Norton Allen

Carbon dioxide column abundances at the Wisconsin Tall Tower site

We have developed an automated observatory for measuring atmospheric column abundances of CO_2 and O_2 using near-infrared spectra of the Sun obtained with a high spectral resolution Fourier Transform Spectrometer (FTS). This is the first dedicated laboratory in a new network of ground-based observatories named the Total Carbon Column Observing Network. This network will be used for carbon cycle studies and validation of spaceborne column measurements of greenhouse gases. The observatory was assembled in Pasadena, California, and then permanently deployed to northern Wisconsin during May 2004. It is located in the heavily forested Chequamegon National Forest at the WLEF Tall Tower site, 12 km east of Park Falls, Wisconsin. Under clear sky conditions, ∼0.1% measurement precision is demonstrated for the retrieved column CO_2 abundances. During the Intercontinental Chemical Transport Experiment–North America and CO_2 Boundary Layer Regional Airborne Experiment campaigns in summer 2004, the DC-8 and King Air aircraft recorded eight in situ CO_2 profiles over the WLEF site. Comparison of the integrated aircraft profiles and CO_2 column abundances shows a small bias (∼2%) but an excellent correlation.

New fast response photofragment fluorescence hygrometer for use on the NASA ER‐2 and the Perseus remotely piloted aircraft

We have developed an in situ instrument to measure water vapor on the NASA ER‐2 as a prototype for use on the Perseus remotely piloted aircraft. It utilizes photofragment fluorescence throughout the stratosphere and the upper to middle troposphere (mixing ratios from 2 to 300 ppmv) with simultaneous absorption measurements in the middle troposphere (water vapor concentrations ≳5×1014 mol/cc). The instrument flew successfully on the NASA ER‐2 aircraft during the 1993 CEPEX and SPADE campaigns. The 2σ measurement precision for a 10 s integration time, limited by variation in the background from scattered solar radiation, is ±6% and the data were tightly correlated with other long‐lived stratospheric tracers throughout the SPADE mission. Its accuracy is estimated to be ±10%, based on laboratory calibrations using a range of water vapor concentrations independently determined by both standard gas addition techniques and by absorption. This accuracy is confirmed by in‐flight absorption measurements in the trop...

A new cavity based absorption instrument for detection of water isotopologues in the upper troposphere and lower stratosphere

We describe here the Harvard integrated cavity output spectroscopy (ICOS) isotope instrument, a mid-IR infrared spectrometer using ICOS to make in situ measurements of the primary isotopologues of water vapor (H(2)O, HDO, and H(2) (18)O) in the upper troposphere and lower stratosphere (UTLS). The long path length provided by ICOS provides the sensitivity and accuracy necessary to measure these or other trace atmospheric species at concentrations in the ppbv range. The Harvard ICOS isotope instrument has been integrated onto NASAs WB-57 high-altitude research aircraft and to date has flown successfully in four field campaigns from winter 2004-2005 to the present. Off-axis alignment and a fully passive cavity ensure maximum robustness against the vibrationally hostile aircraft environment. The very simple instrument design permitted by off-axis ICOS is also helpful in minimizing contamination necessary for accurate measurements in the dry UTLS region. The instrument is calibrated in the laboratory via two separate water addition systems and crosscalibrated against other instruments. Calibrations have established an accuracy of 5% for all species. The instrument has demonstrated measurement precision of 0.14 ppmv, 0.10 ppbv, and 0.16 ppbv in 4 s averages for H(2)O, HDO, and H(2) (18)O, respectively. At a water vapor mixing ratio of 5 ppmv the isotopologue ratio precision is 50[per thousand] and 30[per thousand] for deltaD and delta(18)O, respectively.

Mechanisms for midlatitude ozone loss: Heterogeneous chemistry in the lowermost stratosphere?

The question of midlatitude ozone erosion by chlorine free radical catalysis is examined. We present and analyze simultaneous, high-resolution observations of ClO, H2O, tropopause height, particle reactive surface area, and ice saturation occurrence frequency obtained from the NASA ER-2 aircraft. The objective is to test the hypothesis that the existence of cirrus clouds or cold aerosols in the first few kilometers above the tropopause at midlatitudes is responsible for increasing the ratio of chlorine free radicals to total inorganic chlorine, thus amplifying the rate of catalytic ozone destruction. The observations reveal a sharp decrease in ice saturation frequency at the tropopause, a marked degree of under-saturation just above the tropopause, a corresponding sharp gradient in the product of cold aerosol reactive surface area and reaction probability, γSa, and, finally, the consistent absence of enhanced concentrations of ClO immediately above the tropopause. These results suggest that midlatitude ozone loss is not controlled in situ by the mechanism of cirrus cloud and/or cold aerosol enhancement of chlorine radicals in the vicinity of the tropopause.

Measurements of the Total Water Content of Cirrus Clouds. Part I: Instrument Details and Calibration

Abstract This paper describes an instrument designed to measure the sum of gas phase and solid phase water, or total water, in cirrus clouds, and to be mounted in a pallet in the underbelly of the NASA WB-57 research aircraft. The ice water content of cirrus is determined by subtracting water vapor measured simultaneously by the Harvard water vapor instrument on the aircraft. The total water instrument uses an isokinetic inlet to maintain ambient particle concentrations as air enters the instrument duct, a 600-W heater mounted directly in the flow to evaporate the ice particles, and a Lyman-α photofragment fluorescence technique for detection of the total water content of the ambient air. Isokinetic flow is achieved with an actively controlled roots pump by referencing aircraft pressure, temperature, and true airspeed, together with instrument flow velocity, temperature, and pressure. Laboratory calibrations that utilize a water vapor addition system that adds air with a specific humidity tied to the vapo...

The performance of a new instrument for in situ measurements of ClO in the lower stratosphere

Abundances of chlorine oxide (ClO) have been measured from 16 km to 30 km by a new balloon-borne in situ instrument developed from an optical design flown previously on the NASA ER-2 aircraft. This instrument, a prototype for one to be flown on the Perseus remotely piloted aircraft, was one-third the weight of that on the ER-2, yet retained the high precision and accuracy necessary for detailed photochemical studies of the lower stratosphere. In this paper we discuss the performance of the instrument during its first flight on March 31, 1991 over eastern New Mexico.

A new photolysis laser-induced fluorescence instrument for the detection of H2O and HDO in the lower stratosphere

We present a new instrument, Hoxotope, for the in situ measurement of H(2)O and its heavy deuterium isotopologue (HDO) in the upper troposphere and lower stratosphere aboard the NASA WB-57. Sensitive measurements of deltaD are accomplished through the vacuum UV photolysis of water followed by laser-induced fluorescence detection of the resultant OH and OD photofragments. The photolysis laser-induced fluorescence technique can obtain S/N>20 for 1 ppbv HDO and S/N>30 for 5 ppmv H(2)O for 10 s data, providing the sensitivity required for deltaD measurements in the tropopause region. The technique responds rapidly to changing water concentrations due to its inherently small sampling volume, augmented by steps taken to minimize water uptake on instrument plumbing. Data from the summer 2005 Aura Validation Experiment Water Isotope Intercomparison Flights (AVE-WIIF) out of Houston, TX show agreement for H(2)O between Hoxotope and the Harvard water vapor instrument and for HDO between Hoxotope and the Harvard ICOS water isotope instrument, to within stated instrument uncertainties. The successful intercomparison validates Hoxotope as a credible source of deltaD data in the upper troposphere and lower stratosphere.

Measurements of the Total Water Content of Cirrus Clouds. Part II: Instrument Performance and Validation

Abstract This paper describes the performance and in-flight validation of an instrument mounted in a pallet on the NASA WB-57 research aircraft that measures the sum of gas phase and solid phase water, or total water, in cirrus clouds. Using a heated isokinetic inlet and a Lyman-α photofragment fluorescence technique for detection, measurements of total water have been made over three orders of magnitude. During the Cirrus Regional Study of Tropical Anvils and Cirrus Layers Florida Area Cirrus Experiment (CRYSTAL FACE), the instrument operated at duct temperatures sufficiently warms to completely evaporate particles up to 150-μm diameter. Laboratory calibrations, in-flight diagnostics, intercomparison with water vapor measured by absorption in flight, and intercomparisons in clear air with the Harvard water vapor instrument validate the detection sensitivity of the instrument and illustrate the minimal hysteresis from instrument surface contamination. The Harvard total water and water vapor instruments to...

A new direct absorption tunable diode laser spectrometer for high precision measurement of water vapor in the upper troposphere and lower stratosphere

We present a new instrument for the measurement of water vapor in the upper troposphere and lower stratosphere (UT∕LS), the Harvard Herriott Hygrometer (HHH). HHH employs a tunable diode near-IR laser to measure water vapor via direct absorption in a Herriott cell. The direct absorption technique provides a direct link between the depth of the observed absorption line and the measured water vapor concentration, which is calculated based on spectroscopic parameters in the HITRAN database. While several other tunable diode laser (TDL) instruments have been used to measure water vapor in the UT∕LS, HHH is set apart by its use of an optical cell an order of magnitude smaller than those of other direct absorption TDLs in operation, allowing for a more compact, lightweight instrument. HHH is also unique in its integration into a common duct with the Harvard Lyman-α hygrometer, an independent photo-fragment fluorescence instrument which has been thoroughly validated over 19 years of flight measurements. The instrument was flown for the first time in the Mid-latitude Airborne Cirrus Properties Experiment (MACPEX) on NASAs WB-57 aircraft in spring, 2011, during which it demonstrated in-flight precision of 0.1 ppmv (1 s) with 1-sigma uncertainty of 5% ± 0.7 ppmv. Since the campaign, changes to the instrument have lead to improved accuracy of 5% ± 0.2 ppmv as demonstrated in the laboratory. During MACPEX, HHH successfully measured water vapor at concentrations from 3.5 to 600 ppmv in the upper troposphere and lower stratosphere. HHH and Lyman-α, measuring independently but under the same sampling conditions, agreed on average to within 1% at water vapor mixing ratios above 20 ppmv and to within 0.3 ppmv at lower mixing ratios. HHH also agreed with a number of other in situ water vapor instruments on the WB-57 to within their stated uncertainties, and to within 0.7 ppmv at low water. This agreement constitutes a significant improvement over past in situ comparisons, in which differences of 1.5-2 ppmv were routinely observed, and demonstrates that the accuracy of HHH is consistent with other instruments which use a range of detection methods and sampling techniques.

Development of a cw Cavity Enhanced Instrument for Simultaneous Detection of Multiple Trace Species

An instrument for simultaneous measurement of atmospheric water isotopes using cavity enhanced absorption spectroscopy has been developed. High precision and accuracy measurements (HDO <0.1 ppbv) were achieved by improved cavity design and data fitting algorithms.