NASA - National Aeronautics and Space Administration

Vacuum ultraviolet radiation produced in a low pressure plasma discharge lamp is used to induce resonance scattering in Cl and Br atoms within a flowing sample. ClO and BrO are converted to Cl and Br by the addition of NO such that the rapid bimolecular reaction ClO + NO → Cl + NO2 (BrO + NO → Br + NO2) yields one halogen atom for each halogen oxide radical present in the flowing sample. Three detection axes are used to diagnose the spatial (and thus temporal) dependence of the ClO (BrO) to Cl (Br) conversion and to detect any removal of Cl (Br) following its formation. A double duct system is used both to maintain laminar flow through the detection region and to step the flow velocity in the detection region down from free stream (200 m/sec) to 20 m/sec in order to optimize the kinetic diagnosis.

Many changes from the original Chlorine Nitrate instrument. NO2 instrument removed. New inlet with orifice for one halogen duct, addition of vacuum scroll pump, new RF oscillators and amplifiers, new RF frequency, new lamp housings and cooling for lamp modules. Flew in MACPEX without dissociation heaters, i.e., focus on BrO and ClO measurements and not measure ClONO2 or ClOOCl.

The NO2-ClO-ClONO2-BrO instrument is composed of two separate instruments: A laser-induced fluorescence instrument for the detection of NO2 and a thermal dissociation/resonance fluorescence instrument for the detection of ClO, ClONO2 and BrO.

The NO2 detection system uses laser-induced resonance fluorescence (LIF) for the direct detection of NO2. Ambient air passes through a detection axis where the output of a narrow bandwidth (0.06 cm-1), tunable dye laser operating near 585 nm is used to excite a rovibronic transition in NO2. The excited NO2 molecules are either quenched by collision with air or fluorescence. The NO2 fluorescence is strongly red-shifted, with emission occurring over a broad range of wavelengths from 585 nm to the mid-infrared. The specificity of the technique is accomplished by tuning the laser frequency on and off resonance with a narrow spectral feature (0.04 cm-1) in the NO2 absorption spectrum. The difference between the fluorescence signal on and off resonance is related to the mixing ratio of NO2 through laboratory and in-flight calibrations. The observations are determined with an accuracy (1 sigma) of ±10% ±50 pptv, precision (1 sigma) of ±40 pptv, and a reporting interval of 10 seconds. Higher resolution (0.25 sec) data available on request.

The halogen detection system uses gas-phase thermal dissociation of ambient ClONO2 to produce ClO and NO2 radicals. The pyrolysis is accomplished by passing the air sampled in a 5-cm-square duct through a grid of resistively heated silicon strips at 10 to 20 m/sec, rapidly heating the air to 520 K. The ClO fragment from ClONO2 is converted to Cl atoms by reaction with added NO, and Cl atoms are detected using ultra-violet resonance fluorescence at 118.9 nm. A similar detection axis upstream of the heater provides simultaneous detection of ambient ClO. An identical twin sampling duct provides the capability for diagnostic checks. The flight instrument is calibrated in a laboratory setting with known addition of ClONO2 as a function of pressure, heater temperature and flow velocity. The concentration of ClONO2 is measured with an accuracy and detection limit of ±20% and 10 pptv, respectively, in 35 seconds (all error estimates are 1 sigma). The concentration of ClO is measured with an accuracy and detection limit of ±17% and 3 pptv, respectively, in 35 seconds.

The ASUR (Airborne SUbmillimeter Radiometer) is an airborne radiometer measuring the thermal emission of trace gases in the stratosphere (in an altitude range between 15 and 50 km). The instrument detects the radiation in a frequency range between 604.3 and 662.3 GHz. This corresponds to wavelengths of about 0.45-0.5 mm. In this frequency range a major part of the radiation is absorbed by atmospheric water vapor. As most of the water vapor is found in the troposphere (in the Arctic up to 8 km, in the tropics up to 16 km altitude) the instrument is operated on board of an aircraft flying at an altitude of 10-12 km, such that a major part of the water vapor absorption is avoided. Using appropriate inversion techniques vertical profiles from 15 to over 50 km altitude can be retrieved with a vertical resolution of typically 6 km and 12 km in the lower and upper stratosphere, respectively.

The Submillimeterwave Limb Sounder (SLS) is a heterodyne radiometer measuring thermal emission spectra near 640 GHz (for detection of ClO, HCl, and O3) and 604 GHz. (for detection of HNO3 and N2O) designed for use on high altitude balloons and aircraft. The instrument consists of five subsystems:

-optics which define the instrument field of view (FOV)
-radiometer front-ends which down converts incoming radiance signals
-intermediate frequency (IF) stage which selects and frequency shifts signal bands
-spectrometers which frequency resolve and detect the incoming power spectrum
-command and data handling which controls the instrument and transmits data to the ground

Limb scanning is accomplished by a flat mirror (~20 cm diameter) connected to a stepper motor (0.2 steps) and 14 bit position encoder. This mirror is also used for gain and zero calibration by viewing an absorber target located below the mirror and upward at 47° elevation angle to view the cold sky. A set of three off-axis parabolic reflectors form the instrument field of view (0.35 full width at half maximum) and couple limb radiance to the mixer input waveguide. These reflectors are oversized (~30 dB edge taper) to minimize side lobes in the FOV. Pointing and beam shape were verified by scanning the instrument FOV across the emission from a 600 GHz transmitter (multiplied output of a Gunn oscillator) located in the receiver optical far-field.

The radiometer front-end is an uncooled second harmonic mixer using a waveguide mounted Schottky diode. The radiometer is operated double side band (DSB), i.e., spectral features occurring symmetrically above and below the effective local oscillator frequency (637.050 GHz) appear together in the IF output spectrum. The diode is pumped at a 318.525 GHz. This source is generated by a tripled 106.175 GHz phase-locked InP Gunn oscillator and wave guide coupled to the mixer block. The mixer produces an IF output spectrum of 10.5 to 13 GHz, which corresponds to signals at the mixer input at 647.5 GHz to 650.0 GHz (in the radiometer upper side band) and 626.5 GHz to 624.1 GHz ( in the lower side band). The design of the 604 GHz radiometer system is similar to 637 GHz system but operates at a lower IF frequency of 2 to 3 GHz.

Diagram of the SLS frequency down-conversion scheme. RF signals enter the signal flow path through mixer feeds at the left of the diagram. At the right side, the signal flow enters a set of UARS MLS-type filterbank spectrometers where bands are further spectrally resolved, power detected, and digitized.

The Charged-coupled device Actinic Flux Spectroradiometers (CAFS) instruments measure in situ down- and up-welling radiation and combine to provide 4 pi steradian actinic flux density spectra from 280 to 650 nm. The sampling resolution is ~0.8 nm with a full width at half maximum (FWHM) of 1.7 nm at 297 nm. From the measured flux, photolysis frequencies are calculated for ~40 important atmospheric trace gases including O3, NO2, HCHO, HONO and NO3 using a modified version of the NCAR Tropospheric Ultraviolet and Visible (TUV) radiative transfer model. The absolute spectral sensitivity of the instruments is determined in the laboratory with 1000 W NIST-traceable tungsten-halogen lamps with a wavelength dependent uncertainty of 3–5%. During deployments, spectral sensitivity is assessed with secondary calibration lamps while wavelength assignment is tracked with Hg line sources and comparisons to spectral features in the extraterrestrial flux. The optical collectors are characterized for angular and azimuthal response and the effective planar receptor distance. CAFS have an excellent legacy of performance on the NASA DC-8 and WB-57 platforms during atmospheric chemistry and satellite validation mission. These include AVE Houston 2004 and 2005, PAVE, CR-AVE, TC4, ARCTAS, DC3, SEAC4RS, KORUS-AQ, ATom and FIREX-AQ. For FIREX-AQ, upgraded electronics and cooling reduced noise and allowed for a decrease to 1 Hz acquisition.