×10¹⁰ exp[–(2200±700)/T] l mol^–1 s^–1. The rate coefficients for the reactions of NO₃ with acetic acid (3) and acetate (4) atT=298 K andI=0.19 mol/l were determined as:k ₃=(1.3±0.3)×10⁴ l mol^–1 s^–1 andk ₄=(2.3±0.4)×10⁶ l mol^–1 s^–1. The temperature dependences for these reactions are described by:k ₃(T)=(4.9±0.5)×10⁹ exp[–(3800±700)/T] l mol^–1 s^–1 andk ₄(T)=(1.0±0.2)×10¹² exp[–(3800±1200)/T] l mol^–1 s^–1. The differences in reactivity of the anions HCOO^– and CH₃COO^– compared to their corresponding acids HCOOH and CH₃COOH are explained by the higher reactivity of NO₃ in charge transfer processes compared to H atom abstraction. From a comparison of NO₃ reactions with various droplets constituents it is concluded that the reaction of NO₃ with HCOO^– may present a dominant loss reaction of NO₃ in atmospheric droplets.     

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.     

Nitrogen and sulfur species in Antarctic aerosols at Mawson,Palmer Station,and Marsh (King George Island)

High volume bulk aerosol samples were collected continuously at three Antarctic sites: Mawson (67.60° S, 62.50° E) from 20 February 1987 to 6 January 1992; Palmer Station (64.77° S, 64.06° W) from 3 April 1990 to 15 June 1991; and Marsh (62.18° S, 58.30° W) from 28 March 1990, to 1 May 1991. All samples were analyzed for Na⁺, SO ₄ ^2– , NO ₃ ^– , methanesulfonate (MSA), NH ₄ ⁺ ,²¹⁰Pb, and⁷Be. At Mawson for which we have a multiple year data set, the annual mean concentration of each species sometimes vary significantly from one year to the next: Na⁺, 68–151 ng m^–3; NO ₃ ^– , 25–30 ng m^–3; nss SO ₄ ^2– , 81–97 ng m^–3; MSA, 19–28 ng m^–3; NH ₄ ⁺ , 16–21 ng m^–3;²¹⁰Pb, 0.75–0.86 fCi m^–3. Results from multiple variable regression of non-sea-salt (nss) SO ₄ ^2– with MSA and NO ₃ ^– as the independent variables indicates that, at Mawson, the nss SO ₄ ^2– /MSA ratio resulting from the oxidation of dimethylsulfide (DMS) is 2.80±0.13, about 13% lower than our earlier estimate (3.22) that was based on 2.5 years of data. A similar analysis indicates that the ratio at Palmer is about 40% lower, 1.71±0.10, and more comparable to previous results over the southern oceans. These results when combined with previously published data suggest that the differences in the ratio may reflect a more rapid loss of MSA relative to nss SO ₄ ^2– during transport over Antarctica from the oceanic source region. The mean²¹⁰Pb concentrations at Palmer and Marsh and the mean NO ₃ ^– concentration at Palmer are about a factor of two lower than those at Mawson. The²¹⁰Pb distributions are consistent with a²¹⁰Pb minimum in the marine boundary layer in the region of 40°–60° S. These features and the similar seasonalities of NO ₃ ^– and²¹⁰Pb at Mawson support the conclusion that the primary source regions for NO ₃ ^– are continental. In contrast, the mean concentrations of MSA, nss SO ₄ ^2– , and NH ₄ ⁺ at Palmer are all higher than those at Mawson: MSA by a factor of 2; nss SO ₄ ^2– by 10%; and NH ₄ ⁺ by more than 50%. However, the factor differences exhibit substantial seasonal variability; the largest differences generally occur during the austral summer when the concentrations of most of the species are highest. NH ₄ ⁺ /(nss SO ₄ ^2– +MSA) equivalent ratios indicate that NH₃ neutralizes about 60% of the sulfur acids during December at both Mawson and Palmer, but only about 30% at Mawson during February and March.     

Processing of oxidised nitrogen compounds by passage through winter-time orographic cloud

Four case studies are described, from a three-site field experiment in October/November 1991 using the Great Dun Fell flow-through reactor hill cap cloud in rural Northern England. Measurements of total odd-nitrogen nitrogen oxides (NO _y ) made on either side of the hill, before and after the air flowed through the cloud, showed that 10 to 50% of the NO _y , called NO _z , was neither NO nor NO₂. This NO _z failed to exhibit a diurnal variation and was often higher after passage through cloud than before. No evidence of conversion of NO _z to NO₃ ^- in cloud was found. A simple box model of gas-phase chemistry in air before it reached the cloud, including scavenging of NO₃ and N₂O₅ by aerosol of surface area proportional to the NO₂ mixing ratio, shows that NO₃ and N₂O₅ may build up in the boundary layer by night only if stable stratification insulates the air from emissions of NO. This may explain the lack of evidence for N₂O₅ forming NO₃ ^- in cloud under well-mixed conditions in 1991, in contrast with observations under stably stratified conditions during previous experiments when evidence of N₂O₅ was found. Inside the cloud, some variations in the calculated total atmospheric loading of HNO₂ and the cloud liquid water content were related to each other. Also, indications of conversion of NO _x to NO _z were found. To explain these observations, scavenging of NO _x and HNO₂ by cloud droplets and/or aqueous-phase oxidation of NO₂ ^- by nitrate radicals are considered. When cloud acidity was being produced by aqueous-phase oxidation of NO _x or SO₂, NO₃ ^- which had entered the cloud as aerosol particles was liberated as HNO₃ vapour. When no aqueous-phase production of acidity was occurring, the reverse, conversion of scavenged HNO₃ to particulate NO₃ ^-, was observed.     

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.     

The influence of light intensity,SO2, NOx and C3H6 on sulfate aerosol formation

The photochemical oxidation of SO₂ in the presence of NO and C₃H₆ was studied in a 18.2 liter pyrex reactor. When light intensity, irradiation time and SO₂ concentration were constant, SO₄ ^2- concentration, derived from the total volume of aerosol produced, peaked when [C₃H₆]/[NO] was approximately 6.0. Another increase im SO₄ ^2- formation was reached at very high ratios (>50). The experimental observations are consistent with the two SO₂ oxidation mechanisms. At low [C₃H₆]/[NO] ratios, the processes proceed via the HO–SO₂ reaction, while at high ratios the O₃–C₃H₆ adduct is assumed to oxidize SO₂ to produce SO₄ ^2- aerosols.     

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.     

FTIR studies of reactions between the nitrate radical and haloethenes

Products and mechanisms for the gas-phase reactions of NO₃ radicals with CH₂=CHCl, CH₂=CCl₂, CHCl=CCl₂,cis-CHCl=CHCl andtrans-CHCl=CHCl in air have been studied. The experiments were carried out at 295±2 K and 740±5 Torr in a 480-L Teflon-coated reaction chamber and at 295±2 K and 760±5 Torr in a 250-L stainless steel reactor. NO₃ was generated by the thermal dissociation of N₂O₅. Experiments with¹⁵NO₃ and CD₂CDCl have also been performed. The initially formed nitrate peroxynitrates decay into carbonyl compounds, nitrates, HCl and ClNO₂. In adidtion, there are indications of nitrooxy acid chlorides being produced. The reactions with CH₂=CCl₂ and CHCl=CCl₂ are more complex due to release of chlorine atoms which eventually lead to formation of chloroacid chlorides.A general reaction mechanism is proposed and the observed concentration-time profiles of reactants and products are simulated for each compound. The rate constants for the initial step of NO₃ addition to the chloroethenes are determined as: (2.6±0.5, 9.4±0.9, 2.0±0.4 and 1.4±0.4) × 10^–16 cm³ molecule^–1 s^–1 for CH₂=CHCl, CH₂=CCl₂, CHCl=CCl₂ andcis-CHCl=CHCl, respectively.