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Anderson, J. G.

Publications and source records attributed to Anderson, J. G..

At least 19 records

The Development and Deployment of a Ground-Based, Laser-Induced Fluorescence Instrument for the In Situ Detection of Iodine Monoxide Radicals

High abundances of iodine monoxide (IO) are known to exist and to participate in local photochemistry of the marine boundary layer. Of particular interest are the roles IO plays in the formation of new particles in coastal marine environments and in depletion episodes of ozone and mercury in the Arctic polar spring. This paper describes a ground-based instrument that measures IO at mixing ratios less than one part in 1012. The IO radical is measured by detecting laser-induced fluorescence at wavelengths longer that 500 nm. Tunable visible light is used to pump the A23/2 (v = 2) ← X23/2 (v = 0) transition of IO near 445 nm. The laser light is produced by a solid-state, Nd:YAG-pumped Ti:Sapphire laser at 5 kHz repetition rate. The laser-induced fluorescence instrument performs reliably with very high signal-to-noise ratios (>10) achieved in short integration times (<1 min). The observations from a validation deployment to the Shoals Marine Lab on Appledore Island, ME are presented and are broadly consistent with in situ observations from European Coastal Sites. Mixing ratios ranged from the instrumental detection limit (<1 pptv) to 10 pptv. These data represent the first in situ point measurements of IO in North America.

marine boundary layer↗

Achieving Climate Change Absolute Accuracy in Orbit

The Climate Absolute Radiance and Refractivity Observatory (CLARREO) mission will provide a calibration laboratory in orbit for the purpose of accurately measuring and attributing climate change. CLARREO measurements establish new climate change benchmarks with high absolute radiometric accuracy and high statistical confidence across a wide range of essential climate variables. CLARREO's inherently high absolute accuracy will be verified and traceable on orbit to Système Internationale (SI) units. The benchmarks established by CLARREO will be critical for assessing changes in the Earth system and climate model predictive capabilities for decades into the future as society works to meet the challenge of optimizing strategies for mitigating and adapting to climate change. The CLARREO benchmarks are derived from measurements of the Earth's thermal infrared spectrum (5-50 micron), the spectrum of solar radiation reflected by the Earth and its atmosphere (320-2300 nm), and radio occultation refractivity from which accurate temperature profiles are derived. The mission has the ability to provide new spectral fingerprints of climate change, as well as to provide the first orbiting radiometer with accuracy sufficient to serve as the reference transfer standard for other space sensors, in essence serving as a "NIST [National Institute of Standards and Technology] in orbit." CLARREO will greatly improve the accuracy and relevance of a wide range of space-borne instruments for decadal climate change. Finally, CLARREO has developed new metrics and methods for determining the accuracy requirements of climate observations for a wide range of climate variables and uncertainty sources. These methods should be useful for improving our understanding of observing requirements for most climate change observations.

Wielicki, Bruce A.↗

Quantifying the Impact of the North American Monsoon and Deep Midlatitude Convection on the Subtropical Lowermost Stratosphere using in Situ Measurements

The chemical composition of the lowermost stratosphere exhibits both spatial and temporal variability depending upon the relative strength of (1) isentropic transport from the tropical tropopause layer (TTL), (2) diabatic descent from the midlatitude and northern midlatitude stratosphere followed by equatorward isentropic transport, and (3) diabatic ascent from the troposphere through convection. In situ measurements made in the lowermost stratosphere over Florida illustrate the additional impact of equatorward flow around the monsoon anticyclone. This flow carries, along with older stratospheric air, the distinct signature of deep midlatitude convection. We use simultaneous in situ measurements of water vapor (H2O), ozone (O3), total odd nitrogen (NOy), carbon dioxide (CO2), and carbon monoxide (CO) in the framework of a simple box model to quantify the composition of the air sampled in the lowermost stratosphere during the mission on the basis of tracer mixing ratios ascribed to the source regions for these transport pathways. The results show that in the summer, convection has a significant impact on the composition of air in the lowermost stratosphere, being the dominant source of water vapor up to the 380 K isentrope. The implications of these results extend from the potential for heterogeneous ozone loss resulting from the increased frequency and lifetime of cirrus near the local tropopause, to air with increased water vapor that as part of the equatorward flow associated with the North American monsoon can become part of the general circulation.

Weinstock, E. M.↗

Validation and Determination of Ice Water Content - Radar Reflectivity Relationships during CRYSTAL-FACE: Flight Requirements for Future Comparisons

In order for clouds to be more accurately represented in global circulation models (GCM), there is need for improved understanding of the properties of ice such as the total water in ice clouds, called ice water content (IWC), ice particle sizes and their shapes. Improved representation of clouds in models will enable GCMs to better predict for example, how changes in emissions of pollutants affect cloud formation and evolution, upper tropospheric water vapor, and the radiative budget of the atmosphere that is crucial for climate change studies. An extensive cloud measurement campaign called CRYSTAL-FACE was conducted during Summer 2002 using instrumented aircraft and a variety of instruments to measure properties of ice clouds. This paper deals with the measurement of IWC using the Harvard water vapor and total water instruments on the NASA WB-57 high-altitude aircraft. The IWC is measured directly by these instruments at the altitude of the WB-57, and it is compared with remote measurements from the Goddard Cloud Radar System (CRS) on the NASA ER-2. CRS measures vertical profiles of radar reflectivity from which IWC can be estimated at the WB-57 altitude. The IWC measurements obtained from the Harvard instruments and CRS were found to be within 20-30% of each other. Part of this difference was attributed to errors associated with comparing two measurements that are not collocated in time an space since both aircraft were not in identical locations. This study provides some credibility to the Harvard and CRS-derived IWC measurements that are in general difficult to validate except through consistency checks using different measurement approaches.

Sayres, D. S.↗

Methods for Validation and Intercomparison of Remote Sensing and In situ Ice Water Measurements: Case Studies from CRYSTAL-FACE and Model Results

Remote sensing observations, such as those from AURA, are necessary to understand the role of cirrus in determining the radiative and humidity budgets of the upper troposphere. Using these measurements quantitatively requires comparisons with in situ measurements that have previously been validated. However, a direct comparison of remote and in situ measurements is difficult due to the requirement that the spatial and temporal overlap be sufficient in order to guarantee that both instruments are measuring the same air parcel. A difficult as this might be for gas phase intercomparisons, cloud inhomogeneities significantly exacerbate the problem for cloud ice water content measurements. The CRYSTAL-FACE mission provided an opportunity to assess how well such intercomparisons can be performed and to establish flight plans that will be necessary for validation of future satellite instruments. During CRYSTAL-FACE, remote and in situ instruments were placed on different aircraft (NASA's ER-2 and WB-59, and the two planes flew in tandem so that the in situ payload flew in the field of view of the remote instruments. We show here that, even with this type of careful flight planning, it is not always possible to guarantee that remote and in situ instruments are viewing the same air parcel. We use ice water data derived from the in situ Harvard Total Water (HV-TW) instrument, and the remote Goddard Cloud Radar System (CRS) and show that agreement between HV-TW and CRS is a strong function of the horizontal separation and the time delay between the aircraft transects. We also use a cloud model to simulate possible trajectories through a cloud and evaluate the use of statistical analysis in determining the agreement between the two instruments. This type of analysis should guide flight planning for future intercomparison efforts, whether for aircraft or satellite-borne instrumentation.

Sayres, D.S.↗

Measurements of the Ice Water Content of Cirrus in the Tropics and Subtropics: Instrument Details and Validation - I

We describe an instrument mounted in a pallet on the NASA WB-57 aircraft that is designed to measure the sum of gas phase and solid phase water, or total water, in cirrus clouds. Using an isokinetic inlet, a 600-watt heater mounted directly in the flow, and Lyman-alpha photofragment fluorescence technique for detection, accurate measurements of total water have been made over almost three orders of magnitude. Isokinetic flow is achieved with an actively controlled roots pump by referencing aircraft pressure, temperature, and true air speed, together with instrument flow velocity, temperature, and pressure. During CRYSTAL FACE, the instrument operated at duct temperatures sufficiently warm to completely evaporate particles up to 150 microns diameter. In flight diagnostics, intercomparison with water measured by absorption in flight, as well as intercomparisons in clear air with water vapor measured by the Harvard water vapor instrument and the JPL infrared tunable diode laser hygrometer validate the detection sensitivity of the instrument and illustrate minimal hysteresis from instrument surfaces. The simultaneous measurement of total water and water vapor in cirrus clouds yields their ice water content.

Weinstock, E. M.↗

Inorganic Chlorine Partitioning in the Summer Lower Stratosphere: Modeled and Measured [ClONO2/HCl] During POLARIS

We examine inorganic chlorine (Cly) partitioning in the summer lower stratosphere using in situ ER-2 aircraft observations made during the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) campaign. New steady state and numerical models estimate [ClONO2]/[HCl] using currently accepted photochemistry. These models are tightly constrained by observations with OH (parameterized as a function of solar zenith angle) substituting for modeled HO2 chemistry. We find that inorganic chlorine photochemistry alone overestimates observed [ClONO2]/[HCl] by approximately 55-60% at mid and high latitudes. On the basis of POLARIS studies of the inorganic chlorine budget, [ClO]/[ClONO2], and an intercomparison with balloon observations, the most direct explanation for the model-measurement discrepancy in Cly partitioning is an error in the reactions, rate constants, and measured species concentrations linking HCl and ClO (simulated [ClO]/[HCl] too high) in combination with a possible systematic error in the ER-2 ClONO2 measurement (too low). The high precision of our simulation (+/-15% 1-sigma for [ClONO2]/[HCl], which is compared with observations) increases confidence in the observations, photolysis calculations, and laboratory rate constants. These results, along with other findings, should lead to improvements in both the accuracy and precision of stratospheric photochemical models.

Voss, P. B.↗

The NO(x)-HNO3 System in the Lower Stratosphere: Insights from In Situ Measurements and Implications of the J(HNO3)-[OH] Relationship

During the 1997 Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) mission, simultaneous in situ observations of NOx and HOx radicals, their precursors, and the radiation field were obtained in the lower stratosphere. We use these observations to evaluate the primary mechanisms that control NOx-HNO3 exchange and to understand their control over the partitioning between NO2 and HNO3 in regions of continuous sunlight. We calculate NOx production (PNOx) and loss (LNOx) in a manner directly constrained by the in situ measurements and current rate constant recommendations, using approaches for representing albedo, overhead O3 and [OH] that reduce model uncertainty. We find a consistent discrepancy of 18% between modeled rates of NOx production and loss (LNOx = 1.18P(sub NOx)), which is within the measurement uncertainty of +/- 27%. The partitioning between NOx production processes is [HNO3 + OH (41 +/- 2)%; HNO3 + hv (59 +/- 2)%] and between NOx loss processes is [NO2 + OH, 90% to >97%; BrONO2 + H2O, 10% to <3%]. The steady-state description of NOx-HNO3 exchange reveals the significant influence of the tight correlation between the photolysis rate of HNO3 and [OH] established by in situ measurements throughout the lower stratosphere. Parametrizing this relationship, we find: (1) the steady-state value of [NO2](sub 24h-avg)/[HNO3] in the continuously sunlit, lower stratosphere is a function only of temperature and number density; and (2) the partitioning of NOx production between HNO3 + OH and HNO3 + hv is nearly constant throughout most of the lower stratosphere. We describe a methodology (functions of latitude, day, temperature, and pressure) for accurately predicting the steady-state value of [NO2](sub 24h-avg)/[HNO3] and the partitioning of NOx production within these regions. The results establish a metric to compare observations of [NO2](sub 24h-avg)/[HNO3] within the continuously sunlit region and provide a simple diagnostic for evaluating the accuracy of models that attempt to describe the coupled NOx-HOx photochemistry in the lower stratosphere.

Perkins, K. K.↗

Sources, Sinks, and the Distribution of OH in the Lower Stratosphere

Extensive measurement campaigns by the NASA ER-2 research aircraft have obtained a nearly pole-to-pole database of the species that control HOx (OH + HO2) chemistry. The wide dynamic range of these in situ measurements provides an opportunity to demonstrate empirically the mechanisms that control the HOx system. Measurements in the lower stratosphere show a remarkably tight correlation of OH concentration with the solar zenith angle (SZA). This correlation is nearly invariant over latitudes ranging from 70 S to 90 N and all seasons. An analysis of the production and loss of HOx in terms of the rate determining steps of reaction sequences developed by Johnston and Podolske and Johnston and Kinnison is used to clarify the behavior of the system and to directly test our understanding of the system with observations. Calculations using in situ measurements show that the production rate of HOx is proportional to O3 and ultraviolet radiation flux. The loss rate is proportional to the concentration and the partitioning of NOy (reactive nitrogen) and the concentration of HO2. In the absence of heterogeneous reactions, the partitioning of NOy is controlled by O3 and NOx and the concentration of HO2 is controlled by NOy and O3, so that the removal rate of OH is buffered against changes in the correlation of O3 and NOy. The heterogeneous conversion of NO2 to HNO3 is not an important net source of HO, because production and removal sequences are nearly balanced. Changes in NOy partitioning resulting from heterogeneous chemistry have a large effect on the loss rates of HOx, but little or no impact on the measured abundance of OH. The enhanced loss rates at high NO2/HNO3 are offset in the data set examined here by enhanced production rates resulting from increased photolysis rates resulting from the decreased O3 column above the ER-2.

Hanisco, T. F.↗

Establishing the Dependence of [HO2]/[OH] on Temperature, Halogen Loading, O3, and NO(x) Based on in Situ Measurements from the NASA ER-2

In situ observations of OH and HO2 from the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA), Stratospheric TRacers of Atmospheric Transport (STRAT), and Polar Ozone Loss in the Arctic Region in Summer (POLARIS) NASA ER-2 field campaigns are used to examine the partitioning of HO(x) in the lower stratosphere (tropopause to approx.21 km) and upper troposphere (approx.10 km to tropopause). These measurements span a latitude range from 70degS to 90degN and a variety of atmospheric conditions as a result of seasonal changes and altitude. The response of the observed [HO2]/[OH] to changes in temperature, [03], [CO], [NO], [CIO], and [BrO] is investigated. The measured ratio is accurately described (approx.+/-10%) by a steady-state model constrained by the measured mixing ratios of O3, CO, NO, CIO, and BrO, where the model is valid for conditions of HO(x) cycling much faster than HO(x) production and loss. The concentration of HO2 depends on [OH], which, to first order, has been observed to be a simple function of the solar zenith angle in the lower stratosphere. The partitioning between OH and HO2 is controlled by the local chemistry between the HO, radicals and O3, CO, NO, CIO, and BrO. The response of [HO(x)] to changes in [NO(x)] and [O3] is demonstrated. Further observations are necessary to illustrate the response of HO(x) to changes in halogen concentrations. A quantitative understanding of [HO2]/[OH] is important, since many of the reactions that control this ratio are directly involved in catalytic removal of O3 in the lower stratosphere and production of O3 in the upper troposphere.

Lanzendorf, E. J.↗

An Examination of the Inorganic Chlorine Budget in the Lower Stratosphere

We use the first simultaneous in situ measurements of ClONO2, ClO, and HCl acquired using the NASA ER-2 aircraft during the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) mission to test whether these three compounds quantitatively account for total inorganic chlorine (Cly) in the lower stratosphere in 1997. We find (ClO + ClONO2 + HCl)/Cly = 0.92 +/- 0.10, where Cly is inferred from in situ measurements of organic chlorine source gases. These observations are consistent with our current understanding of the budget and partitioning of Cly in the lower stratosphere. We find no evidence in support of missing inorganic chlorine species that compose a significant fraction of Cly. We apply the analysis to earlier ER-2 observations dating from 1991 to investigate possible causes of previously observed discrepancies in the inorganic chlorine budget. Using space shuttle, satellite, balloon, and aircraft measurements in combination with ER-2 data, we find that the discrepancy is unlikely to have been caused by missing chlorine species or an error in the photolysis rate of chlorine nitrate. We also find that HCl/Cly is not significantly controlled by aerosol surface area density in the lower stratosphere.

Bonne, G. P.↗

Simulating Observed Ozone Loss in the Northern Hemisphere Winter

Ozone amounts observed at high Northern latitudes in late winter and early spring have been relatively very low in four of the last six years. On the face of it, this decline appears similar to that observed in the Antarctic in the mid-1980s in spite of the fact that the abundance of stratospheric chlorine is currently steady or decreasing. In order to predict the extent to which this change represents a trend, and to understand what combination of factors produces the low ozone, we need to accurately simulate these observations with models. In this presentation, we focus on the winter of 1999-2000, which exhibited some of the lowest ozone ever recorded in the Northern hemisphere. It also contained the largest-ever assembled set of atmospheric measurements and modeling activities in the SAGE III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone (SOLVE/THESEO). We use SOLVE/THESEO observations in comparison with the Goddard 3-D global model of stratospheric chemistry and transport to explore the model's capability to simulate the evolution of ozone and other species through the winter. We will discuss advective transport and mixing, chlorine activation, and denitrification, which are key processes to accurately simulating wintertime ozone. Preliminary results show that, although the model tracer transport and chlorine activation compare relatively well with observations, the magnitude of observed ozone loss is difficult to achieve in the model. Calculated ozone loss is sensitive to denitrification, which presents a major challenge to parameterization in a global model. Simulation requirements and uncertainties will be evaluated.

Kawa, S. R.↗

The Coupling of ClONO2, ClO, and NO2 in the Lower Stratosphere From in Situ Observations Using the NASA ER-2 Aircraft

The first in situ measurements of ClONO2 in the lower stratosphere, acquired using the NASA ER-2 aircraft during the Polar Ozone Loss in the Arctic Region in Summer (POLARIS) mission, are combined with simultaneous measurements of ClO, NO2, temperature, pressure, and the calculated photolysis rate coefficient (J(sub ClONO2)) to examine the balance between production and loss of ClONO2. The observations demonstrate the ClONO2 photochemical steady state measurement, [ClONO2](sup PSS) = k[ClO][No2]/J(sub ClONO2), is in good agreement with the direct measurement, [ClONO2](sup MEAS). For the bulk of the data (80%), where T > 220 K and latitudes > 45 N, [ClONO2](sup PPS) = 1.15 +/- 0.36(1-sigma)[ClONO2](sup MEAS), while for T< 220 K and latitudes < 45 N, the result is somewhat less at 1.01 +/- 0.30. The cause of the temperature and/or latitude trend is unidentified. These results are independent of solar zenith angle and air density, thus there is no evidence in support of a pressure-dependent quantum yield for photodissociation of ClONO2 at wavelengths > 300 nm. These measurements confirm the mechanism by which active nitrogen (NOx = NO + NO2) controls the abundance of active chlorine (Clx = ClO + Cl) in the stratosphere.

Stimpfle, R. E.↗

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta about 330-380 K near 40N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta =352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. while most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta <362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta-330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta=352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta<362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O, and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta approximately 330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta = 352-364 K. Temperatures on the 355 K surface 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta < 362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta = 330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta = 352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta < 362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Hintsa, E. J.↗