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1.
Jussi Malila Antti-Pekka Hyvrinen Yrj Viisanen Ari Laaksonen 《Atmospheric Research》2008,90(2-4):303-ICNAA07
Nucleation phenomena have a great importance in many areas of science. However, the main theoretical tool to analyse these phenomena, the classical nucleation theory (CNT), has known weaknesses. A decade ago a nucleation theorem based correction to CNT was developed [McGraw, R., Laaksonen, A., 1996. Scaling properties of the critical nucleus in classical and molecular-based theories of vapor–liquid nucleation. Phys. Rev. Lett. 76, 2754–2757]. We have analysed experimental nucleation rate data of two homologous series of molecular fluids in terms of this scaling relation. Our first results suggest possible universal functional form for correction to the temperature dependence of CNT. 相似文献
2.
《Atmospheric Research》2007,83(3-4):481-488
Gradient theory (GT), a form of density functional theory (DFT), was applied to water, methanol, and ethanol using the cubic perturbed hard body (CPHB) equation of state (EOS). Compared to the standard form of classical nucleation theory (CNT), the GT results for water showed an improved temperature dependence, but the supersaturation dependence was slightly poorer. GT and several forms of CNT were also found to be in good agreement with a single high T molecular dynamics rate for TIP4P water. The rates predicted by GT for methanol and ethanol were improved by several orders of magnitude compared to CNT, but no improvement in the predicted temperature dependence of the rates was found. 相似文献
3.
Gradient theory (GT), a form of density functional theory (DFT), was applied to water, methanol, and ethanol using the cubic perturbed hard body (CPHB) equation of state (EOS). Compared to the standard form of classical nucleation theory (CNT), the GT results for water showed an improved temperature dependence, but the supersaturation dependence was slightly poorer. GT and several forms of CNT were also found to be in good agreement with a single high T molecular dynamics rate for TIP4P water. The rates predicted by GT for methanol and ethanol were improved by several orders of magnitude compared to CNT, but no improvement in the predicted temperature dependence of the rates was found. 相似文献
4.
《Atmospheric Research》2007,83(3-4):503-513
The binary water–sulphuric acid nucleation has long been considered an important path for new particle formation in the atmosphere. The formation rate depends nonlinearly on temperature and vapour concentrations. We aim to find out if atmospheric small scale and mesoscale spatial and temporal variability can increase the nucleation rate significantly. Simultaneous and separate effects of variation in temperature, humidity and sulphuric acid concentration on the mean nucleation rate have been modelled. We have assumed that the distributions of variables are Gaussian and compare the mean of simulated nucleation rates with the nucleation rate in mean conditions without variation. According to our studies the atmospheric variability can increase the mean nucleation rate by orders of magnitude but the significant effect is limited to specific conditions. The effect seems to be more important in the lower troposphere than in the upper troposphere, where temperature and sulphuric acid concentrations are lower. In addition, our model simulations indicate that the atmospheric variability can only explain part of the difference between measured and theoretically required sulphuric acid concentrations in conditions where particle formation has been observed. We have parametrised the effect of atmospheric variability as a simple correction factor for the effect of temperature and humidity variation. 相似文献
5.
Quantifying the radiative forcing due to aerosol–cloud interactions especially through cirrus clouds remains challenging because of our limited understanding of aerosol and cloud processes. In this study, we investigate the anthropogenic aerosol indirect forcing (AIF) through cirrus clouds using the Community Atmosphere Model version 5 (CAM5) with a state-of-the-art treatment of ice nucleation. We adopt a new approach to isolate anthropogenic AIF through cirrus clouds in which ice nucleation parameterization is driven by prescribed pre-industrial (PI) and presentday (PD) aerosols, respectively. Sensitivities of anthropogenic ice AIF (i.e., anthropogenic AIF through cirrus clouds) to different ice nucleation parameterizations, homogeneous freezing occurrence, and uncertainties in the cloud microphysics scheme are investigated. Results of sensitivity experiments show that the change (PD minus PI) in global annual mean longwave cloud forcing (i.e., longwave anthropogenic ice AIF) ranges from 0.14 to 0.35 W m–2, the change in global annual mean shortwave cloud forcing (i.e., shortwave anthropogenic ice AIF) from–0.47 to–0.20 W m–2, and the change in net cloud forcing from–0.12 to 0.05 W m–2. Our results suggest that different ice nucleation parameterizations are an important factor for the large uncertainty of anthropogenic ice AIF. Furthermore, improved understanding of the spatial and temporal occurrence characteristics of homogeneous freezing events and the mean states of cirrus cloud properties are also important for constraining anthropogenic ice AIF. 相似文献
6.
The binary water–sulphuric acid nucleation has long been considered an important path for new particle formation in the atmosphere. The formation rate depends nonlinearly on temperature and vapour concentrations. We aim to find out if atmospheric small scale and mesoscale spatial and temporal variability can increase the nucleation rate significantly. Simultaneous and separate effects of variation in temperature, humidity and sulphuric acid concentration on the mean nucleation rate have been modelled. We have assumed that the distributions of variables are Gaussian and compare the mean of simulated nucleation rates with the nucleation rate in mean conditions without variation. According to our studies the atmospheric variability can increase the mean nucleation rate by orders of magnitude but the significant effect is limited to specific conditions. The effect seems to be more important in the lower troposphere than in the upper troposphere, where temperature and sulphuric acid concentrations are lower. In addition, our model simulations indicate that the atmospheric variability can only explain part of the difference between measured and theoretically required sulphuric acid concentrations in conditions where particle formation has been observed. We have parametrised the effect of atmospheric variability as a simple correction factor for the effect of temperature and humidity variation. 相似文献
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9.
《Dynamics of Atmospheres and Oceans》2001,33(2):135-156
Symmetry properties of steady solutions of the barotropic quasigeostrophic vorticity equation are explored using mirror reflections with respect to mid-basin longitude and latitude. The analysis is conducted by perturbing the fully inertial solution, the zeroth-order solution or the Fofonoff mode, by introducing forcing and dissipation as a first order correction. In the context of a classical square-basin and single-gyre circulation subject to bottom friction, it is shown numerically and analytically that the full solution can be approximated by the superposition of three components each having definite symmetry properties under longitude and latitude reflections: the north–south symmetric and antisymmetric components of the zeroth-order solution and the east–west antisymmetric component of the first-order correction. The flow patterns of the individual components are discussed. 相似文献
10.
Hou Guangliang E Chongyi Liu Xiangjun Zeng Fangming 《Theoretical and Applied Climatology》2013,113(1-2):259-269
Using 1,981 pieces of temperature records extracted from a selection of tree rings, ice cores, sediments, and other materials with high-resolution historical temperature proxy data, a temperature series of the past 2,000 years on the Tibetan Plateau (TP) with 10-year intervals was reconstructed by the method of single sample correction—multi-sample average integration equations. This series shows that the warm periods mainly appeared before 235 A.D., 775–1275 A.D. and 1845–2000 A.D., while the cold periods occurred 245–765 A.D., 1045–1145 A.D., and 1285–1835 A.D. The Little Ice Age left clear evidence on the TP and its coldest period was between 1635 and 1675 A.D. The Medieval Warm Period on the TP was not as warm as that in the late twentieth century. During the nineteenth century, overall temperature tends to be warmer with a clear rising trend, and in the late twentieth century new highs broke the record of the past 2,000 years. Power spectrum analysis shows that temperature on the TP changes consistently and evidently in a 150-year cycle. This integrated series also shows clear correlations with sunspot activity and solar radiation, as high sunspot activities generally led to warmer periods, and vice versa. Solar activities and intense radiation of recent years are naturally conducive to the global warming since the nineteenth century. The combination of greenhouse gases and natural fluctuations in climate has been the main culprit behind the global warming in the twentieth century. 相似文献
11.
Growth of homogeneously nucleated water droplets: a quantitative comparison of experiment and theory
The formation of aerosols proceeds through nucleation, growth and aging stages. The understanding of nucleation and droplet growth is essential for handling the more complex atmospheric condensation processes. To achieve this goal, measurements of the nucleation rate of various systems are performed in an expansion chamber. In this manner nucleation and growth are decoupled by applying a short nucleation pulse of about 1 ms during which the nuclei are formed. The subsequent droplet growth is quantitatively monitored by Mie-scattering. To this end, the Mie-maxima and -minima are detected as a function of time and compared to theoretical Mie-scattering calculations for increasing radii. In this fashion, a wealth of growth curves for pure water depending on supersaturations, number densities of droplets, and temperatures were obtained. Following the approach of Fuchs and Sutugin [Fuchs, N.A., Sutugin, A.G., 1970. Highly Dispersed Aerosols. Ann Arbor Science Publishers, Ann Arbor; Fuchs, N.A., Sutugin, A.G., 1971. In: Hidy, G.M., Brock, J.R. (Eds.), International Reviews in Aerosol Physics and Chemistry: Topics in Current Aerosol Research (Part 2), Pergamon, New York, p. 1], we calculated theoretical growth curves taking into account the depletion of water vapor, the increase of droplet- and system-temperature, temperature-dependent functions of the diffusion coefficient, surface tension, liquid density and latent heat of condensation. The calculated growth curves and experimental data for 230, 240 and 250 K with number densities of droplets between 5×102 and 2×106 droplets/cm3 yield quantitative agreement between theory and experiment. This is remarkable in so far as the theory contains no adjustable parameters and assumes the sticking probability of the vapor molecules to be unity. Using a sticking probability smaller than 0.8 in the calculation leads to growth functions already outside the experimental error. 相似文献
12.
A.-K. Viitanen T. Mattila J.M. Mkel M. Marjamki O. Anttalainen J. Keskinen 《Atmospheric Research》2008,90(2-4):115-ICNAA07
Ion mobility spectrometry offers a robust and effective technique to study ion clusters in ambient conditions. Here, we have experimentally studied the influence of temperature on the positive ion cluster formation of 2-propanol vapor in air, along with parallel measurements for n-butyl acetate vapor in air. For both of these low proton affinity compounds in the ppm concentration range, temperatures below 0 °C tend to favor formation of dimers and trimers. The measurements indicate that approximate estimations for the fractions of these n-mers (n > 1) in the ion spectra, can be obtained by classical theory for ion induced nucleation. Presence of natural background vapors however slightly blurs the data, especially for the fraction of monomers, so that accurate prediction of the fractions of n-mers in the spectra would require more accurate information on the gas composition. The findings concerning thermal behavior of ions help to understand better ion phenomena also in field conditions. 相似文献
13.
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. 相似文献
14.
Further laboratory experiments of thunderstorm charging by ice crystal collisions with riming graupel pellets have led to results that may help account for a major difference between two independent studies reported earlier. The problem concerns values of the cloud liquid water content required to change the sign of graupel charging. The present work has noted and investigated differences in the techniques of cloud nucleation used in the two studies. In one set of measurements by Takahashi, ice crystals are nucleated continuously in a supercooled water droplet cloud, while in the other experiments by Jayaratne et al. and Saunders et al., the droplet cloud is nucleated only briefly. These two nucleation methods lead to differences in the mass of cloud particles collected on a sampling probe used to determine the liquid water content of the cloud. In the continuous nucleation case, the probe collects sufficient numbers of ice crystals to lead to a substantial overestimate of the cloud liquid water content. 相似文献
15.
A wind tunnel was constructed to study mountain lee-wave phenomena and heated-island effects. The present wind tunnel appears to have several advantages over a towing tank facility for modeling atmospheric gravity-wave phenomena, i.e., non-uniform approach flows, stationary measuring conditions, variation of boundary temperature condition in the longitudinal direction, and no slip at the wall. Simple design criteria and characteristics of the present wind tunnel are discussed. A numerical program was utilized to explain peculiar standing-wave disturbances in the wind-tunnel test section. The above disturbances seemed unavoidable under the chosen mechanical constants. Nevertheless, a practical solution was found by extending the tunnel length.Postdoctoral Fellow, Princeton University, New Jersey, U.S.A.Associate Professor, Fluid Mechanics Program, Colorado State University, Fort Collins, U.S.A. 相似文献
16.
《Atmospheric Research》2009,91(2-4):132-150
In this paper we summarize recent experimental, theoretical and observational results on the formation and growth of atmospheric nanoparticles. During the last years significant progress has occurred to explain atmospheric nucleation and initial steps of the growth. Due to climatic and health effects of fine and ultrafine particles the formation and growth of new aerosol particles is of growing interest. The question “How and under which conditions does the formation of new atmospheric aerosol particles take place?” has exercised the minds of scientists since the time of John Aitken, who in the late 1880s built the first apparatus to measure the number of dust and fog particles. However, only during the last 15–20 years has the measurement technology developed to such a level that size distributions of nanometer-size particles and concentrations of gases participating in particle formation can be measured in the atmosphere. Also from a theoretical point of view atmospheric nucleation mechanisms have not been resolved: several mechanisms such as ion-induced (or ion mediated) nucleation, ternary and kinetic (barrier-less) nucleation have been suggested. In the most recent theory, the activation of existing neutral and/or ion clusters has been suggested. 相似文献
17.
Rashid Mavliev 《Atmospheric Research》2002,62(3-4)
The construction and operating principles of the Turbulent Mixing Condensation Nucleus Counter (TM CNC) are described. Estimations based on the semiempirical theory of turbulent jets and the classical theory of nucleation and growth show the possibility of detecting particles as small as 2.5 nm without the interference of homogeneous nucleation. This conclusion was confirmed experimentally during the International Workshop on Intercomparison of Condensation Nuclei and Aerosol Particle Counters (Vienna, Austria). Number concentration, measured by the Turbulent Mixing CNC and other participating instruments, is found to be essentially equal. 相似文献
18.
王鹏飞 《南京气象学院学报》1992,(2)
《周礼》十煇为世界最早的光象分类体系。其含义历来众说纷纭。有探讨、重建并评价的必要。本文比照历史上有影响的五家十煇定义,分析其含糊矛盾之处,提出复原十煇原义的三条原则,从而重建了十煇原义表,介绍了古代观测十煇的方法。最后对《周礼》十煇这个光象分类体系进行了评价。 相似文献
19.
A new parametric bias correction method for precipitation with an extension for extreme values is compared to an empirical and an existing parametric method. The bias corrections are applied to the regional climate model COSMO-CLM (consortium for small-scale modelling – climate limited area modelling) with a resolution of 4.5 km for the time periods 1991–2000 and 2091–2100. In addition to a comparison in a cross-validation framework, a focus is laid on the investigation of extreme value correction and the effect of the bias correction on the climate change signal. According to the statistical methods used in this study, it was found that the empirical method outperforms both parametric alternatives. However, due to the limited length of the available time series, some outliers occurred, and all methods had problems correcting extreme values. The climate change signal is moderately influenced by all three methods, and the power of climate change detection is reduced. The largest effect was found for the number of dry days and the mean daily intensity, which are considerably altered after correction. 相似文献
20.
Yihe Fang Haishan Chen Zhiqiang Gong Fangshu Xu Chunyu Zhao 《Acta Meteorologica Sinica》2017,31(6):1085-1095
Based on summer precipitation hindcasts for 1991–2013 produced by the Beijing Climate Center Climate System Model (BCC_CSM), the relationship between precipitation prediction error in northeastern China (NEC) and global sea surface temperature is analyzed, and dynamic–analogue prediction is carried out to improve the summer precipitation prediction skill of BCC_CSM, through taking care of model historical analogue prediction error in the real-time output. Seven correction schemes such as the systematic bias correction, pure statistical correction, dynamic–analogue correction, and so on, are designed and compared. Independent hindcast results show that the 5-yr average anomaly correlation coefficient (ACC) of summer precipitation is respectively improved from –0.13/0.15 to 0.16/0.24 for 2009–13/1991–95 when using the equally weighted dynamic–analogue correction in the BCC_CSM prediction, which takes the arithmetical mean of the correction based on regional average error and that on grid point error. In addition, probabilistic prediction using the results from the multiple correction schemes is also performed and it leads to further improved 5-yr average prediction accuracy. 相似文献