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Mesoscale circulations over complex terrain in the Valencia coastal region, Spain – Part 1: Simulation of diurnal circulation regimes

We collected ground-based and aircraft vertical profile measurements of meteorological parameters during a 2-week intensive campaign over the Valencia basin, in order to understand how mesoscale circulations develop over complex terrain and affect the atmospheric transport of tracers. A high-resolution version of the RAMS model was run to simulate the campaign and characterize the diurnal patterns of the flow regime: night-time katabatic drainage, morning sea-breeze development and its subsequent coupling with mountain up-slopes, and evening flow-veering under larger-scale interactions. An application of this mesoscale model to the transport of CO2 is given in a companion paper. A careful evaluation of the model performances against diverse meteorological observations is carried out. Despite the complexity of the processes interacting with each other, and the uncertainties on modeled soil moisture boundary conditions and turbulence parameterizations, we show that it is possible to simulate faithfully the contrasted flow regimes during the course of one day, especially the inland progression and organization of the sea breeze. This gives confidence with respect to future applicability of mesoscale models to establish a reliable link between surface sources of tracers and their atmospheric concentration signals over complex terrain.
Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä

This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3–6) or formation rates at 1 nm and 3 nm (J1 and J3); 2) the time delays between [H2SO4] and N3–6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3–6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The nucleation coefficients were about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3–6 and [H2SO4]. The exponents in the J3∝[H2SO4 ]nJ3-connection were consistently higher than or equal to the exponents in the relation N3–6∝[H2SO4 ]nN36. In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for.
Precision validation of MIPAS-Envisat products

This paper discusses the variation and validation of the precision, or estimated random error, associated with the ESA Level 2 products from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). This quantity represents the propagation of the radiometric noise from the spectra through the retrieval process into the Level 2 profile values. The noise itself varies with time, steadily rising between ice decontamination events, but the Level 2 precision has a greater variation due to the atmospheric temperature which controls the total radiance received. Hence, for all species, the precision varies latitudinally/seasonally with temperature, with a small superimposed temporal structure determined by the degree of ice contamination on the detectors. The precision validation involves comparing two MIPAS retrievals at the intersections of ascending/descending orbits. For 5 days per month of full resolution MIPAS operation, the standard deviation of the matching profile pairs is computed and compared with the precision given in the MIPAS Level 2 data, except for NO2 since it has a large diurnal variation between ascending/descending intersections. Even taking into account the propagation of the pressure-temperature retrieval errors into the VMR retrieval, the standard deviation of the matching pairs is usually a factor 1–2 larger than the precision. This is thought to be due to effects such as horizontal inhomogeneity of the atmosphere and instability of the retrieval.
A single parameter representation of hygroscopic growth and cloud condensation nucleus activity

We present a method to describe the relationship between particle dry diameter and cloud condensation nuclei (CCN) activity using a single hygroscopicity parameter κ. Values of the hygroscopicity parameter are between 0.5 and 1.4 for highly-CCN-active salts such as sodium chloride, between 0.01 and 0.5 for slightly to very hygroscopic organic species, and 0 for nonhygroscopic components. Observations indicate that atmospheric particulate matter is typically characterized by 0.1<κ<0.9. If compositional data are available and if the hygroscopicity parameter of each component is known, a multicomponent hygroscopicity parameter can be computed by weighting component hygroscopicity parameters by their volume fractions in the mixture. In the absence of information on chemical composition, experimental data for complex, multicomponent particles can be fitted to obtain the hygroscopicity parameter. The hygroscopicity parameter can thus also be used to conveniently model the CCN activity of atmospheric particles, including those containing insoluble components. We confirm the applicability of the hygroscopicity parameter and its mixing rule by applying it to published hygroscopic diameter growth factor and CCN-activation data for single- and multi-component particles containing varying amounts of inorganic, organic and surface active compounds. We suggest that κ may be fit to CCN data assuming σs/a=0.072 J m−2 and present a table of κ derived for this value and T=298.15 K. The predicted hygroscopicities for mixtures that contain the surfactant fulvic acid agree within uncertainties with the measured values. It thus appears that this approach is adequate for predicting CCN activity of mixed particles containing surface active materials, but the generality of this assumption requires further verification.
Observations of total peroxy nitrates and aldehydes: measurement interpretation and inference of OH radical concentrations

We describe measurements of total peroxy nitrates (ΣPNs), NO2, O3 and several aldehydes at Granite Bay, California, during the Chemistry and Transport of the Sacramento Urban Plume-2001 (CATSUP 2001) campaign, from 19 July–16 September 2001. We observed a strong photochemically driven variation of ΣPNs during the day with the median of 1.2 ppb at noon. Acetaldehyde, pentanal, hexanal and methacrolein had median abundances in the daytime of 1.2 ppb, 0.093 ppb, 0.14 ppb, and 0.27 ppb, respectively. We compare steady state and time dependent calculations of the dependence of ΣPNs on aldehydes, OH, NO and NO2 showing that the steady state calculations are accurate to ±30% between 10:00 and 18:00 h. We use the steady state calculation to investigate the composition of ΣPNs and the concentration of OH at Granite Bay. We find that PN molecules that have never been observed before make up an unreasonably large fraction of the ΣPNs unless we assume that there exists a PAN source that is much larger than the acetaldehyde source. We calculate that OH at the site varied between 2 and 7×106 molecule cm−3 at noon during the 8 weeks of the experiment.
Atmospheric effects and societal consequences of regional scale nuclear conflicts and acts of individual nuclear terrorism

We assess the potential damage and smoke production associated with the detonation of small nuclear weapons in modern megacities. While the number of nuclear warheads in the world has fallen by about a factor of three since its peak in 1986, the number of nuclear weapons states is increasing and the potential exists for numerous regional nuclear arms races. Eight countries are known to have nuclear weapons, 2 are constructing them, and an additional 32 nations already have the fissile material needed to build substantial arsenals of low-yield (Hiroshima-sized) explosives. Population and economic activity worldwide are congregated to an increasing extent in megacities, which might be targeted in a nuclear conflict. We find that low yield weapons, which new nuclear powers are likely to construct, can produce 100 times as many fatalities and 100 times as much smoke from fires per kt yield as previously estimated in analyses for full scale nuclear wars using high-yield weapons, if the small weapons are targeted at city centers. A single "small" nuclear detonation in an urban center could lead to more fatalities, in some cases by orders of magnitude, than have occurred in the major historical conflicts of many countries. We analyze the likely outcome of a regional nuclear exchange involving 100 15-kt explosions (less than 0.1% of the explosive yield of the current global nuclear arsenal). We find that such an exchange could produce direct fatalities comparable to all of those worldwide in World War II, or to those once estimated for a "counterforce" nuclear war between the superpowers. Megacities exposed to atmospheric fallout of long-lived radionuclides would likely be abandoned indefinitely, with severe national and international implications. Our analysis shows that smoke from urban firestorms in a regional war would rise into the upper troposphere due to pyro-convection. Robock et al. (2007) show that the smoke would subsequently rise deep into the stratosphere due to atmospheric heating, and then might induce significant climatic anomalies on global scales. We also anticipate substantial perturbations of global ozone. While there are many uncertainties in the predictions we make here, the principal unknowns are the type and scale of conflict that might occur. The scope and severity of the hazards identified pose a significant threat to the global community. They deserve careful analysis by governments worldwide advised by a broad section of the world scientific community, as well as widespread public debate.
Climatic consequences of regional nuclear conflicts

We use a modern climate model and new estimates of smoke generated by fires in contemporary cities to calculate the response of the climate system to a regional nuclear war between emerging third world nuclear powers using 100 Hiroshima-size bombs (less than 0.03% of the explosive yield of the current global nuclear arsenal) on cities in the subtropics. We find significant cooling and reductions of precipitation lasting years, which would impact the global food supply. The climate changes are large and long-lasting because the fuel loadings in modern cities are quite high and the subtropical solar insolation heats the resulting smoke cloud and lofts it into the high stratosphere, where removal mechanisms are slow. While the climate changes are less dramatic than found in previous "nuclear winter" simulations of a massive nuclear exchange between the superpowers, because less smoke is emitted, the changes are more long-lasting because the older models did not adequately represent the stratospheric plume rise.
ENSO surface longwave radiation forcing over the tropical Pacific

We have studied the spatial and temporal variation of the surface longwave radiation (downwelling and net) over a 21-year period in the tropical and subtropical Pacific Ocean (40 S–40 N, 90 E–75 W). The fluxes were computed using a deterministic model for atmospheric radiation transfer, along with satellite data from the ISCCP-D2 database and reanalysis data from NCEP/NCAR (acronyms explained in main text), for the key atmospheric and surface input parameters. An excellent correlation was found between the downwelling longwave radiation (DLR) anomaly and the Niño-3.4 index time-series, over the Niño-3.4 region located in the central Pacific. A high anti-correlation was also found over the western Pacific (15–0 S, 105–130 E). There is convincing evidence that the time series of the mean downwelling longwave radiation anomaly in the western Pacific precedes that in the Niño-3.4 region by 3–4 months. Thus, the downwelling longwave radiation anomaly is a complementary index to the SST anomaly for the study of ENSO events and can be used to asses whether or not El Niño or La Niña conditions prevail. Over the Niño-3.4 region, the mean DLR anomaly values range from +20 Wm−2 during El Niño episodes to −20 Wm−2 during La Niña events, while over the western Pacific (15–0 S, 105–130 E) these values range from −15 Wm−2 to +10 Wm−2, respectively. The long- term average (1984–2004) distribution of the net downwelling longwave radiation at the surface over the tropical and subtropical Pacific for the three month period November-December-January shows a net thermal cooling of the ocean surface. When El Niño conditions prevail, the thermal radiative cooling in the central and south-eastern tropical Pacific becomes weaker by 10 Wm−2 south of the equator in the central Pacific (7–0 S, 160–120 W) for the three-month period of NDJ, because the DLR increase is larger than the increase in surface thermal emission. In contrast, the thermal radiative cooling over Indonesia is enhanced by 10 Wm−2 during the early (August–September–October) El Niño phase.
Model sensitivity studies regarding the role of the retention coefficient for the scavenging and redistribution of highly soluble trace gases by deep convective cloud systems

The role of the retention coefficient (i.e. the fraction of a dissolved trace gas which is retained in hydrometeors during freezing) for the scavenging and redistribution of highly soluble trace gases by deep convective cloud systems is investigated using a modified version of the Weather Research and Forecasting (WRF) model. Results from cloud system resolving model runs (in which deep convection is initiated by small random perturbations in association with so-called "large scale forcings (LSF)") for a tropical oceanic (TOGA COARE) and a mid-latitude continental case (ARM) are compared to two runs in which bubbles are used to initiate deep convection (STERAO, ARM). In the LSF runs, scavenging is found to almost entirely prevent a highly soluble tracer initially located in the lowest 1.5 km of the troposphere from reaching the upper troposphere, independent of the retention coefficient. The release of gases from freezing hydrometeors leads to mixing ratio increases in the upper troposphere comparable to those calculated for insoluble trace gases only in the two runs in which bubbles are used to initiate deep convection. A comparison of the two ARM runs indicates that using bubbles to initiate deep convection may result in an overestimate of the influence of the retention coefficient on the vertical transport of highly soluble tracers. It is, however, found that the retention coefficient plays an important role for the scavenging and redistribution of highly soluble trace gases with a (chemical) source in the free troposphere and also for trace gases for which even relatively inefficient transport may be important. The large difference between LSF and bubble runs is attributed to differences in dynamics and microphysics in the inflow regions of the storms. The dependence of the results on the model setup indicates the need for additional model studies with a more realistic initiation of deep convection, e.g., considering effects of orography in a nested model setup.
Definition of "banner clouds" based on time lapse movies

Banner clouds appear on the leeward side of a mountain and resemble a banner or a flag. This article provides a comprehensive definition of "banner clouds". It is based primarily on an extensive collection of time lapse movies, but previous attempts at an explanation of this phenomenon are also taken into account. The following ingredients are considered essential: the cloud must be attached to the mountain but not appear on the windward side; the cloud must originate from condensation of water vapour contained in the air (rather than consist of blowing snow); the cloud must be persistent; and the cloud must not be of convective nature. The definition is illustrated and discussed with the help of still images and time lapse movies taken at Mount Zugspitze in the Bavarian Alps.