A role of aerosol particles in atmospheric ice nucleation

Considered is the process of ice nucleation in the atmosphere as a result of heterogeneous condensation of water vapor in surface inhomogeneities of aerosol particles and of subsequent heterogeneous crystallization of supercooled water accumulation. It is revealed that the size, structure, and composition of aerosol particles determine the thermal regime of crystallization.     

Surface aerosol measurements at Barrow during AGASP-II

Measurements at Barrow during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), conducted in April 1986, showed no rapid long-range transport from lower-latitude source regions to Barrow, and only limited vertical transport from above the boundary layer to the surface. New aerosol size distribution measurements in the 0.005–0.1 m diameter size range using a Nuclepore-filter diffusion battery apparatus showed a median diameter of about 0.01 m during times of high condensation nucleus (CN) concentrations. Aerosol black carbon concentrations exceeding 400 ng m^–3 were detected at the surface and were more strongly correlated with CN concentrations than with aerosol scattering extinction (_sp), suggesting that aerosol carbon was generally associated with small particles rather than large particles. Measurements at Barrow during AGASP-I, conducted in March–April 1983, showed a series of aerosol events detected at the ground that were caused by rapid long-range transport paths to the vicinity of Barrow from Eurasia. These events were strongly correlated with aerosol loading in the vertical column (optical depth).     

Shortwave aerosol optical depth of Arctic haze measured on board the NOAA WP-3D during AGASP-II,April 1986

Measurements of spectral aerosol optical depth in the Alaskan and Canadian Arctic were made from the NOAA Lockheed WP-3D aircraft as part of the second Arctic Gas and Aerosol Sampling Program (AGASP-II) during April 1986. The flight tracks and altitudes flown enabled measurements of the vertical and horizontal distribution of aerosol optical depth in the troposphere as well as direct determination of the stratospheric component. Tropospheric aerosol optical depth ranged from about 0.1 to 0.7. The factor of 7 variability sometimes occurred within 50 km horizontally; comparable variability occurred within less than 1 to 2 km vertically. The Angstrom exponents of the spectral optical depths ranged from 0.5 to 2.0, and some of the variability was apparently related to distinct aerosol regimes.     

Aerosol black carbon measurements in the Arctic haze during AGASP-II

During the second Arctic Gas and Aerosol Sampling Program conducted in April 1986, we performed measurements of the optically absorbing carbonaceous component of the ambient aerosol from the NOAA WP-3D aircraft operating between sea level and 10 km altitude. We collected the aerosol of filters that were exposed for several hours; we also operated the aethalometer to measure the concentration of aerosol black carbon in real time. The filter analyses represent averages over the altitude range and time span during which the filter was collecting. The real-time results were sorted by altitude to calculate vertical profiles of black carbon concentration. Values typically ranged from 300 to 500 ng m^–3 at lower altitudes, decreasing gradually to 25 to 100 ng m^–3 at 8–10 km. Strong stratification at lower altitudes was frequently observed. The magnitude of these concentrations suggests that the sources are distant regions of considerable fuel consumption. The presence of this material in the tropospheric column and its probable deposition to the high-albedo surface may result in perturbations of the solar radiation balance. The concentrations measured at the highest altitudes may mean that particulate carbon and accompanying emissions for which it is a tracer are mixing into the stratosphere.     

三套冰晶核化参数化方案的对比分析

基于大气模式CAM5对比分析了三套基于物理过程发展而来的冰晶核化参数化方案,包括BN方案、KL方案和CAM5自带的LP方案。针对三个方案的离线测试结果表明,由LP和BN方案计算得出的冰晶数浓度随硫酸盐溶液滴的数浓度增加而明显增加,而KL方案对硫酸盐溶液滴的数浓度不敏感;CAM5模拟结果显示,这三套方案得出的云辐射强迫、冰晶数浓度及其概率分布非常相似,基本上都接近观测。但是,使用KL方案得出的全球平均云长波辐射强迫从工业革命前到当代增加0.05 W·m~(-2),明显低于LP方案的0.36 W·m~(-2)和BN方案的0.33 W·m~(-2);由此可见,选择哪个冰晶核化参数化方案不会明显影响模式对冰云的模拟性能,但对评估人为产生气溶胶的间接效应可能有显著影响。     

On Mechanisms of Nucleation of Ice Crystals by Aerodynamic Cooling

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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.     

Physical characterization of aerosol particles during nucleation events

Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July–21 August 1998 and 20 March–24 April 1999) in Hyytiälä, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm⁻³ and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm⁻³. A coarse mode was also present, extending up to sizes of 20 μm having a number concentration of 1.2 cm⁻³, volume mean diameter of 2.0 μm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm⁻³, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.     

CICE海冰模式中反照率相关参数对北极海冰模拟的影响

国家气候中心气候系统模式BCC_CSM2.0最新耦合了美国Los Alamos国家实验室发展的海冰模式CICE5.0,为试验模式中与反照率相关参数的敏感性及其对模拟结果的影响,提高模式对北极海冰的模拟能力,选取海冰模式中3个主要参数进行了敏感性试验。利用以BCC_CSM2.0耦合框架为基础建立的海冰-海洋耦合模式,选取CORE资料为大气强迫场开展试验,试验的3个参数分别为冰/雪表面反射率、雪粒半径和雪粒半径参考温度。结果表明,参数取值的不同对北极海冰的模拟有显著的影响,优化后的取值组合极大提高了模式的模拟能力,主要表现在:（1）改善了对北极冬季海冰厚度的模拟,海冰厚度增大,与观测资料更为吻合;（2）显著提高了对北极夏季海冰密集度的模拟能力,从而模拟的北极海冰范围年际循环与观测更为一致。参数取值的优化改进了模式对海冰反照率的模拟,进而影响了冰面短波辐射的吸收和海冰表层的融化,最终提高了模式对海冰密集度和厚度的模拟效果。      

An experimental study of aerosol scavenging by hexagonal plate ice crystals

The scavenging efficiency, E, of small hexagonal plate ice crystals for aerosol particles has been measured in a series of laboratory cloud experiments. The ice crystal diameters, D μm ranged from 35 to 150 μm with aerosol particles in the range 4 to 6 μm. An ice crystal replication technique made possible the individual examination of more than 43m500 individual crystals from which the relation: log₁₀ E = 1.554 − 1.047 log₁₀D was established with values of E in the range 0.2–0.9 corresponding to the range of crystal sizes investigated. For some crystal collectors, values of E extended above unity and this was attributed to wake capture, oscillations and the extended sweep out path of the ice crystals associated with their spiral fall pattern.     

Arctic aerosol and Arctic climate: Results from an energy budget model

An energy budget model is used to study the effect on Arctic climate of optically active aerosol in the Arctic atmosphere. The dependence of the change in surface temperature on the vertical distribution of the aerosol and on the radiative properties of the aerosol-free atmosphere, the Arctic surface, and the aerosol, itself, are calculated. An extensive sensitivity analysis is performed to assess the degree to which the results of the model are dependent upon the assumptions underlying it.List of Symbols Used I ₀ Solar flux at the top of the Arctic Atmosphere (Arctic here means 70° N latitude to the pole) - a _S Surface albedo of the Arctic (a _S ^c is the value of surface albedo at which the sign of the surface temperature perturbation changes) - Reflection coefficient of the aerosol-free Arctic atmosphere - Absorption coefficient of the aerosol-free Arctic atmosphere - Transmission coefficient of the aerosol-free Arctic atmosphere - RI ₀ Total flux of sunlight reflected from the Arctic - A _A I ₀ Total flux of sunlight absorbed in the Arctic atmosphere - A _S I ₀ Total flux of sunlight absorbed at the Arctic surface - A _aer I ₀ Total flux of sunlight absorbed in the Arctic aerosol - Q _A Net atmospheric flow of energy, per unit of Arctic surface area, north across 70° N latitude - Q _S Net oceanic flow of energy, per unit of Arctic surface area, north across 70° N latitude - E Convective plus latent heat fluxes from surface to atmosphere - F _A Net flow of energy to the Arctic atmosphere - F _S Net flow of energy to the Arctic surface - T _A An effective temperature of the Arctic atmosphere - T _S Surface temperature of the Arctic - w Single-scattering albedo of the aerosol - t Optical depth of the aerosol - g Fraction of incident radiation scattered forward by the aerosol - Reflection coefficient of the aerosol - Absorption coefficient of the aerosol - Transmission coefficient of the aerosol - p,q Number of atmospheric layers and the inverse of the fraction of incident IR absorbed in each layer in the energy budget model - F,G,H Measures of the amount of IR-active atmosphere above the surface, the aerosol, and the clouds     

不同类型ENSO事件对初冬北极海冰的影响

基于1951—2019年NCEP/NCAR再分析资料、Hadley环流中心海温、海冰密集度资料,通过合成分析和诊断温度异常方程,研究不同类型ENSO对初冬北极海冰的影响。结果表明,EP La Ni1a发展年初冬(11—12月),巴伦支—喀拉海海冰异常减少;CP La Ni1a发展初冬,巴伦支—喀拉海海冰异常增加。EP和CP型El Ni1o对初冬北极海冰的影响类似：格陵兰海海冰异常减少,而哈德逊—巴芬湾海冰异常增加。不同类型ENSO对初冬北极海冰的影响主要通过产生不同的大气遥相关,引起同期和前期的海表气温异常而实现。     

冰晶核化对雷暴云闪电行为影响的数值模拟研究

为了探讨冰晶核化对雷暴云闪电行为的影响,通过已有的三维对流云起、放电模式探讨对比了3种冰晶核化方案,分别为原模式中的经验公式YS方案及与气溶胶相关的DE方案和LP方案。研究表明冰晶核化方案对雷暴云内冰晶微物理发展特征、起电及放电过程均有一定影响。模拟结果显示:(1)考虑了气溶胶的两种新参数化方案中冰晶粒子在高温区(高于-13.8℃)出现,在雷暴云发展过程中DE方案和LP方案冰晶的垂直分布均大于YS方案。(2)DE方案和LP方案中高温区出现的冰晶所带电荷极性有明显的反转现象,导致雷暴云电荷结构产生差异;雷暴云发展旺盛时刻DE方案和LP方案出现三级性电荷结构,而YS方案在整个雷暴云过程都是偶极性,并且DE方案和LP方案中电荷空间分布区域更加广泛。(3)不同核化方案下雷暴云放电特征存在差异,YS方案在偶极性电荷结构背景下没有负地闪产生,而DE方案和LP方案中次正电荷区的存在促进了负地闪的发生,并且负先导出现在较低的高度范围内;DE方案和LP方案中电荷量级较大,因此云闪发生频次以及正、负先导传播次数增加明显。     

The impact of Arctic sea ice on the Arctic energy budget and on the climate of the Northern mid-latitudes

The atmospheric general circulation model EC-EARTH-IFS has been applied to investigate the influence of both a reduced and a removed Arctic sea ice cover on the Arctic energy budget and on the climate of the Northern mid-latitudes. Three 40-year simulations driven by original and modified ERA-40 sea surface temperatures and sea ice concentrations have been performed at T255L62 resolution, corresponding to 79?km horizontal resolution. Simulated changes between sensitivity and reference experiments are most pronounced over the Arctic itself where the reduced or removed sea ice leads to strongly increased upward heat and longwave radiation fluxes and precipitation in winter. In summer, the most pronounced change is the stronger absorption of shortwave radiation which is enhanced by optically thinner clouds. Averaged over the year and over the area north of 70° N, the negative energy imbalance at the top of the atmosphere decreases by about 10?W/m² in both sensitivity experiments. The energy transport across 70° N is reduced. Changes are not restricted to the Arctic. Less extreme cold events and less precipitation are simulated in sub-Arctic and Northern mid-latitude regions in winter.     

BCC-CSM2-MR模式对北极海冰和气候的模拟及预估

基于第六次耦合模式比较计划(CMIP6),使用新一代全球模式BCC-CSM2-MR的历史试验和未来共享社会经济路径(SSPs)数据,依据Hadley中心的海表面温度和海冰密集度数据及NCEP/NCAR I再分析资料,评估了BCC-CSM2-MR模式对北极海冰及北极气候的模拟能力,并对未来变化进行了预估.结果表明:BCC...     

Modeling of fast ice evolution in the Arctic seas

A one-dimensional model of fast ice wind-induced break-up developed before was adapted for two-dimensional case that enabled to explain many regularities of this phenomenon. A numerical scheme is proposed of the integration of the acting stresses and potential resistivity by the fast ice area as well as the method for taking into account the correlation between the wind direction and prevailing coastline orientation that enables to simulate practically any combination of tensile and shearing stresses in the basins of arbitrary shape. The seasonal variability of strengthening ice properties is taken into account. All numerical tests carried out within the frameworks of this investigation demonstrated the qualitative and, partly, quantitative similarity of computation results and regularities observed in nature. The model sensitivity to the variation of some parameters is studied. The limits of model applicability are discussed and the directions of further research are proposed.