In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 campaign in ...connection with a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For example, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere, but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
A compact widely-tunable fiber-coupled sensor for trace gas detection of hydrogen sulfide (H₂S) in the mid infrared is reported. The sensor is based on an external-cavity quantum cascade laser ...(EC-QCL) tunable between 7.6 and 8.3 μm wavelengths coupled into a single-mode hollow-core waveguide. Quartz-enhanced photoacoustic spectroscopy has been selected as detecting technique. The fiber coupling system converts the astigmatic beam exiting the laser into a TEM(00) mode. During a full laser scan, we observed no misalignment between the optical beam and the tuning fork, thus making our system applicable for multi-gas or broad absorber detections. The sensor has been tested on N₂:H₂S gas mixtures. The minimum detectable H₂S concentration is 450 ppb in ~3 s integration time, which is the best value till now reported in literature for H₂S optical sensors.
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•Ammonia was measured as a target gas in an artificial stack.•Optical detection techniques exhibit different resilience to absorption lineshapes.•Target gas absorption widths are ...sensitive to the concentrations of water and CO2.•Direct absorption and derivative detection were compared with respect to calibration.•An optical multipass cell was used, completely inside an artificial stack at 140 °C.
The quantitative detection of pollutants in industrial emissions, in particular the emissions of biomass burners, requires different types of analyzers. Optical devices are usually sensitive to the transparency and dirtiness of the exhaust gases, so optical measurements are normally carried out by extracting the samples from the stacks. This paper has a twofold aim. First, we will prove that the molecular composition of the exhaust mixture (in particular the concentration of water and carbon dioxide) can deeply affect the outcome of optical analyzers, depending on the adopted detection technique. This is a critical issue, in particular with a view to the necessity of providing suitable reference methods for monitoring biomass burners emissions. Second, we will show how it is possible to measure inside an artificial stack by using an optical multipass cell located across the gas flow, even at 140 °C, or in presence of soot.
Variations in the mixing ratio of trace gases of tropospheric origin entering the stratosphere in the tropics are of interest for assessing both troposphere to stratosphere transport fluxes in the ...tropics and the impact of these transport fluxes on the composition of the tropical lower stratosphere. Anomaly patterns of carbon monoxide (CO) and long-lived tracers in the lower tropical stratosphere allow conclusions about the rate and the variability of tropical upwelling to be drawn. Here, we present a simplified chemistry scheme for the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the simulation, at comparatively low numerical cost, of CO, ozone, and long-lived trace substances (CH4, N2O, CCl3F (CFC-11), CCl2F2 (CFC-12), and CO2) in the lower tropical stratosphere. For the long-lived trace substances, the boundary conditions at the surface are prescribed based on ground-based measurements in the lowest model level. The boundary condition for CO in the lower troposphere (below about 4 km) is deduced from MOPITT measurements. Due to the lack of a specific representation of mixing and convective uplift in the troposphere in this model version, enhanced CO values, in particular those resulting from convective outflow are underestimated. However, in the tropical tropopause layer and the lower tropical stratosphere, there is relatively good agreement of simulated CO with in situ measurements (with the exception of the TROCCINOX campaign, where CO in the simulation is biased low 10–15 ppbv). Further, the model results (and therefore also the ERA-Interim winds, on which the transport in the model is based) are of sufficient quality to describe large scale anomaly patterns of CO in the lower stratosphere. In particular, the zonally averaged tropical CO anomaly patterns (the so called "tape recorder" patterns) simulated by this model version of CLaMS are in good agreement with observations, although the simulations show a too rapid upwelling compared to observations as a consequence of the overestimated vertical velocities in the ERA-Interim reanalysis data set. Moreover, the simulated tropical anomaly patterns of N2O are in good agreement with observations. In the simulations, anomaly patterns of CH4 and CFC-11 were found to be very similar to those of N2O; for all long-lived tracers, positive anomalies are simulated because of the enhanced tropical upwelling in the easterly shear phase of the quasi-biennial oscillation.
This paper describes the results of a series of experiments conducted with the PALS laser at intensities of interest for the shock ignition approach to inertial fusion. In particular, we addressed ...the generation of hot electrons (HE) (determining their average energy and number), as well as the parametric instabilities which are producing them. In addition, we studied the impact of HE on the formation and dynamics of strong shocks.
Laser–plasma interaction (LPI) at intensities
$10^{15}{-}10^{16}~\text{W}\cdot \text{cm}^{-2}$
is dominated by parametric instabilities which can be responsible for a significant amount of ...non-collisional absorption and generate large fluxes of high-energy nonthermal electrons. Such a regime is of paramount importance for inertial confinement fusion (ICF) and in particular for the shock ignition scheme. In this paper we report on an experiment carried out at the Prague Asterix Laser System (PALS) facility to investigate the extent and time history of stimulated Raman scattering (SRS) and two-plasmon decay (TPD) instabilities, driven by the interaction of an infrared laser pulse at an intensity
${\sim}1.2\times 10^{16}~\text{W}\cdot \text{cm}^{-2}$
with a
${\sim}100~\unicodeSTIX{x03BC}\text{m}$
scalelength plasma produced from irradiation of a flat plastic target. The laser pulse duration (300 ps) and the high value of plasma temperature (
${\sim}4~\text{keV}$
) expected from hydrodynamic simulations make these results interesting for a deeper understanding of LPI in shock ignition conditions. Experimental results show that absolute TPD/SRS, driven at a quarter of the critical density, and convective SRS, driven at lower plasma densities, are well separated in time, with absolute instabilities driven at early times of interaction and convective backward SRS emerging at the laser peak and persisting all over the tail of the pulse. Side-scattering SRS, driven at low plasma densities, is also clearly observed. Experimental results are compared to fully kinetic large-scale, two-dimensional simulations. Particle-in-cell results, beyond reproducing the framework delineated by the experimental measurements, reveal the importance of filamentation instability in ruling the onset of SRS and stimulated Brillouin scattering instabilities and confirm the crucial role of collisionless absorption in the LPI energy balance.
Processes occurring in the tropical upper troposphere (UT), the Tropical Transition Layer (TTL), and the lower stratosphere (LS) are of importance for the global climate, for stratospheric dynamics ...and air chemistry, and for their influence on the global distribution of water vapour, trace gases and aerosols. In this contribution we present aerosol and trace gas (in-situ) measurements from the tropical UT/LS over Southern Brazil, Northern Australia, and West Africa. The instruments were operated on board of the Russian high altitude research aircraft M-55 "Geophysica" and the DLR Falcon-20 during the campaigns TROCCINOX (Araçatuba, Brazil, February 2005), SCOUT-O3 (Darwin, Australia, December 2005), and SCOUT-AMMA (Ouagadougou, Burkina Faso, August 2006). The data cover submicron particle number densities and volatility from the COndensation PArticle counting System (COPAS), as well as relevant trace gases like N2O, ozone, and CO. We use these trace gas measurements to place the aerosol data into a broader atmospheric context. Also a juxtaposition of the submicron particle data with previous measurements over Costa Rica and other tropical locations between 1999 and 2007 (NASA DC-8 and NASA WB-57F) is provided. The submicron particle number densities, as a function of altitude, were found to be remarkably constant in the tropical UT/LS altitude band for the two decades after 1987. Thus, a parameterisation suitable for models can be extracted from these measurements. Compared to the average levels in the period between 1987 and 2007 a slight increase of particle abundances was found for 2005/2006 at altitudes with potential temperatures, Θ, above 430 K. The origins of this increase are unknown except for increases measured during SCOUT-AMMA. Here the eruption of the Soufrière Hills volcano in the Caribbean caused elevated particle mixing ratios. The vertical profiles from Northern hemispheric mid-latitudes between 1999 and 2006 also are compact enough to derive a parameterisation. The tropical profiles all show a broad maximum of particle mixing ratios (between Θ≈340 K and 390 K) which extends from below the TTL to above the thermal tropopause. Thus these particles are a "reservoir" for vertical transport into the stratosphere. The ratio of non-volatile particle number density to total particle number density was also measured by COPAS. The vertical profiles of this ratio have a maximum of 50% above 370 K over Australia and West Africa and a pronounced minimum directly below. Without detailed chemical composition measurements a reason for the increase of non-volatile particle fractions cannot yet be given. However, half of the particles from the tropical "reservoir" contain compounds other than sulphuric acid and water. Correlations of the measured aerosol mixing ratios with N2O and ozone exhibit compact relationships for the tropical data from SCOUT-AMMA, TROCCINOX, and SCOUT-O3. Correlations with CO are more scattered probably because of the connection to different pollution source regions. We provide additional data from the long distance transfer flights to the campaign sites in Brazil, Australia, and West-Africa. These were executed during a time window of 17 months within a period of relative volcanic quiescence. Thus the data represent a "snapshot picture" documenting the status of a significant part of the global UT/LS fine aerosol at low concentration levels 15 years after the last major (i.e., the 1991 Mount Pinatubo) eruption. The corresponding latitudinal distributions of the measured particle number densities are presented in this paper to provide data of the UT/LS background aerosol for modelling purposes.
In situ measurements of ice crystal size distributions in tropical upper troposphere/lower stratosphere (UT/LS) clouds were performed during the SCOUT-AMMA campaign over West Africa in August 2006. ...The cloud properties were measured with a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP) operated aboard the Russian high altitude research aircraft M-55 Geophysica with the mission base in Ouagadougou, Burkina Faso. A total of 117 ice particle size distributions were obtained from the measurements in the vicinity of Mesoscale Convective Systems (MCS). Two to four modal lognormal size distributions were fitted to the average size distributions for different potential temperature bins. The measurements showed proportionately more large ice particles compared to former measurements above maritime regions. With the help of trace gas measurements of NO, NOy, CO2, CO, and O3 and satellite images, clouds in young and aged MCS outflow were identified. These events were observed at altitudes of 11.0 km to 14.2 km corresponding to potential temperature levels of 346 K to 356 K. In a young outflow from a developing MCS ice crystal number concentrations of up to (8.3 ± 1.6) cm−3 and rimed ice particles with maximum dimensions exceeding 1.5 mm were found. A maximum ice water content of 0.05 g m−3 was observed and an effective radius of about 90 μm. In contrast the aged outflow events were more diluted and showed a maximum number concentration of 0.03 cm−3, an ice water content of 2.3 × 10−4 g m−3, an effective radius of about 18 μm, while the largest particles had a maximum dimension of 61 μm. Close to the tropopause subvisual cirrus were encountered four times at altitudes of 15 km to 16.4 km. The mean ice particle number concentration of these encounters was 0.01 cm−3 with maximum particle sizes of 130 μm, and the mean ice water content was about 1.4 × 10−4 g m−3. All known in situ measurements of subvisual tropopause cirrus are compared and an exponential fit on the size distributions is established for modelling purposes. A comparison of aerosol to ice crystal number concentrations, in order to obtain an estimate on how many ice particles may result from activation of the present aerosol, yielded low ratios for the subvisual cirrus cases of roughly one cloud particle per 30 000 aerosol particles, while for the MCS outflow cases this resulted in a high ratio of one cloud particle per 300 aerosol particles.
During the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board the high-altitude research aircraft Geophysica (ozone, water vapor, ...NO, NOy, CH4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the entire TTL region roughly extending between 350 and 420 K. Here, analysis of transport across the TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by meteorological analysis winds and heating/cooling rates derived from a radiation calculation. Below the tropopause, the model smoothly transforms from the isentropic to the hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the vertical wind of the meteorological analysis. As in previous CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates. Stratospheric and tropospheric signatures in the TTL can be seen both in the observations and in the model. The composition of air above ≈350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the tropical flanks of the subtropical jets and, to some extent, in the the outflow regions of the large-scale convection, offers an explanation for the upward transport of trace species from the main convective outflow at around 350 K up to the tropical tropopause around 380 K.
We present airborne in situ measurements made during the AMMA (African Monsoon Multidisciplinary Analysis)/SCOUT-O3 campaign between 31 July and 17 August 2006 on board the M55 Geophysica aircraft, ...based in Ouagadougou, Burkina Faso. CO2 and N2O were measured with the High Altitude Gas Analyzer (HAGAR), CO was measured with the Cryogenically Operated Laser Diode (COLD) instrument, and O3 with the Fast Ozone ANalyzer (FOZAN). We analyse the data obtained during five local flights to study the dominant transport processes controlling the tropical tropopause layer (TTL, here ~350–375 K) and lower stratosphere above West-Africa: deep convection up to the level of main convective outflow, overshooting of deep convection, and horizontal inmixing across the subtropical tropopause. Besides, we examine the morphology of the stratospheric subtropical barrier. Except for the flight of 13 August, distinct minima in CO2 mixing ratios indicate convective outflow of boundary layer air in the TTL. The CO2 profiles show that the level of main convective outflow was mostly located at potential temperatures between 350 and 360 K, and for 11 August reached up to 370 K. While the CO2 minima indicate quite significant convective influence, the O3 profiles suggest that the observed convective signatures were mostly not fresh, but of older origin (several days or more). When compared with the mean O3 profile measured during a previous campaign over Darwin in November 2005, the O3 minimum at the main convective outflow level was less pronounced over Ouagadougou. Furthermore O3 mixing ratios were much higher throughout the whole TTL and, unlike over Darwin, rarely showed low values observed in the regional boundary layer. Signatures of irreversible mixing following overshooting of convective air were scarce in the tracer data. Some small signatures indicative of this process were found in CO2 profiles between 390 and 410 K during the flights of 4 and 8 August, and in CO data at 410 K on 7 August. However, the absence of expected corresponding signatures in other tracer data makes this evidence inconclusive, and overall there is little indication from the observations that overshooting convection has a profound impact on gas-phase tracer TTL composition during AMMA. We find the amount of photochemically aged air isentropically mixed into the TTL across the subtropical tropopause to be not significant. Using the N2O observations we estimate the fraction of aged extratropical stratospheric air in the TTL to be 0.0±0.1 up to 370 K during the local flights. Above the TTL this fraction increases to 0.3±0.1 at 390 K. The subtropical barrier, as indicated by the slope of the correlation between N2O and O3 between 415 and 490 K, does not appear as a sharp border between the tropics and extratropics, but rather as a gradual transition region between 10° N and 25° N where isentropic mixing between these two regions may occur.
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