Ground-based water vapour soundings by microwave radiometry and Raman lidar on Jungfraujoch (Swiss Alps)

International audienceWater vapour has been measured from the International Scientific Station Jungfraujoch (ISSJ, 47° N, 7° E, 3580m above sea level) during the winters of 1999/2000 and 2000/2001 by microwave radiometry and Raman lidar. The abundance of atmospheric water vapour between the planetary boundary layer and the upper stratosphere varies over more than three orders of magnitude. The currently used measurement techniques are only suited to determine the abundance of water vapour in different atmospheric regimes. None can resolve the vertical distribution profile from ground level to the top of the stratosphere by itself. We present such a water vapour profile where simultaneous measurements from a Raman lidar and a microwave radiometer were combined to cover both the troposphere and the stratosphere, respectively. We also present a study of the stratospheric and tropospheric water vapour variability for the two consecutive winters

Direct measurement of the total reaction rate of OH in the atmosphere

A new method to investigate atmospheric chemical kinetics is presented. It is based on the pump and probe principle. Preliminary measurements are described on the decay rate of OH in the planetary boundary layer after its concentration has been raised by laser flash photolysis of background ozone and subsequent reaction of the O(1D) with atmospheric water vapor. The measured OH disappearance kinetics are compared with model calculations yielding information on the fast reaction of OH. The presented point measurements can be extended to a range resolved differential absorption LIDAR technique

Simultaneous measurement of atmospheric temperature, humidity, and aerosol extinction and backscatter coefficients by a combined vibrational-pure-rotational Raman lidar

Implementation of the pure-rotational Raman (PRR) lidar method for simultaneous measurement of atmospheric temperature, humidity, and aerosol extinction and backscatter coefficients is reported. The isolation of two wavelength domains of the PRR spectrum and the suppression of the elastically scattered light is carried out by a double-grating polychromator. Experiments involving elastic backscatter from dense clouds and a solid target confirm the high level of suppression of the elastic light in the corresponding acquisition channels of the two selected PRR domains. Calibration of the temperature channel was done both by comparison with an experimentally verified atmospheric temperature model profile and by inter-comparison with radiosondes. Night-time temperature profiles with high vertical resolution were obtained up to the lower stratosphere. The PRR temperature profile combined with the water vapor mixing ratio obtained from the ro-vibrational Raman channel is used to estimate the relative humidit

Total VOC reactivity in the planetary boundary layer: 2. A new indicator for determining the sensitivity of the ozone production to VOC and NO

A new indicator is proposed for determining if tropospheric ozone production in a specifiacr eai s limitedb yV OC or NOx.T he indicato1r 9= r•ø•C/•oød•Xes cribeths e ratio of the lifetimes of OH against the losses by reacting with VOC and NOx. Whereas •oøx• c anb e obtainebdy c onventionmale asurementthse, n ewp umpa ndp robeO H approach which is described in part one of this publication makes it now possible to obtain also ß_ov •o c ßI ndicator values above a thresholdv alue of 0.2 __+50 % are representativeo f NOx-saturatedc onditionsw here an increaseo f NOx emissionsc auses lower ozone production.F or valuesb elow 0.01 the ozone productioni s very insensitivet o changeso f VOC emissionsT. he robustnesso f this indicator againsts everalp arameters sucha s temperature,h umidity,p hotolysisa, nd initial ozone concentrationsis tested in a box model and comparedt o the robustnesso f other earlier proposedi ndicators.I n contrast to earlier proposed indicators, this new one is not based on photochemically producedl ong-liveds peciesb ut describest he instantaneousr egime of an air parcel. Three-dimensionasl imulations howst hat this indicator is quite successfuiln estimatingt he impact of increasedo r reducede missionso n the ozone concentrationsfo r each location in the modeling area. This will make it a very helpful tool for developing ozone abatement strategies

Ozone detection by differential absorption spectroscopy at ambient pressure with a 9.6μm pulsed quantum-cascade laser

We report direct absorption spectroscopic detection of ozone at ambient pressure with a pulsed, DFB quantum-cascade laser (QCL) tuned within 1044-1050cm-1 by temperature scanning. Wavelength calibration curves were derived from FTIR and CO2 spectra and interpreted with respect to the heat transfer from the heterostructure to the sink. The laser linewidth (∼0.13cm-1 FWHM) was found to decrease with temperature, probably as a result of operation at constant current. Spurious spectral features due to baseline inaccuracies were successfully filtered out from the QCL O3 spectra using differential absorption. Reference O3 concentrations were obtained by applying the same method to UV spectra, simultaneously measured with a differential optical absorption spectrometer (DOAS). Column densities retrieved from QCL spectra are in fairly good agreement (±20%) with the DOAS values above 28ppm m. The estimated QCL lowest detectable, absolute and differential absorptions, (7×10-3 and 2×10-3, respectively), entail effective detection limits of 14 and 25ppm m, respectively. Ongoing improvements in the acquisition system should allow the achievement of detection limits at the level of commercial open-path DOAS systems (∼2ppm m) in the near future. Our results demonstrate the applicability of the differential absorption method to QCL spectroscopy at ambient pressure, and encourage its use for open path detectio

An investigation of ozone and planetary boundary layer dynamics over the complex topography of Grenoble combining measurements and modeling

International audienceThis paper concerns an evaluation of ozone (O3) and planetary boundary layer (PBL) dynamics over the complex topography of the Grenoble region through a combination of measurements and mesoscale model (METPHOMOD) predictions for three days, during July 1999. The measurements of O3 and PBL structure were obtained with a Differential Absorption Lidar (DIAL) system, situated 20 km south of Grenoble at Vif (310 m a.s.l.). The combined lidar observations and model calculations are in good agreement with atmospheric measurements obtained with an instrumented aircraft (METAIR). Ozone fluxes were calculated using lidar measurements of ozone vertical profiles concentrations and the horizontal wind speeds measured with a Radar Doppler wind profiler (DEGREANE). The ozone flux patterns indicate that the diurnal cycle of ozone production is controlled by local thermal winds. The convective PBL maximum height was some 2700 m above the land surface while the nighttime residual ozone layer was generally found between 1200 and 2200 m. Finally we evaluate the magnitude of the ozone processes at different altitudes in order to estimate the photochemical ozone production due to the primary pollutants emissions of Grenoble city and the regional network of automobile traffic

Total VOC reactivity in the planetary boundary layer: 1. Estimation by a pump and probe OH experiment

The reactivityo f hydroxyrl adical (OH) with total volatile organicc ompounds (VOC), Z kvoc[VOC ], is directly obtained in the planetary boundary layer (PBL). The method is basedo n a perturbationt echniquew here high initial OH concentrationsa re createdb yf lashp hotolysoisf ozonea nds ubsequerneta ctiono f O(•D) withH 20. Laserinduced fluorescence is used to measure the residual OH concentration at different time delays after the perturbation (<100 ms) and obtain a direct estimate of the OH lifetime rOH for different atmospheric conditions. For specific experimental conditions the transportb y the wind may be neglected,a nd the chemicalp rocessesg overningt he OH decaym ay be expressedb y a detailed box model. With a simple chemicale quation derived in this paper using roll and complementarym easurementso f CO, 03, and NOx, an in situ estimate of Z kvoc[VOC ] in the PBL is retrieved with an uncertainty of less than 20% in comparisont o the detailed box model calculationsT. his analysisi s applied to laboratory measurementsw ith three syntheticN Ox/VOC/O 3 gas mixtures,a nd the retrieved OH lifetimes and total VOC reactivitya re discusseda gainstm odel predictions

Ozone detection by differential absorption spectroscopy at ambient pressure with a 9.6 mu m pulsed quantum-cascade laser

We report direct absorption spectroscopic detection of ozone at ambient pressure with a pulsed, DFB quantum-cascade laser (QCL) tuned within 1044-1050 cm(-1) by temperature scanning. Wavelength calibration curves were derived from FTIR and CO2 spectra and interpreted with respect to the heat transfer from the heterostructure to the sink. The laser linewidth (similar to0.13 cm(-1) FWHM) was found to decrease with temperature, probably as a result of operation at constant current. Spurious spectral features due to baseline inaccuracies were successfully filtered out from the QCL O-3 spectra using differential absorption. Reference O-3 concentrations were obtained by applying the same method to UV spectra, simultaneously measured with a differential optical absorption spectrometer (DOAS). Column densities retrieved from QCL spectra are in fairly good agreement (+/-20%) with the DOAS values above 28 ppm m. The estimated QCL lowest detectable, absolute and differential absorptions, (7x10(-3) and 2x10(-3), respectively), entail effective detection limits of 14 and 25 ppm m, respectively. Ongoing improvements in the acquisition system should allow the achievement of detection limits at the level of commercial open-path DOAS systems (similar to2 ppm m) in the near future. Our results demonstrate the applicability of the differential absorption method to QCL spectroscopy at ambient pressure, and encourage its use for open path detection

How stratospheric are deep stratospheric intrusions? LUAMI 2008

A large-scale comparison of water-vapour vertical-sounding instruments took place over central Europe on 17 October 2008, during a rather homogeneous deep stratospheric intrusion event (LUAMI, Lindenberg Upper-Air Methods Intercomparison). The measurements were carried out at four observational sites: Payerne (Switzerland), Bilthoven (the Netherlands), Lindenberg (north-eastern Germany), and the Zugspitze mountain (Garmisch-Partenkichen, German Alps), and by an airborne water-vapour lidar system creating a transect of humidity profiles between all four stations. A high data quality was verified that strongly underlines the scientific findings. The intrusion layer was very dry with a minimum mixing ratios of 0 to 35 ppm on its lower west side, but did not drop below 120 ppm on the higher-lying east side (Lindenberg). The dryness hardens the findings of a preceding study (“Part 1”, Trickl et al., 2014) that, e.g., 73 % of deep intrusions reaching the German Alps and travelling 6 days or less exhibit minimum mixing ratios of 50 ppm and less. These low values reflect values found in the lowermost stratosphere and indicate very slow mixing with tropospheric air during the downward transport to the lower troposphere. The peak ozone values were around 70 ppb, confirming the idea that intrusion layers depart from the lowermost edge of the stratosphere. The data suggest an increase of ozone from the lower to the higher edge of the intrusion layer. This behaviour is also confirmed by stratospheric aerosol caught in the layer. Both observations are in agreement with the idea that sections of the vertical distributions of these constituents in the source region were transferred to central Europe without major change. LAGRANTO trajectory calculations demonstrated a rather shallow outflow from the stratosphere just above the dynamical tropopause, for the first time confirming the conclusions in “Part 1” from the Zugspitze CO observations. The trajectories qualitatively explain the temporal evolution of the intrusion layers above the four stations participating in the campaign