Impact of Accurate Photolysis Calculations on the Simulation of Stratospheric Chemistry

The interpretation of atmospheric measurements and the forecasting of the atmospheric composition require a hierarchy of accurate chemical transport and global circulation models. Here, the results of studies using Bremens Atmospheric Photochemical Model (BRAPHO) are presented. The focus of this study is given to the calculation of the atmospheric photolysis frequencies It is shown that the spectral high resolved simulation of the O₂ Schumann–Runge bands leads to differences in the order of 10% in the calculated O₂ photolysis frequency when compared with parameterizations used in other atmospheric models. Detailed treatment of the NO absorption leads to even larger differences (in the order of 50%) compared to standard parameterizations. Refraction leads to a significant increase in the photolysis frequencies at large solar zenith angles and, under polar spring conditions, to a significant change in the nighttime mixing ratio of some trace gases, e.g., NO₃. It appears that recent changes in some important rate constants significantly alter the simulated BrO_x- and HO_x-budgets in the mid-latitude stratosphere.     

Stratospheric Photolysis Frequencies: Impact of an Improved Numerical Solution of the Radiative Transfer Equation

Numerical schemes for the calculation of photolysis rates are usually employed in simulations of stratospheric chemistry. Here, we present an improvement of the treatment of the diffuse actinic flux in a widely used stratospheric photolysis scheme (Lary and Pyle, 1991). We discuss both the consequences of this improvement and the correction of an error present in earlier applications of this scheme on the calculation of stratospheric photolysis frequencies. The strongest impact of both changes to the scheme is for small solar zenith angles. The effect of the improved treatment of the diffuse flux is most pronounced in the lower stratosphere and in the troposphere. Overall, the change in the calculated photolysis frequencies in the region of interest in the stratosphere is below about 20%, although larger deviations are found for H₂O, O₂, NO, N₂O, and HCl.     

辐射参数化方案对一个海气耦合模式云和辐射模拟的影响

比较Morcrette辐射方案和Fu_Liou辐射方案对NCC/IAP T63海气耦合模式云和辐射模拟的影响, 结果表明:两种方案模拟的大气顶入射辐射存在明显的差异; 晴空大气Fu_Liou方案的短波吸收能力在全球普遍较Morcrette方案低; 在60°S~60°N之间, Fu_Liou方案模拟的行星反照率更接近于ERBE卫星观测; 在对大气顶净辐射的模拟上, 除了冬季的太平洋和大西洋东岸云量明显减少的部分地区外, Fu_Liou方案对大气顶净辐射的模拟总体上较Morcrette方案有了较为明显的改善; Fu_Liou方案模拟的海洋低层云显著减少, 而热带地区高云的模拟明显增加; 由于采用了“二元云量”算法, 尽管云量有所减少, Fu_Liou方案模拟的云短波吸收作用仍有所增强, 一定程度上改进了Morcrette方案云的短波吸收作用偏弱的现象。     

典型站点气溶胶对云特性的影响

结合Cloud Sat对云的主动观测和MODIS(MODerate-Resolution Imaging Spectroradiometer)对气溶胶的被动反演,研究了典型站点气溶胶对云的宏观、微观和辐射特性的影响。结果表明,气溶胶对大陆性和海洋性站点的云均有显著影响。1)随气溶胶光学厚度(Aerosol Optical Depth,AOD)增加,水汽含量较弱站点的低层(高层)云量呈减小(增加)趋势,而水汽条件较强站点的各层云量均增大,且具有较高(较低)云顶的云层发生概率在各个站点都呈增加(减小)趋势。2)AOD的增大导致各站点云滴和冰晶粒子的有效半径均减小、大气层顶的短波和长波云辐射强迫均增强、短波云辐射强迫绝对值的加强更显著、长波云辐射强迫增加的幅度相对更大。3)气象要素在AOD大(小)值情况下的变化表明,大尺度动力条件并不能解释云的上述特性随AOD的显著改变。     

三维辐射传输模式分析非均匀云对天空辐射场影响

为了解非均匀分立云体分布状况下的天空辐射场与无云晴空辐射场的差异, 本文借助一个三维辐射传输数值模式SHDOM模拟了离散云块分布条件下的天空辐射场分布, 重点分析不同云况分布情况下“非云”大气的辐射分布特征, 并将该区域与无云晴空大气辐射场的相同区域进行了比对。工作主要从辐亮度以及450 nm/650 nm的辐射比两参数入手进行讨论。研究发现, 相对无云晴空大气, 云的存在会对周围“非云”大气散射辐射产生影响, 影响程度与云量、云及气溶胶光学厚度等参数相关。数值模拟结果表明, 在云量不太大的条件下, 无云视场空间的大部分辐射值与无云晴空相比变化很小, 集中在±2％之间。这一结果表明, 已有的一维均匀大气辐射传输模式运算结果所得云与非云相元的判据基本适用于非均匀分布的有云大气。另一方面, 模拟结果表明我们也完全可以利用非均匀有云大气中的无云视场观测结果进行大气气溶胶等晴空大气光学特征的探测研究。     

Effects of ocean particles on the upwelling radiance and polarized radiance in the atmosphere-ocean system

Based on a vector radiative transfer model of the atmosphere-ocean system, the influence of oceanic components on radiation processes, including polarization effects, was investigated in the wavelength region ranging from 0.380 to 0.865 μm. The components considered were phytoplankton, inorganic suspended material (sediment), and colored, dissolved organic matter. Due to their important roles in oceanic radiation processes, the sensitivity of the bidirectional reflectance to the rough ocean surface, represented by the wind velocity 10 m above the ocean surface, and aerosol, were taken into account. The results demonstrated that both radiance and polarized radiance just below the ocean surface were sensitive to the change of the concentrations of the considered components, while the dependence of polarized radiance on the observation geometry was more sensitive than radiance. Significant differences in the specular plane existed between the impacts of the phytoplankton and sediment on the degree of polarization just above the ocean surface at 670 nm. At the top of the atmosphere (TOA), polarization was relatively insensitive to changing concentrations of ocean particles at longer wavelengths. Furthermore, the radiance at the TOA in the solar plane was more sensitive to the aerosol optical thickness than wind velocity. In contrast, wind velocity strongly influenced the radiance at the TOA in the sun glint region, while the polarization degree showed less dependence in that region. Finally, a nonlinear optimal inversion method was proposed to simultaneously retrieve the aerosol and wind velocity using radiance measurement.     

Calculating the Climatology and Anomalies of Surface Cloud Radiative Effect Using Cloud Property Histograms and Cloud Radiative Kernels

Cloud radiative kernels (CRK) built with radiative transfer models have been widely used to analyze the cloud radiative effect on top of atmosphere (TOA) fluxes, and it is expected that the CRKs would also be useful in the analyses of surface radiative fluxes, which determines the regional surface temperature change and variability. In this study, CRKs at the surface and TOA were built using the Rapid Radiative Transfer Model (RRTM). Longwave cloud radiative effect (CRE) at the surface is primarily driven by cloud base properties, while TOA CRE is primarily decided by cloud top properties. For this reason, the standard version of surface CRK is a function of latitude, longitude, month, cloud optical thickness (τ) and cloud base pressure (CBP), and the TOA CRK is a function of latitude, longitude, month, τ and cloud top pressure (CTP). Considering that the cloud property histograms provided by climate models are functions of CTP instead of CBP at present, the surface CRKs on CBP-τ histograms were converted to CTP-τ fields using the statistical relationship between CTP, CBP and τ obtained from collocated CloudSat and MODIS observations. For both climate model outputs and satellites observations, the climatology of surface CRE and cloud-induced surface radiative anomalies calculated with the surface CRKs and cloud property histograms are well correlated with those calculated from surface radiative fluxes. The cloud-induced surface radiative anomalies reproduced by surface CRKs and MODIS cloud property histograms are not affected by spurious trends that appear in Clouds and the Earth's Radiant Energy System (CERES) surface irradiances products.     

Three-Dimensional Calculation of Photolysis Frequencies in the Presence of Clouds and Impact on Photochemistry

For atmospheric photochemistry, clouds can significantly affect actinic flux distributions. In this paper, we examine the effects of convective clouds on the three-dimensional distribution of the spectral actinic flux and on photolysis frequencies for various chemical species. Three-dimensional solutions of the UV-VIS radiative transfer equation are produced using the Spherical Harmonic Discrete Ordinary Method solution technique. This solver uses as input the 3-D cloud characteristics simulated by a dynamical cloud model. The ultraviolet and visible spectra are divided into 5 intervals in order to explore the wavelength dependency of the cloud effect on the actinic flux. Results show that the distribution of the actinic flux over the cloud domain is far from homogeneous and depends primarily on the cloud extinction associated with the hydrometeors. Maximum actinic flux is found at the top edge of the cloud and is related to scattering by ice crystals. The actinic flux is enhanced by a factor of 2 to 5, compared to clear air values, above, at the top edge, and around the cloud. The 3-D actinic flux is used to calculate the photolysis rates for some chemical species (e.g. NO₂, O₃, and HCHO). Forcomputing photolysis rates, a discretized spectral representation of the absorption wavelengths is used in the model. The calculated photolysis rates are distributed inhomogeneously throughout the cloud, and maxima are found in regions where the actinic flux is enhancement is large. Temperature effects on absorption are found in the photolysis frequencies of some species. Finally, the potential importance of this photolysis enhancement on photochemistry is studied using box model simulations. Results show that enhanced OH concentrations are found in the upper troposphere (120–200%) overthe clouds and changes in ozone production rates (+15%) are obtained in quasi-steady state conditions.     

Characteristics of Surface Solar Radiation under Different Air Pollution Conditions over Nanjing,China: Observation and Simulation

Surface solar radiation (SSR) can affect climate, the hydrological cycle, plant photosynthesis, and solar power. The values of solar radiation at the surface reflect the influence of human activity on radiative climate and environmental effects, so it is a key parameter in the evaluation of climate change and air pollution due to anthropogenic disturbances. This study presents the characteristics of the SSR variation in Nanjing, China, from March 2016 to June 2017, using a combined set of pyranometer and pyrheliometer observations. The SSR seasonal variation and statistical properties are investigated and characterized under different air pollution levels and visibilities. We discuss seasonal variations in visibility, air quality index (AQI), particulate matter (PM₁₀ and PM_2.5), and their correlations with SSR. The scattering of solar radiation by particulate matter varies significantly with particle size. Compared with the particulate matter with aerodynamic diameter between 2.5 μm and 10 μm (PM_2.5?10), we found that the PM_2.5 dominates the variation of scattered radiation due to the differences of single-scattering albedo and phase function. Because of the correlation between PM_2.5 and SSR, it is an effective and direct method to estimate PM_2.5 by the value of SSR, or vice versa to obtain the SSR by the value of PM_2.5. Under clear-sky conditions (clearness index ≥0.5), the visibility is negatively correlated with the diffuse fraction, AQI, PM₁₀, and PM_2.5, and their correlation coefficients are ?0.50, ?0.60, ?0.76, and ?0.92, respectively. The results indicate the linkage between scattered radiation and air quality through the value of visibility.     

云三维结构对加热率廓线及通量影响的模拟

大气加热率强度与结构是驱动全球大气环流的关键因素,实际加热率分布与云三维结构密切相关。作者使用三维蒙特卡洛辐射传输模式,模拟计算了云分辨模式所得3个典型三维云场的加热率廓线及通量;定义了两个参数来同时描述加热率廓线的垂直分布和强度,通过与独立像素近似算法对比,定量统计分析了高分辨率下云三维结构对辐射的影响。结果表明,在高分辨率条件下云三维结构对加热率廓线和通量影响十分显著,且不同结构云场所体现的影响各具特点,提出需要考察现有大气模式中云三维结构对当前所用加热率计算方案的订正方向。     

A Possible Photochemical Link Between Stratospheric and Near-Surface Ozone on Swiss Mountain Sites in Late Winter

Record high near-surface ozone concentrations at two elevated sites (Chaumont, 1140 m asl, and Rigi, 1030 m asl) in Switzerland were observed simultaneously with extremely low total ozone during a fair weather period in mid-February 1993. An analysis of ozone, temperature, humidity, and wind profiles suggests that the surface ozone peaks were most possibly generated within the region in a layer between about 1000 and 1500 m asl. Mean diurnal cycles of ozone concentration during the period shows a strong increase from late morning to late afternoon at Chaumont and at the same time a decrease at the high alpine site Jungfraujoch (3580 m asl). The different diurnal ozone cycles can both be explained photochemically by taking into account the large difference in NOx concentrations (about two orders of magnitude) between the sites. Photochemical processes are also indicated by the diurnal cycles of NO2 and NO concentration. As a strong photochemical activity is not expected in mid-February at 47°N, we hypothesize that the extremely low total ozone played a role. Total ozone controls the amount of UV-B radiation reaching the troposphere and thus influences photochemical processes. Using a radiation model, we calculated an increase in ozone photolysis at Chaumont and Jungfraujoch of 73% and 83%, respectively, on the day with the lowest total ozone (243 DU) compared to average February conditions (335 DU). It is suggested that total ozone changes have the potential to stimulate photochemistry sufficiently to produce the observed surface ozone peaks at Chaumont and Rigi of 61 and 64 ppbv, respectively. A fog layer just below Chaumont during these days probably also influenced photochemistry, but on a smaller spatial scale. Our empirical results on the influence of changing UV radiation on tropospheric photochemistry are in close agreement with model studies of other groups. Although this case study represents unique conditions, a distinct anticorrelation between near-surface ozone at Chaumont and total ozone also appears in other years (1992–1997) when selecting fair weather days in mid-February. However, other influences cannot be excluded. The selected days provide evidence of a significant photochemical source of ozone in the mid-latitude lower troposphere in late winter.     

紫外辐射传输模式计算与实际测量的比较

利用改进的离散坐标法紫外辐射传输模式,应用各种可测得的实际大气物理参数,模拟了1993年7月24日德国加尔米希-帕特科琛（Garmisch-Partenkirchen,47.47oN, 11.07oE）地面紫外辐射的全天分布,并与1993年秋天第三次欧洲紫外辐射光谱仪比对活动期间通过了严格绝对标定的奥地利英斯布鲁克（Innsbruck）大学的紫外光谱仪的实际观测资料进行了比较,进行了余弦响应订正后,计算与测量的绝对值差别很小,最大误差对地面UVB通量（280～320 nm）是0.07 W/m2（正午的通量为3.2 W/m2）。对UVA（320～400 nm）最大误差是2.6 W/m2（正午通量为54 W/m2）。计算与测量的平均偏差为5%～13%,这表明,地面紫外辐射水平也可以利用其他大气观测资料通过模式计算间接得到。     

辐射参数化的变化对模式中期和月预报的影响

在T106中期数值预报模式和T63气候模式中进行了两种辐射过程参数化的对比试验。目前在这两个模式中用作对照积分的辐射方案(OPE)是ECMWF的早期业务方案，而新的辐射方案(NEW)是ECMWF 1989年5月2日成为业务的版本。试验结果表明，OPE高估了短波水的吸收，导致太大的短波大气吸收和地表太小的向下短波辐射；OPE还低估了长波辐射冷却和大气顶的向外长波辐射(OLR)；NEW增加了地表有效辐射能量和对流层总的冷却，产生了较大的湍流热通量，对流活动加强，降水量明显增加；NEW还使平流层温度偏暖得到矫正。业务平行试验的统计检验表明，NEW对4～7天中期预报有较显著的改进。     

The Canadian Fourth Generation Atmospheric Global Climate Model (CanAM4). Part I: Representation of Physical Processes

The Canadian Centre for Climate Modelling and Analysis (CCCma) has developed the fourth generation of the Canadian Atmospheric Global Climate Model (CanAM4). The new model includes substantially modified physical parameterizations compared to its predecessor. In particular, the treatment of clouds, cloud radiative effects, and precipitation has been modified. Aerosol direct and indirect effects are calculated based on a bulk aerosol scheme. Simulation results for present-day global climate are analyzed, with a focus on cloud radiative effects and precipitation. Good overall agreement is found between climatological mean short- and longwave cloud radiative effects and observations from the Clouds and Earth's Radiant Energy System (CERES) experiment. An analysis of the responses of cloud radiative effects to variations in climate will be presented in a companion paper.

[Traduit par la rédaction] Le Centre canadien de la modélisation et de l'analyse climatique (CCmaC) a mis au point la quatrième génération du modèle canadien de circulation générale de l'atmosphère (CanAM4). Le nouveau modèle comprend des paramétrisations physiques passablement modifiées comparativement à son prédécesseur. En particulier, le traitement des nuages, des effets radiatifs des nuages et des précipitations a été modifié. Les effets directs et indirects des aérosols sont calculés à l'aide d'un schéma d'aérosols en bloc. Nous analysons des résultats de simulation pour le climat général du jour présent en mettant l'accent sur les effets radiatifs des nuages et les précipitations. Nous trouvons un bon accord général entre la moyenne climatologique des effets radiatifs des nuages pour les courtes et les grandes longueurs d'onde et les observations de l'expérience CERES (Clouds and Earth's Radiant Energy System). Une analyse de la réponse des effets radiatifs des nuages aux variations du climat sera présentée dans un article connexe.     

A finite element–spherical harmonics model for radiative transfer in inhomogeneous clouds: Part I. The EVENT model

We present a new numerical radiative transfer model for application to solar radiation transport in three-dimensional (3D) cloudy atmospheres. The code uses the finite element–spherical harmonics (FE–P_N) approximation to solve the second-order even-parity form of the transport equation. It is validated by comparison with solutions from two well-established, deterministic radiative transfer models, the one-dimensional (1D) DISORT code and the spherical harmonics discrete ordinates method (SHDOM). The cases solved show generally good agreement, but also reveal some differences. EVEn-parity Neutral particle Transport (EVENT) is very efficient at performing 1D calculations quickly and, even for quite high angular resolutions, is faster. EVENT also has a competitive speed for the simpler, less-heterogeneous multidimensional cases but it is slower than SHDOM for more variable cases. However, there is significant potential to improve the performance of EVENT; it has not yet been optimised for speed and, as such, is not a finished product. Even as it is, EVENT could be used to produce fast, lower-resolution estimates for applications where this would be sufficient, or at lower-spatial resolutions with partial homogenisation.Another difference between the models is that the SHDOM algorithm is designed for small-scale inhomogeneous cloud fields in which the grid spacing is comparable to the mean free path. Problems arise from the use of larger grid cell optical depths, with an increase in the number of iterations required and a lack of flux conservation. Neither of the models is specifically constrained to conserve flux, but the conservation of flux gives an indication of the accuracy of the solution. Increasing the spatial and angular resolution can improve the accuracy but this is not always possible for very large 3D scenes. The grid-point method of property definition in SHDOM means that it performs best for cases with a continuous variation in extinction as this avoids discontinuities in the source function. The finite clouds used in our tests have sharp boundaries that are easily defined in EVENT but the difficulties caused by these in SHDOM are evident in excesses of up to 10 fluxes.The EVENT mesh resolution is determined by the local optical depth; it has no problem in dense areas but has more trouble in coping with voids or optically thin regions. These conditions are easily handled in SHDOM through streaming of photons along discrete ordinates but EVENT must implement methods such as a ray-tracing algorithm. Cases with extreme values of the extinction coefficient are probably best avoided with EVENT, but slightly larger-scale cases with greater optical depths, not suitable for SHDOM, may be solved more easily. These factors should be considered when selecting the most appropriate method for a particular application.     

黑碳气溶胶辐射强迫全球分布的模拟研究

利用一个改进的辐射传输模式,结合全球气溶胶数据集（GADS）,计算晴空条件下冬夏两季黑碳气溶胶的直接辐射强迫在对流层顶和地面的全球分布。计算结果表明,与温室气体引起的整层大气都是正的辐射强迫不同,黑碳气溶胶的辐射强迫在对流层顶为正值,而在地面的辐射强迫却是负值。作者从理论上解释了造成这种结果的原因。对北半球冬季和夏季而言,在对流层顶黑碳气溶胶的全球辐射强迫的平均值分别为0.085W/m2和0.155 W/m2,在地面则分别为-0.37 W/m2和-0.63 W/m2。虽然气溶胶的辐射强迫主要依赖于其本身的光学性质和在大气中的浓度,太阳高度角和地表反照率对黑碳气溶胶的辐射强迫会产生很大的影响。研究指出:黑碳气溶胶在对流层顶正的辐射强迫和在地面负的辐射强迫的绝对值都随太阳天顶角的余弦和地表反照率的增加线性增大;地表反照率对黑碳气溶胶辐射强迫的强度和分布都有重要影响。黑碳气溶胶的辐射强迫分布具有明显的纬度变化特征,冬夏两季的大值区都位于30°N~90°N之间,表明人类活动是造成黑碳气溶胶辐射强迫的主要原因。     

On the Nonlinear Response of Lower Stratospheric Ozone to External Forces---The Inclusion of BrOx and Radiation Processes

In this paper the bromine family and radiative effects are considered in an updated box model under the framework of ozone-temperature feedback,in order to further analyze the possible behavior of atmospheric ozone in the lower mid-latitude stratosphere.Results show that this updated photochemical system can present several different solutions,within a certain domain of parameters,with fixed-point and periodic states appearing in turn.The temperature feedback effect introduced in this box model has not changed the topology of the ozone system.This result presents nonlinear characteristics of the ozone system,and possible trends in the stratospheric atmosphere between complex chemistry and radiation processes.     

平流层气溶胶的辐射强迫及其气候响应的水平二维分析

利用比较先进的辐射模式计算了平流层气溶胶的辐射强迫,并对之进行了参数化。结果发现平流层气溶胶的辐射强迫的水平分布不仅与其本身的水平变化有关,而且与下垫面的反照率有很大的关系。利用近期开发的二维能量平衡模式模拟了皮纳图博火山气溶胶对地面平衡温度的影响,结果表明:皮纳图博火山至喷发后1年半左右降温达最大,至喷发后第5年降温已很小。     

Photochemistry of N2O4 Adsorbed on Ice Surfaces at 193 nm

A multi-layer deposited ice film was prepared through water vapor deposition on a Ni plate in a vacuum chamber at 90 K, and was used as it was or after annealing at 140 K. NO₂ was adsorbed as N₂O₄ approximately 90 K on the ice film prepared as above, and irradiated by 193 nm excimer laser light. The time-of-flight (TOF) spectra of the desorbed species, i.e., NO₂, NO, O₂ and O, were measured by a quadrupole mass spectrometer. The photochemical process obeyed an one-photon process. The relative yields of the products and their TOF spectra were dependent on the preparation condition of the ice film and also varied with the continuation of the laser irradiation. From the ice film annealed at 140 K, NO₂, NO and O₂ were desorbed with an approximate ratio of 1:1:0.01. From the non-annealed film, the relative yield of NO₂ was much smaller than that of NO. The TOF spectrum of NO from the non-annealed ice film consisted of distinctly different two components corresponding to the 1700 and 100 K translational temperature, respectively. The fast component was lost when additional ice was deposited on the adsorbed N₂O₄. NO was supposed to be a predissociation product from the electronically excited NO₂ prepared through the photodissociation of N₂O₄.     

Evaluating the Impacts of Cloud Microphysical and Overlap Parameters on Simulated Clouds in Global Climate Models

The improvement of the accuracy of simulated cloud-related variables, such as the cloud fraction, in global climate models (GCMs) is still a challenging problem in climate modeling. In this study, the influence of cloud microphysics schemes (one-moment versus two-moment schemes) and cloud overlap methods (observation-based versus a fixed vertical decorrelation length) on the simulated cloud fraction was assessed in the BCC_AGCM2.0_CUACE/Aero. Compared with the fixed decorrelation length method, the observation-based approach produced a significantly improved cloud fraction both globally and for four representative regions. The utilization of a two-moment cloud microphysics scheme, on the other hand, notably improved the simulated cloud fraction compared with the one-moment scheme; specifically, the relative bias in the global mean total cloud fraction decreased by 42.9%–84.8%. Furthermore, the total cloud fraction bias decreased by 6.6% in the boreal winter (DJF) and 1.64% in the boreal summer (JJA). Cloud radiative forcing globally and in the four regions improved by 0.3%?1.2% and 0.2%?2.0%, respectively. Thus, our results showed that the interaction between clouds and climate through microphysical and radiation processes is a key contributor to simulation uncertainty.