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1.
The Arrhenius expressions and the data plotted in Figure 2 of Rodriguez et al. 2008 give rate coefficients of approximately 2?×?10-8 cm3 molecule-1 s-1 at 255 K. Such values are approximately two orders of magnitude larger than expected from simple collision theory (Finlayson-Pitts and Pitts 1986). The rate coefficients reported at sub-ambient temperatures are substantially greater than the gas kinetic limit and are not physically plausible. The rate coefficients reported by Rodriguez et al. imply a long range attraction between the reactants which is not reasonable for reaction of neutral species such as chlorine atoms and unsaturated alcohols. We also note that the pre-exponential A factors (10-23-10-20) and activation energies (?15 kcal mol-1) are not physically plausible. We conclude that there are large systematic errors in the study by Rodriguez et al. (Atmos Chem 59:187–197, 2008).  相似文献   

2.
Expert elicitation studies have become important barometers of scientific knowledge about future climate change (Morgan and Keith, Environ Sci Technol 29(10), 1995; Reilly et al., Science 293(5529):430–433, 2001; Morgan et al., Climate Change 75(1–2):195–214, 2006; Zickfeld et al., Climatic Change 82(3–4):235–265, 2007, Proc Natl Acad Sci 2010; Kriegler et al., Proc Natl Acad Sci 106(13):5041–5046, 2009). Elicitations incorporate experts’ understanding of known flaws in climate models, thus potentially providing a more comprehensive picture of uncertainty than model-driven methods. The goal of standard elicitation procedures is to determine experts’ subjective probabilities for the values of key climate variables. These methods assume that experts’ knowledge can be captured by subjective probabilities—however, foundational work in decision theory has demonstrated this need not be the case when their information is ambiguous (Ellsberg, Q J Econ 75(4):643–669, 1961). We show that existing elicitation studies may qualitatively understate the extent of experts’ uncertainty about climate change. We designed a choice experiment that allows us to empirically determine whether experts’ knowledge about climate sensitivity (the equilibrium surface warming that results from a doubling of atmospheric CO2 concentration) can be captured by subjective probabilities. Our results show that, even for this much studied and well understood quantity, a non-negligible proportion of climate scientists violate the choice axioms that must be satisfied for subjective probabilities to adequately describe their beliefs. Moreover, the cause of their violation of the axioms is the ambiguity in their knowledge. We expect these results to hold to a greater extent for less understood climate variables, calling into question the veracity of previous elicitations for these quantities. Our experimental design provides an instrument for detecting ambiguity, a valuable new source of information when linking climate science and climate policy which can help policy makers select decision tools appropriate to our true state of knowledge.  相似文献   

3.
Developing economy greenhouse gas emissions are growing rapidly relative to developed economy emissions (Boden et al. 2010) and developing economies as a group have greater emissions than developed economies. These developments are expected to continue (U.S. Energy Information Administration 2010), which has led some to question the effectiveness of emissions mitigation in developed economies without a commitment to extensive mitigation action from developing economies. One often heard argument against proposed U.S. legislation to limit carbon emissions to mitigate climate change is that, without participation from large developing economies like China and India, stabilizing temperature at 2 degrees Celsius above preindustrial (United Nations 2009), or even reducing global emissions levels, would be impossible (Driessen 2009; RPC Energy Facts 2009) or prohibitively expensive (Clarke et al. 2009). Here we show that significantly delayed action by rapidly developing countries is not a reason to forgo mitigation efforts in developed economies. This letter examines the effect of a scenario with no explicit international climate policy and two policy scenarios, full global action and a developing economy delay, on the probability of exceeding various global average temperature changes by 2100. This letter demonstrates that even when developing economies delay any mitigation efforts until 2050 the effect of action by developed economies will appreciably reduce the probability of more extreme levels of temperature change. This paper concludes that early carbon mitigation efforts by developed economies will considerably affect the distribution over future climate change, whether or not developing countries begin mitigation efforts in the near term.  相似文献   

4.
Measurements of total peroxy radicals (HO2?+?RO2) and nitrate radical (NO3) were made on the NOAA research vessel R/V?Brown along the U.S. Gulf Coast during the TexAQS 2006 field campaign. The measurements were modelled using a constrained box-model based upon the Master Chemical Mechanism (MCM). The agreement between modelled and measured HO2?+?RO2 was typically within ??40% and, in the unpolluted regions, within 30%. The analysis of the model results suggests that the MCM might underestimate the concentrations of some acyl peroxy radicals and other small peroxy radicals. The model underestimated the measurements of NO3 by 60?C70%, possibly because of rapid heterogeneous uptake of N2O5. The MCM model results were used to estimate the composition of the peroxy radical pool and to quantify the role of DMS, isoprene and alkenes in the formation of RO2 in the different regions. The measurements of HO2?+?RO2 and NO3 were also used to calculate the gas-phase budget of NO3 and quantify the importance of organic peroxy radicals as NO3 sinks. RO2 accounted, on average, for 12?C28% of the total gas-phase NO3 losses in the unpolluted regions and for 1?C2% of the total gas-phase NO3 losses in the polluted regions.  相似文献   

5.
The scientific community is developing new global, regional, and sectoral scenarios to facilitate interdisciplinary research and assessment to explore the range of possible future climates and related physical changes that could pose risks to human and natural systems; how these changes could interact with social, economic, and environmental development pathways; the degree to which mitigation and adaptation policies can avoid and reduce risks; the costs and benefits of various policy mixes; and the relationship of future climate change adaptation and mitigation policy responses with sustainable development. This paper provides the background to and process of developing the conceptual framework for these scenarios, as described in the three subsequent papers in this Special Issue (Van Vuuren et al., 2013; O’Neill et al., 2013; Kriegler et al., Submitted for publication in this special issue). The paper also discusses research needs to further develop, apply, and revise this framework in an iterative and open-ended process. A key goal of the framework design and its future development is to facilitate the collaboration of climate change researchers from a broad range of perspectives and disciplines to develop policy- and decision-relevant scenarios and explore the challenges and opportunities human and natural systems could face with additional climate change.  相似文献   

6.
With very few exceptions, just about all limited area models (LAMs) used in operational NWP and regional climate modeling use the Davies (Q J R Meteorol Soc 102:405–418, 1976) relaxation lateral boundary conditions (LBCs), even though they make no effort to respect the basic mathematics of the problem. While in the early stages of the primitive equation LAM development in the seventies numerous schemes have been proposed and tested, LAM communities have eventually for the most part settled on the relaxation LBCs with few questions asked. An exception is the Eta model used extensively at NCEP and several other centers, in which the Mesinger (Contrib Atmos Phys 50:200–210, 1977) LBCs are used, designed and based on knowledge available before the introduction of the relaxation scheme. They prescribe variables along the outermost row of grid points only; all of them at the inflow points and one less at the outflow points where the tangential velocity components are extrapolated from inside of the model domain. Additional schemes are in place to suppress separation of gravity-wave solutions on C-subgrids of the model’s E-grid. A recent paper of Veljovic et al. (Meteor Zeitschrift 19:237–246, 2010) included three 32-day forecasts done with both the Eta and the relaxation LBCs and the comparison of some of their verification results. Here we extend this experiment by three additional forecasts to arrive at an ensemble of six members run with both schemes, and present a more complete discussion of results. We in addition show results of one of these forecasts in which the linear change of relaxation coefficients was replaced by the change following the recommendation of Lehmann (Meteorol Atmos Phys 52:1–14, 1993). We feel that the results of our two verification schemes strongly suggest the advantage of the Eta over the conventional relaxation scheme, thereby raising doubts as to the justification for its use.  相似文献   

7.
To clarify the link between existing infrastructure legacy and the 2°C target, we extend the work of Davis et al. (Science 329:1330–1333, 2010) by introducing non-CO2 greenhouse gases and the inertia in transportation-needs drivers. We conclude that climate policies able to maintain climate change below 2°C cannot disregard existing infrastructure.  相似文献   

8.
Static flux chamber measurements of CCl4 uptake by soils in boreal, subtropical and tropical forests have been used to reassess the sink strength for this ozone depleting chemical. Happell and Roche (Geophys. Res. Lett. 30(2), 1088–1091, 2003) used flux estimates from soil concentration gradients to calculate a partial CCl4 atmospheric lifetime (τsoil) of 90 years. More recently, it is has been assumed that a better estimate of τsoil is 195 years (Montzka et al. 2011). In the work here, the rate of CCl4 uptake was calculated from 453 flux chamber measurements using an exponential fit to the chamber CCl4 concentration change with time. This analysis indicated that the flux rate estimate in Happell and Roche (Geophys. Res. Lett. 30(2) 1088–1091, 2003) was overestimated by 2.75, yielding a new estimate of τsoil for CCl4 of 245 years. Significant correlations of CCl4 uptake to temperature, soil moisture, or time of year were not observed. This work provides additional evidence that CCl4 uptake by soils is a common process and needs to be considered when developing an atmospheric budget for this compound.  相似文献   

9.
Gary Yohe 《Climatic change》2010,99(1-2):295-302
Article 2 of the United Nations Framework Convention on Climate Change commits its parties to stabilizing greenhouse gas concentrations in the atmosphere at a level that “would prevent dangerous anthropogenic interference with the climate system.” Authors of the Third Assessment Report of the Intergovernmental Panel on Climate Change (IPCC 2001a, b) offered some insight into what negotiators might consider dangerous by highlighting five “reasons for concern” (RFC’s) and tracking concern against changes in global mean temperature; they illustrated their assessments in the now iconic “burning embers” diagram. The Fourth Assessment Report reaffirmed the value of plotting RFC’s against temperature change (IPCC 2007a, b), and Smith et al. (2009) produced an unpated embers visualization for the globe. This paper applies the same assessment and communication strategies to calibrate the comparable RFC’s for the United States. It adds “National Security Concern” as a sixth RFC because many now see changes in the intensity and/or frequency of extreme events around the world as “risk enhancers” that deserve attention at the highest levels of the US policy and research communities. The US embers portrayed here suggest that: (1) US policy-makers will not discover anything really “dangerous” over the near to medium term if they consider only economic impacts that are aggregated across the entire country but that (2) they could easily uncover “dangerous anthropogenic interference with the climate system” by focusing their attention on changes in the intensities, frequencies, and regional distributions of extreme weather events driven by climate change.  相似文献   

10.
Greenhouse gases emission inventories are computed with rather low precision. Moreover, their uncertainty distributions may be asymmetric. This should be accounted for in the compliance and trading rules. In this paper we model the uncertainty of inventories as intervals or using fuzzy numbers. The latter allows us to better shape the uncertainty distributions. The compliance and emission trading rules obtained generalize the results for the symmetric uncertainty distributions that were considered in the earlier papers by the present authors (Nahorski et al., Water Air & Soil Pollution. Focus 7(4–5):539–558, 2007; Nahorski and Horabik, 2007, J Energy Eng 134(2):47–52, 2008). However, unlike in the symmetric distribution, in the asymmetric fuzzy case it is necessary to apply approximations because of nonlinearities in the formulas. The final conclusion is that the interval uncertainty rules can be applied, but with a much higher substitutional noncompliance risk, which is a parameter of the rules.  相似文献   

11.
We present further steps in our analysis of the early anthropogenic hypothesis (Ruddiman, Clim Change 61:261–293, 2003) that increased levels of greenhouse gases in the current interglacial, compared to lower levels in previous interglacials, were initiated by early agricultural activities, and that these increases caused a warming of climate long before the industrial era (~1750). These steps include updating observations of greenhouse gas and climate trends from earlier interglacials, reviewing recent estimates of greenhouse gas emissions from early agriculture, and describing a simulation by a climate model with a dynamic ocean forced by the low levels of greenhouse gases typical of previous interglacials in order to gauge the magnitude of the climate change for an inferred (natural) low greenhouse gas level relative to a high present day level. We conduct two time slice (equilibrium) simulations using present day orbital forcing and two levels of greenhouse gas forcing: the estimated low (natural) levels of previous interglacials, and the high levels of the present (control). By comparing the former to the latter, we estimate how much colder the climate would be without the combined greenhouse gas forcing of the early agriculture era (inferred from differences between this interglacial and previous interglacials) and the industrial era (the period since ~1750). With the low greenhouse gas levels, the global average surface temperature is 2.7 K lower than present day—ranging from ~2 K lower in the tropics to 4–8 K lower in polar regions. These changes are large, and larger than those reported in a pre-industrial (~1750) simulation with this model, because the imposed low greenhouse gas levels (CH4 = 450 ppb, CO2 = 240 ppm) are lower than both pre-industrial (CH4 = 760 ppb, CO2 = 280 ppm) and modern control (CH4 = 1,714 ppb, CO2 = 355 ppm) values. The area of year-round snowcover is larger, as found in our previous simulations and some other modeling studies, indicating that a state of incipient glaciation would exist given the current configuration of earth’s orbit (reduced insolation in northern hemisphere summer) and the imposed low levels of greenhouse gases. We include comparisons of these snowcover maps with known locations of earlier glacial inception and with locations of twentieth century glaciers and ice caps. In two earlier studies, we used climate models consisting of atmosphere, land surface, and a shallow mixed-layer ocean (Ruddiman et al., Quat Sci Rev 25:1–10, 2005; Vavrus et al., Quat Sci Rev 27:1410–1425, 2008). Here, we replaced the mixed-layer ocean with a complete dynamic ocean. While the simulated climate of the atmosphere and the surface with this improved model configuration is similar to our earlier results (Vavrus et al., Quat Sci Rev 27:1410–1425, 2008), the added information from the full dynamical ocean is of particular interest. The global and vertically-averaged ocean temperature is 1.25 K lower, the area of sea ice is larger, and there is less upwelling in the Southern Ocean. From these results, we infer that natural ocean feedbacks could have amplified the greenhouse gas changes initiated by early agriculture and possibly account for an additional increment of CO2 increase beyond that attributed directly to early agricultural, as proposed by Ruddiman (Rev Geophys 45:RG4001, 2007). However, a full test of the early anthropogenic hypothesis will require additional observations and simulations with models that include ocean and land carbon cycles and other refinements elaborated herein.  相似文献   

12.
Evaluation of Two Energy Balance Closure Parametrizations   总被引:1,自引:0,他引:1  
A general lack of energy balance closure indicates that tower-based eddy-covariance (EC) measurements underestimate turbulent heat fluxes, which calls for robust correction schemes. Two parametrization approaches that can be found in the literature were tested using data from the Canadian Twin Otter research aircraft and from tower-based measurements of the German Terrestrial Environmental Observatories (TERENO) programme. Our analysis shows that the approach of Huang et al. (Boundary-Layer Meteorol 127:273–292, 2008), based on large-eddy simulation, is not applicable to typical near-surface flux measurements because it was developed for heights above the surface layer and over homogeneous terrain. The biggest shortcoming of this parametrization is that the grid resolution of the model was too coarse so that the surface layer, where EC measurements are usually made, is not properly resolved. The empirical approach of Panin and Bernhofer (Izvestiya Atmos Oceanic Phys 44:701–716, 2008) considers landscape-level roughness heterogeneities that induce secondary circulations and at least gives a qualitative estimate of the energy balance closure. However, it does not consider any feature of landscape-scale heterogeneity other than surface roughness, such as surface temperature, surface moisture or topography. The failures of both approaches might indicate that the influence of mesoscale structures is not a sufficient explanation for the energy balance closure problem. However, our analysis of different wind-direction sectors shows that the upwind landscape-scale heterogeneity indeed influences the energy balance closure determined from tower flux data. We also analyzed the aircraft measurements with respect to the partitioning of the “missing energy” between sensible and latent heat fluxes and we could confirm the assumption of scalar similarity only for Bowen ratios $\approx $ 1.  相似文献   

13.
The laser flash photolysis/UV absorption spectrometry technique has been used to investigate the kinetics of the peroxy radical permutation reactions (i.e. self and cross reactions) arising from the OH-initiated oxidation of isoprene (2-methyl-1,3-butadiene), and of the simpler, but related conjugated dienes, 1,3-butadiene and 2,3-dimethyl-1,3-butadiene. The results of the two simpler systems are analysed to provide values of the rate coefficients for the 6 peroxy radical permutation reactions of the three types of isomeric peroxy radical produced in each system (T = 298 K, P = 760 Torr). The rate coefficients are all significantly larger than values estimated previously by extrapolation of structure-reactivity relationships based on the kinetics of a limited dataset of simpler radicals containing similar structural features. The results are discussed in terms of trends in self and cross reaction reactivity of primary, secondary and tertiary peroxy radicals containing combinations of allyl, -hydroxy and -hydroxy functionalities. Since the peroxy radicals formed in these systems are structurally very similar to those formed in the isoprene system, the kinetic parameters derived from the results of the simpler systems are used to assist the assignment of kinetic parameters to the 21 permutation reactions of the six types of isomeric peroxy radical generated in the isoprene system. Kinetic models describing the OH-initiated degradation of all three conjugated dienes to first generation products in the absence of NOx are recommended, which are also consistent with available end product studies. The model for isoprene is considered to be a further improvement on that suggested previously for its OH-initiated oxidation in the absence of NOx. The mechanism is further extended to include chemistry applicable to NOx-present conditions, and calculated product yields are compared with those reported in the literature.  相似文献   

14.
A new approach is proposed to predict concentration fluctuations in the framework of one-particle Lagrangian stochastic models. The approach is innovative since it allows the computation of concentration fluctuations in dispersing plumes using a Lagrangian one-particle model with micromixing but with no need for the simulating of background particles. The extension of the model for the treatment of chemically reactive plumes is also accomplished and allows the computation of plume-related chemical reactions in a Lagrangian one-particle framework separately from the background chemical reactions, accounting for the effect of concentration fluctuations on chemical reactions in a general, albeit approximate, manner. These characteristics should make the proposed approach an ideal tool for plume-in-grid calculations in chemistry transport models. The results are compared to the wind-tunnel experiments of Fackrell and Robins (J Fluid Mech, 117:1–26, 1982) for plume dispersion in a neutral boundary layer and to the measurements of Legg et al. (Boundary-Layer Meteorol, 35:277–302, 1986) for line source dispersion in and above a model canopy. Preliminary reacting plume simulations are also shown comparing the model with the experimental results of Brown and Bilger (J Fluid Mech, 312:373–407, 1996; Atmos Environ, 32:611–628, 1998) to demonstrate the feasibility of computing chemical reactions in the proposed framework.  相似文献   

15.
Heat flux density at the soil surface (G 0) was evaluated hourly on a vegetal cover 0.08 m high, with a leaf area index of 1.07 m2 m?2, during daylight hours, using Choudhury et al. (Agric For Meteorol 39:283–297, 1987) ( $ G_0^{\text{rn}} $ ), Santanello and Friedl (J Appl Meteorol 42:851–862, 2003) ( $ G_0^{\text{s}} $ ), and force-restore ( $ G_0^{\text{fr}} $ ) models and the plate calorimetry methodology ( $ G_0^{\text{pco}} $ ), where the gradient calorimetry methodology (G 0R ) served as a reference for determining G 0. It was found that the peak of G 0R was at 1 p.m., with values that ranged between 60 and 100 W m?2 and that the G 0/Rn relation varied during the day with values close to zero in the early hours of the morning and close to 0.25 in the last hours of daylight. The $ G_0^{\text{s}} $ model presented the best performance, followed by the $ G_0^{\text{rn}} $ and $ G_0^{\text{fr}} $ models. The plate calorimetry methodology showed a similar behavior to that of the gradient calorimetry referential methodology.  相似文献   

16.
Simultaneous measurements of ozone and ozoneprecursors were made during a field campaign atSchauinsland in the Black Forest and in the valleynorth of Schauinsland that channels the flow ofpolluted air from the city of Freiburg to the site.From the decay of hydrocarbons and NOx between the twomeasuring sites and the known rate coefficients, theconcentration of OH radicals was calculated. From abudget analysis of OH and HOx it is concluded that therelatively high OH concentrations (5–8 ×106cm-3) in the presence of high NO2concentrations cannot be explained by the knownprimary sources. The budget can be closed if efficientrecycling of OH via HO2 is assumed to occur andthat, based on the measured hydrocarbons, 2 HO2molecules are formed for each OH radical that reactswith a hydrocarbon molecule. This assumption is inaccordance with the budget of Ox obtained from ourmeasurements and with results from earliermeasurements of alkylnitrates and peroxy radicals atSchauinsland. A possible conclusion is that the decayof precursors and production of photooxidants in urbanplumes proceeds at a faster rate than is currentlyassumed. The potential role of biogenichydrocarbons for the radical budget is alsodiscussed.  相似文献   

17.
The unit root testing within a breaking trend framework for global and hemispheric temperatures of Gay-Garcia, Estrada and Sánchez Clim Chang 94:333–349, 2009 is extended in two directions: first, the extended HadCRUT3 temperature series from Brohan et al. J Geophys Res 111:D12106, 2006 are used and, second, new breaking trend estimators and unit root tests are employed, along with direct modelling of breaking trend and unit root processes for the series. Some differences to the results of Gay-Garcia et al. are found: break dates are shifted to 1976 for global and northern hemisphere temperatures and to 1964 for the southern hemisphere. Although the results are somewhat ambiguous, global and northern hemisphere temperatures are probably best modelled by unit root processes with a break in drift, while southern hemisphere temperatures follow a breaking trend process with stationary fluctuations about this trend. Irrespective of the models selected, there is little evidence of trend warming before the breaks, i.e., until the third quarter of the 20th century, and after the breaks northern hemisphere and global trend temperatures warm quicker than in the southern hemisphere, the range being between 0.01 and 0.02 °C per annum.  相似文献   

18.
Chris Hope 《Climatic change》2013,117(3):531-543
PAGE09 is an updated version of the PAGE2002 integrated assessment model (Hope 2011a). The default PAGE09 model gives a mean estimate of the social cost of CO2 (SCCO2) of $106 per tonne of CO2, compared to $81 from the PAGE2002 model used in the Stern review (Stern 2007). The increase is the net result of several improvements that have been incorporated into the PAGE09 model in response to the critical debate around the Stern review: the adoption of the A1B socio-economic scenario, rather than A2 whose population assumptions are now thought to be implausible; the use of ranges for the two components of the discount rate, rather than the single values used in the Stern review; a distribution for the climate sensitivity that is consistent with the latest estimates from IPCC 2007a; less adaptation than in PAGE2002, particularly in the economic sector, which was criticised for possibly being over-optimistic; and a more theoretically-justified basis of valuation that gives results appropriate to a representative agent from the focus region, the EU. The effect of each of these adjustments is quantified and explained.  相似文献   

19.
The surface air temperature increase in the southwestern United States was much larger during the last few decades than the increase in the global mean. While the global temperature increased by about 0.5 °C from 1975 to 2000, the southwestern US temperature increased by about 2 °C. If such an enhanced warming persisted for the next few decades, the southwestern US would suffer devastating consequences. To identify major drivers of southwestern climate change we perform a multiple-linear regression of the past 100 years of the southwestern US temperature and precipitation. We find that in the early twentieth century the warming was dominated by a positive phase of the Atlantic multi-decadal oscillation (AMO) with minor contributions from increasing solar irradiance and concentration of greenhouse gases. The late twentieth century warming was about equally influenced by increasing concentration of atmospheric greenhouse gases (GHGs) and a positive phase of the AMO. The current southwestern US drought is associated with a near maximum AMO index occurring nearly simultaneously with a minimum in the Pacific decadal oscillation (PDO) index. A similar situation occurred in mid-1950s when precipitation reached its minimum within the instrumental records. If future atmospheric concentrations of GHGs increase according to the IPCC scenarios (Solomon et al. in Climate change 2007: working group I. The Physical Science Basis, Cambridge, 996 pp, 2007), climate models project a fast rate of southwestern warming accompanied by devastating droughts (Seager et al. in Science 316:1181–1184, 2007; Williams et al. in Nat Clim Chang, 2012). However, the current climate models have not been able to predict the behavior of the AMO and PDO indices. The regression model does support the climate models (CMIP3 and CMIP5 AOGCMs) projections of a much warmer and drier southwestern US only if the AMO changes its 1,000 years cyclic behavior and instead continues to rise close to its 1975–2000 rate. If the AMO continues its quasi-cyclic behavior the US SW temperature should remain stable and the precipitation should significantly increase during the next few decades.  相似文献   

20.
Simultaneous measurements of peroxy and nitrate radicals at Schauinsland   总被引:3,自引:0,他引:3  
We present simultaneous field measurements of NO3 and peroxy radicals made at night in a forested area (Schauinsland, Black Forest, 48° N, 8° N, 1150 ASL), together with measurements of CO, O3, NO x , NO y , and hydrocarbons, as well as meteorological parameters. NO2, NO3, HO2, and (RO2) radicals are detected with matrix isolation/electron spin resonance (MIESR). NO3 and HO2 were found to be present in the range of 0–10 ppt, whilst organic peroxy radicals reached concentrations of 40 ppt. NO3, RO2, and HO2 exhibited strong variations, in contrast to the almost constant values of the longer lived trace gases. The data suggest anticorrelation between NO3 and RO2 radical concentrations at night.The measured trace gas set allows the calculation of NO3 and peroxy radical concentrations, using a chemical box model. From these simulations, it is concluded that the observed anthropogenic hydrocarbons are not sufficient to explain the observed RO2 concentrations. The chemical budget of both NO3 and RO2 radicals can be understood if emissions of monoterpenes are included. The measured HO2 can only be explained by the model, when NO concentrations at night of around 5 ppt are assumed to be present. The presence of HO2 radicals implies the presence of hydroxyl radicals at night in concentrations of up to 105 cm–3.  相似文献   

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