Multiple Axis Resonance Fluorescence Chemical Conversion Detector for ClO and BrO

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.

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In Situ Airborne Formaldehyde

The NASA GSFC In Situ Airborne Formaldehyde (ISAF) instrument measures formaldehyde on high altitude NASA aircraft. The instrument uses laser induced fluorescence (LIF) to obtain the high detection sensitivity needed to detect formaldehyde in the upper troposphere and lower stratosphere where abundances are 10 parts per trillion. LIF also enables a fast time response needed to measure the abundance of formaldehyde in the finely structured outflow of convective storms. These measurements of formaldehyde will be used elucidate mechanisms of convective transport and quantify the effects of boundary layer pollutants on the ozone photochemistry and cloud microphysics of the upper atmosphere.

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Vacuum UV Resonance Fluorescence CO Instrument

The NCAR/NSF G-V vacuum UV resonance fluorescence instrument is a commercial version of the instrument published by Gerbig, et al. (Journal of Geophysical Research, Vol. 104, No. D1, 1699-1704, 1999). The source is a flowing RF discharge gas lamp emitting in the VUV. An optical filter provides a narrow band of source radiation centered at 151 nm with a 10 nm bandpass. CO fluorescence is detected using photon counting. The internal data system can accommodate sampling rates from 1-18 samples/second. For SEAC4RS, the instrument was integrated into the HAIS ozone instrument rack and shared a pressure-controlled inlet.

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Harvard Halogen Instrument

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.

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UNH Mercury

The UNHMERC instrument provides detailed information on atmospheric mercury. Measurements of total gaseous mercury (TGM) and gaseous elemental mercury (Hg°) are performed simultaneously with one minute time resolution using a custom four-channel atomic fluorescence spectrometer. The relative amount of reactive gaseous mercury (RGM = HgCl2 + HgBr2+ HgOBr + …) will be assessed through careful examination of the difference between TGM and Hg°. TGM is defined as the sum Hg° + RGM. Targeted aerosol sampling will also be conducted for particulate-phase mercury (HgP).

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Thermal-Dissociation Laser Induced Fluorescence

The UC Berkeley thermal-dissociation laser-induced fluorescence (TD- LIF) instrument detects NO2 directly and detects total peroxynitrates (ΣPNs ≡ PAN + PPN +N2O5 + HNO4. . .), total alkyl- and other thermally stable organic nitrates (ΣANs), and HNO3 following thermal dissociation of these NOy species to NO2. The sensitivity for NO2 at 1 Hz is 30 pptv (S/N=2) with a slope uncertainty of 5%. The uncertainties for the dissociated species are 10% for ΣPNs and 15% for ΣANs and HNO3.

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URI Peroxides and Formaldehyde Instrument

POPS measures CH2O, H2O2, and CH3OOH.

CH2O is measured by aqueous collection followed by enzyme fluorescence detection.

H2O2 and CH3OOH is measured by aqueous collection followed by HPLC separation and enzyme fluorescence detection.

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Georgia Tech Laser-Induced Fluorescence

The Georgia Tech Laser-Induced Fluorescence instrument measures nitric oxide (NO), formaldehyde (HCHO), and nitrogen dioxide (NO2). Each species is measured by laser-induced fluorescence at reduced pressure. Ambient air is drawn in through a pinhole orifice into a pair of multipass White cells. The pressure in the White cells is maintained at 5-10 mbar to extend the fluorescence lifetime, and the multiple passes (typically 32-40) effectively extends the probe interaction volume. The ambient air is probed at 90o from the flow and the fluorescence collected at 90o to the flow and probe.

NO is probed at the 226 absorption line and monitored at the 247 nm fluorescence. The laser pulse and scattering will be time-gated out using microchannel plate detectors. The expected 2-sigma limit of detection is 5 pptv/min. Formaldehyde is probed at 353 nm and the fluorescence monitored in a range from 400 to 450 nm. The expected performance is 10 pptv/min. NO2 will be probed near 435 nm and the fluorescence around 780 nm collected. Its expected performance is 15 pptv/min. In each case, the probe wavelength will be alternately switched from the absorption feature to a nearby “off-line” position to determine the background. The actual frequency will be monitored in reference cells. Calbration is done by standard addition to the airflow. The light sources used are custom-built cavities pumped by a diode-pumped Nd:YAG laser operating at ~10 kHz.

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Chlorine Nitrate Instrument

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.

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Harvard Total Water

The design of the newly developed total water instrument is based on the same principles as the water vapor instrument, and is intended to fly in conjunction with it. Conceptually, the total water instrument can be thought of as containing four subsystems:
1. An inlet through which liquid and/or solid water particles can be brought into an instrument duct without perturbing the ambient particle density.
2. A heater that efficiently evaporates the liquid/solid water before it reaches the detection axis.
3. Ducting through which the air flows to the detection axis without perturbing the (total) water vapor mixing ratio.
4. A water vapor detection axis that accurately and precisely measures the total water content of the ambient air.

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