Water vapor concentrations are measured using the cryogenically-cooled, chilled mirror hygrometer (Buck Research model CR-1). This instrument has a wide dynamic range (-90 to +30 C or approximately 1 to 30,000 ppmv H2O) and reasonably rapid response time (2 to 20 seconds, depending on the temporal and quantitative characteristics of the change in water vapor concentrations). The model CR-1 hygrometer utilizes a cryogenically chilled mirror and electro-optical technique to determine the dew/frost point of a gas. The primary difference between the CR-1 and other chilled mirror hygrometers is the mechanism used to cool the mirror surface. The mirror surface on which the dew/frost layer is preserved is coupled to a rod cooled by LN2 cryogen. The mirror surface is heated to the dew/frost point by means of a heater winding attached to the mirror rod. A control circuit controlled by optics monitors the reflectance from a LED off the mirror surface and maintains the condensate layer at a preset level. A thermistor embedded in the mirror measures the surface temperature and is output as a direct reading of the dew/frost point of the sample gas.

Air samples for the CR-1 hygrometer are provided by a separate window-mounted droplet-excluding inlet probe which has been used aboard the DC-8 platform in previous field missions. The in situ sampling probe consists of a stainless steel tubing inlet probe insert combined with a Rosemount type102 non-deiced temperature sensor housing. This type forward-facing probe provides inboard sampling of ambient air while maintaining efficient inertial separation of droplets and particles from the sampled air stream. The outer structural portion of the probe is manufactured by Rosemount Aerospace, Inc. and is flight-certified for use aboard both research and commercial jet aircraft. In normal subsonic flight, the inlet is self-pumping and develops enough pressure head to provide up to 15 liters/minute airflow through the approximately the 1 meter of ¼ “ stainless steel tubing which connects the inlet to the sensors. The tubing used to supply the sample air to the hygrometer is heated to approximately 50° C to avoid any chance of internal condensation in the sample line and reduce errors associated with wall effects.

The NOy instrument has three independent chemiluminescence detectors for simultaneous measurements of NOy, NO2, and NO. Each detector utilizes the reaction between NO in the sample with reagent O3. The NO/O3 reaction produces excited state NO2 which emits light of near 1µ m wavelength. Emitted photons are detected with a cooled photomultiplier tube.

Because NOy species other than NO do not respond in the chemiluminescence detector, NOy component species are reduced to NO by catalytic reduction on a gold surface with carbon monoxide (CO) acting as a reducing agent. Conversion efficiencies are > 90% at surface temperatures of 300°C. An NO signal representing NOy is then detected by chemiluminescence in the detector module. The catalyst is located outside the aircraft fuselage in order to avoid inlet line losses. NO2 is photolytically converted to NO in a glass cell in the presence of intense UV light between 300 and 400 nm. The conversion fraction is > 50% for a residence time of 1 s. The chemiluminescence detector detects NO as well as the additional NO from NO2. The third channel measures NO directly by passing the ambient sample through the detector module.

The response of each detector is checked several times in flight by standard addition of NO or NO2 calibration gas. The baseline of each measurement is determined in part by the addition of synthetic air that contains no reactive nitrogen. A continuous flow of water vapor is added directly to the sample flow in order to reduce the background signal in the detectors.

The sampling inlet for NOy is located outside the fuselage of the aircraft in a separate football-shaped housing. The shape of the housing allows for the inertial separation of large aerosols (> 5 µm diameter) from the NOy inlet at the downstream end of the housing.

NO is measured using a chemiluminescence detector. One of the four NO detectors is used for the NO measurements. NOy is measured simultaneously by catalytically converting it to NO on the surface of gold tubes heated to ±° C, with carbon monoxide (CO) acting as a reducing agent. The converter system is contained in a pod mounted outside the cabin to minimize the length of the inlet tubes. Gas phase-NOy measurements are made by sampling air through the rearward facing inlet which discriminates against particles of diameter larger than 1 mm. The mixing ratios of total NOy (gas phase-NOy + amplified particulate-NOy) are measured by sampling air through the forward facing inlet which is heated to 100° C. The mixing ratios of gas phase and total NOy are measured independently. A humidifier maintains the H2O mixing ratio in sample flows at a few % in order to stabilize the instrument background against humidity variations in the ambient air. The absolute sensitivities of the NO and NOy channels are measured every 80 minutes by adding NO or NO2 standard gases. The pressure in the gold catalytic converter for gas-phase NOy is maintained at a constant value of about 50 hPa, independent of the ambient pressure. The pressure is held constant by controlling the sample flow using a servo-controlled Teflon valve mounted upstream of the converter tube. All parts of the inlet system upstream of the gold catalyst are made of Perfluoroalkoxy (PFA) Teflon which is temperature controlled at 40˚C. The NO2 conversion efficiency is 99.0611%. The HCN conversion efficiency is lower than 5% for dry air with O3 mixing ratios lower than 100 ppbv. It decreases to 2% for humid air with an H2O mixing ratio of 0.1% and O3 mixing ratios lower than 100 ppbv. This instrument is also equipped with an NO2 photolytic converter combined with an NO detector in our first attempt to access the accuracy of the NO2 measurements.

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 absorption of infrared solar radiation along a slant path to the sun is recorded from 2 to 15 micrometers. Six spectral filters are used to cover the region from 2-15 microns. An interferogram is recorded in about 10 seconds. Interferograms are transformed to produce spectra. Column amounts are retrieved by fitting the observed spectra using the non-linear least squares fitting code SFIT2 that employs an Optimal Estimation retrieval algorithm.

The major chlorine reservoirs (HCl and ClONO2), the important nitrogen-containing gases in the stratosphere (N2O, NO, NO2, and HNO3), stratospheric and tropospheric tracers (HF, CH4, C2H6, H2O, CO2), a major source CFC (CF2Cl2) and ozone may be routinely retrieved.

• Technique: Chemluminescent reaction of ozone with nitric oxide
• Dynamic Range: 0.6 - 1600 ppb
• Accuracy: 5% or 2 ppb
• Precision: 2% or 0.6 ppb
• Response: 2-3 Hz; recorded at 6 Hz, reported at 1 Hz, faster data on request
• Spatial Resolution: <10 m vertical (aircraft spiral), 200 m horizontal (at 400 kts)

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 Aerosol Lidar system measures profiles of aerosol and/or cloud backscatter at 532 and 1064 nm and aerosol/cloud depolarization at 532 nm. Backscatter profiles at these two wavelengths provide information on the relative concentration and spatial distribution of aerosol/cloud particles. Comparison of aerosol/cloud backscatter at the two wavelengths provides some indication of particle size. Measurement of the depolarizing effect of the particles (that is, the degree to which the polarization of the backscattered light from the particles differs from the linear polarization of the transmitted laser light) provides an indication of particle phase.

The Aerosol Lidar is a piggy-back instrument on AROTEL lidar fielded by John Burris and Tom McGee of NASA Goddard Space Flight Center. The light source for the aerosol measurements is a Continuum 9050 Nd:YAG laser operating at 50 shots per second. The laser transmits approximately 600 mJ at 1064 nm, 250 mJ at 532 nm, and 350 mJ at 355 nm. AROTEL also employs an excimer laser transmitting at 308 nm and uses the molecular and Raman backscatter from the 355 and 308 beams to measure ozone and temperature. Backscattered light at all wavelengths is collected by a 16-inch diameter Newtonian telescope with a selectable field stop. In the aft optics assembly following the telescope and field stop, the UV signals are separated from the 532- and 1064-nm signals by a dichroic beam splitter. The UV signals are directed to the AROTEL receiver assembly and the 532- and 1064-nm signals are directed to the Aerosol Lidar receiver assembly. In the Aerosol Lidar receiver, a rotating shutter blocks the very strong near-range 532- and 1064-nm signals in order to reduce distortion in the relatively weaker signals from higher altitudes. The 532- and 1064-nm signals are separated by a dichroic beam splitter and the 532-nm signal is further separated into orthogonal polarization components using a polarizing beam cube. A computer-controlled half-wave plate in front of the polarizing beam cube is rotated so that the polarization of the 532 signals are parallel and perpendicular to the polarization of the transmitted laser pulses. The signals at both wavelengths and both 532-nm polarizations are transmitted to detectors at the Aerosol Lidar data acquisition rack via fiber optic cables. Each optical signal, the 1064-nm total backscatter and the 532-nm parallel and perpendicularly polarized backscatter, is directed to two separate detectors, with 10% going to one detector and 90% to the other, in order to more accurately measure the signals over their full dynamic range. The 532-nm returns are measured with photo-multiplier tubes and the 1064-nm returns are measured with avalanche photo-diodes. Because of the high optical signal levels, all data are acquired in analog mode, using 12-bit analog-to-digital converters. The instrument operates under both daytime and nighttime lighting conditions, with a slight degradation in data quality during the daytime.

The Whole Air Sampler (WAS) collects samples from airborne platforms for detailed analysis of a wide range of trace gases. The compounds that are typically measured from the WAS includes trace gases with sources from industrial midlatitude emissions, from biomass burning, and from the marine boundary layer, with certain compounds (e.g. organic nitrates) that have a unique source in the equatorial surface ocean. The use of a broad suite of tracers with different sources and lifetimes provides powerful diagnostic information on air mass history and chemical processing that currently is only available from measurements from whole air samples. Previous deployments of the whole air sampler have shown that the sampling and analytical procedures employed by our group are capable of accessing the wide range of mixing ratios at sufficient precision to be used for tracer studies. Thus, routine measurement of species, such as methyl iodide, at <= 0.1 x 10-12 mole fraction, or NMHC at levels of a few x 10-12 mole fraction are possible. In addition to the tracer aspects of the whole air sampler measurements, we measure a full suite of halocarbon species that provide information on the role of short-lived halocarbons in the tropical UT/LS region, on halogen budgets in the UT/LS region, and on continuing increasing temporal trends of HFCs (such as 134a), HCFCs (such as HCFC 141b), PFCs (such as C2F6), as well as declining levels of some of the major CFCs and halogenated solvents. The measurements of those species that are changing rapidly in the troposphere also give direct indications of the age and origin of air entering the stratosphere.

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.