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At least 55 records · Page 3

In-Situ Measurements of HCN and CH3CN in the Pacific Troposphere: Sources, Sinks, and Comparisons with Spectroscopic Observations

We report the first in-situ measurements of hydrogen cyanide (HCN) and acetonitrile (CH3CN) from the Pacific troposphere (0-12 km) obtained during the NASA/Trace-P mission (Feb.-April, 2001). Mean HCN and CH3CN mixing ratios of 243 (+/-118) ppt and 149 (+/-56) ppt respectively, were measured. The in-situ observations correspond to a total HCN column of 4.4-4.9 x 10(exp 15) molec. cm(exp -2) and a CH3CN column of 2.8-3.0 x 10(exp 15) molec. cm(exp -2). This HCN column is in good agreement with available spectroscopic observations. The atmospheric concentrations of HCN and CH3CN were greatly influenced by outflow of pollution from Asia. There is a linear relationship between the mixing ratios of HCN and CH3CN, and in turn these are well correlated with tracers of biomass combustion (e.g. CH3Cl, CO). Relative enhancements with respect to known tracers of biomass combustion within selected plumes in the free troposphere, and pollution episodes in the boundary layer allow an estimation of a global biomass burning source of 0.8+/-0.4 Tg (N)/y for HCN and 0.4+/-0.1 Tg (N)/y for CH3CN. In comparison, emissions from automobiles and industry are quite small (<0.05 Tg (N)/y). The vertical structure of HCN and CH3CN indicated reduced mixing ratios in the MBL (Marine Boundary Layer). Using, a simple box model, the observed gradients across the top of the MBL are used to derive an oceanic flux of 6.7 x 10(exp -15) g (N) cm(exp -2)/s for HCN and 4.8 x 10(exp -15) g (N) cm(exp -2)/s for CH3CN. An air-sea exchange model is used to conclude that this flux can be maintained if the oceans are under-saturated in HCN and CH3CN by 23% and 17%, respectively. It is inferred that oceanic loss is a dominant sink for these nitrites, and they deposit some 1.3 Tg (N) of nitrogen annually to the oceans. Assuming reaction with OH radicals and loss to the oceans as the major removal processes, a mean atmospheric residence time of 4.7 months for HCN and 5.1 months for CH3CN is calculated. A global budget analysis shows that the sources and sinks of HCN and CH3CN are roughly in balance. There are indications that biogenic sources may also be present. Mechanisms involved in nitrate formation during combustion and removal in the oceans are poorly understood.

Singh, Hanwant B.↗

Meteorological variations in the middle clouds of Venus from Vega balloon in situ measurements

Instruments aboard the gondolas of the two Vega balloons obtained in situ measurements of pressure, temperature, vertical velocity relative to the balloon, cloud particle backscatter, lightning and the ambient light level. Atmospheric motions at the balloon float altitudes were also determined from earth-based tracking results. To illustrate the history of the balloon flights and to facilitate comparisons between some of the different observed quantities, measurements of pressure, temperature and backscatter are presented as time series for the entire lifetime of each balloon. Both long and short period variations have been detected. In addition, the environmental entropy encountered by each balloon will be discussed.

Elson, Lee S.↗

In situ measurements of the NO2/NO ratio for testing atmospheric photochemical models

Simultaneous in situ measurements of NO2, NO, O3, ClO, pressure and temperature have been made for the first time, presenting a unique opportunity to test our current understanding of the photochemistry of the lower stratospere. Data were collected from several flights of the ER-2 aircraft at mid-latitudes in May 1993 during NASA's Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE). The daytime ratio of NO2/NO remains fairly constant at 19 km with a typical value of 0.68 and standard deviation of +/- 17. The ratio observations are compared with simple steady-state calculations based on laboratory-measured reaction rates and modeled NO2 photolysis rates. At each measurement point the daytime NO2/NO with its measurements uncertainty overlap the results of steady-state caculations and associated uncertainty. Possible sources of error are examined in both model and measurements. It is shown that more accurate laboratory determinations of the NO + 03 reaction rate and of the NO2 cross-sections in the 200-220 K temperature range characteristic of the lower stratosphere would allow for a more robust test of our knowledge of NO(X) phtochemistry by reducing significant sources if uncertainties in the interpretation of statospheric measurements.

Jaegle, L.↗

In Situ Measurements of the NO2/NO Ratio for Testing Atmospheric Photochemical Models

Simultaneous in situ measurements of NO2, NO, O3, ClO, pressure and temperature have been made for the first time, presenting a unique opportunity to test our current understanding of the photochemistry of the lower stratosphere. Data were collected from several flights of the ER-2 aircraft at mid-latitudes in May 1993 during NASA's Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE). The daytime ratio of NO2/NO remains fairly constant at 19 km with a typical value of 0.68 and standard deviation of +/- 0.17. The ratio observations are compared with simple steady-state calculations based on laboratory-measured reaction rates and modeled NO2 photolysis rates. At each measurement point the daytime NO2/NO with its measurement uncertainty overlap the results of steady-state calculations and associated uncertainty. However, over all the ER-2 flights examined, the model systematically overestimates the ratio by 40% on average. Possible sources of error are examined in both model and measurements. It is shown that more accurate laboratory determinations of the NO + O3 reaction rate and of the NO2 cross-sections in the 200-220 K temperature range characteristic of the lower stratosphere would allow for a more robust test of our knowledge of NO(x) photochemistry by reducing significant sources of uncertainties in the interpretation of stratospheric measurements. The present measurements are compared with earlier observations of the ratio at higher altitudes.

Jaegle, L.↗

In situ measurements constraining the role of sulphate aerosols in mid-latitude ozone depletion

In situ measurements of stratospheric sulphate aerosol, reactive nitrogen and chlorine concentrations at middle latitudes confirm the importance of aerosol surface reactions that convert active nitrogen to a less active, reservoir form. This makes mid-latitude stratospheric ozone less vulnerable to active nitrogen and more vulnerable to chlorine species. The effect of aerosol reactions on active nitrogen depends on gas phase reaction rates, so that increases in aerosol concentration following volcanic eruptions will have only a limited effect on ozone depletion at these latitudes.

Fahey, D. W.↗

Simultaneous in situ measurements and diurnal variations of NO, NO2, O3, jNO2, CH4, H2O, and CO2 in the 40- to 26-km region using an open path tunable diode laser spectrometer

Simultaneous in situ measurements of temperature, pressure, and the NO, NO2, O3, jNO2, CH4, H2O, and CO2 concentrations were conducted in the 40- to 26-km region of the stratosphere using the JPL Balloon-borne Laser In Situ Sensor, a tunable diode laser absorption spectrometer. The NO, NO2, CH4, H2O, and CO2 concentration measurements generally show good agreement with previous observations, with a tendency for somewhat lower NO2 amounts. Measured O3 concentrations at 38 km agree well with comparable measurements from in situ UV photometers, but at 28 km they are lower by about 10 percent and agree more closely with the solar backscattered UV data. A decline was found in NO2 during the night over a 5-km altitude range, which implies either lower NO2 postsunset profiles, or an NO2 decay rate that is significantly higher than current model predictions that use N2O5 chemistry.

Webster, Christopher R.↗

Estimating Total Heliospheric Magnetic Flux from Single-Point in Situ Measurements

A fraction of the total photospheric magnetic flux opens to the heliosphere to form the interplanetary magnetic field carried by the solar wind. While this open flux is critical to our understanding of the generation and evolution of the solar magnetic field, direct measurements are generally limited to single-point measurements taken in situ by heliospheric spacecraft. An observed latitude invariance in the radial component of the magnetic field suggests that extrapolation from such single-point measurements to total heliospheric magnetic flux is possible. In this study we test this assumption using estimates of total heliospheric flux from well-separated heliospheric spacecraft and conclude that single-point measurements are indeed adequate proxies for the total heliospheric magnetic flux, though care must be taken when comparing flux estimates from data collected at different heliocentric distances.

Owens, M. J.↗

In Situ Measurements of Ammonia In Plumes Emitted From Wildfires And Agricultural Fires in the US

Emissions of trace gases and particles from fires have a major impact on climate, visibility, air quality, and public health. Biomass burning emissions include reactive nitrogen gases, among which ammonia (NH3) plays a prominent role. NH3 is a short-lived gas that acts as precursor for secondary inorganic aerosols. This process is still poorly constrained in downwind fire plumes. In summer 2019, NASA and NOAA carried out the joint airborne FIREX-AQ (Fire Influence on Regional to global Environments and Air Quality) mission over the continental US to sample plumes from wildfires and agricultural fires. On board the NASA DC-8, we used a modified PTR-ToF-MS instrument for measuring NH3 in situ and at high time resolution. Over the course of the mission, we collected a large set of NH3 data in plumes emitted from fires differing in fuel type and burning stage. Herein, we will present the measured NH3 emissions ratios and factors, compare them with the literature, and investigate the dependence of NH3 emissions on fuel type and burning conditions.

ammonia↗

In situ measurements of the mesosphere and stratosphere

The operation of a subsonic, Gerdien condenser probe for in situ measurements of the mesosphere and stratosphere is presented. The inclusion of a flashing Lyman alpha ultraviolet source provides an artifically produced ionization of particular constituents. Detailed theory of operation is presented and the data results from two flights are shown. A great deal of fine structure in mobility is observed due to the presence of various hydrated positive ions. The effect of the Lyman alpha source in the 35 km region was to dissociate a light hydrate ion rather than produce additional ionization. At the 70 km region, photodissociation of the heaviest ions (probably ice crystals) was also observed.

Crosky, C.↗

Indicators of transport and vertical motion from correlations between in situ measurements in the Airborne Antarctic Ozone Experiment

Analysis of small-scale structure in the in situ measurements made from the ER-2 during the Airborne Antarctic Ozone Experiment shows the existence of a region at the boundary of the chemiclly perturbed region where the mixing ratios and small-scale structure of trace gases are influenced by transport across the boundary. This transition region is characterized by horizontal interchange and vertical layering of air parcels from within and outside of the chemically perturbed region and negative small-scale correlations between ClO and ozone. The horizontal transport in this region creates large surface areas between dissimilar air masses, providing the potential for substantial mixing. Correlations between ClO and O3 show that the transition region extends to 2-4 deg of latitude to either side of the boundary of the chemically perturbed region. A + or - 4-deg-wide transition region would contain nearly as much air as the chemically perturbed region proper. Analysis of water vapor and nitrous oxide data suggests that diabatic descent is associated with dehydration. This could be caused by strong radiative cooling of those polar stratospheric clouds in which enough water condenses for the particles to fall and dehydrate the air.

Murphy, D. M.↗

In situ measurement of water vapor in the stratosphere with a cryogenically cooled Lyman-alpha hygrometer

In situ measurements of water vapor in the stratosphere with a new instrument are reported. The instrument has been designed to observe daytime water vapor from a multiinstrument balloon gondola that simultaneously measures free radicals such as OH, HO2, and O3 in the stratosphere up to 40 km. Lyman-alpha photofragment fluorescence is used to measure water molecules in a flowing sample of ambient air. A brief description of the instrument is given, followed by the results of the first four balloon flights. The measured mixing ratio for this flight varies from 3.0-5.5 ppmv over the altitude range of 17-34 km. Adjustments in the cooling protocol for the flights of July 6, 1988, July 28, and August 25, 1989, result in a much higher signal-to-noise ratio. Profiles from these three flights are similar to, but somewhat higher, than the 1987 profile. Implications of measurements are discussed, as are the issues of short- and long-term variability of stratospheric water vapor.

Schwab, J. J.↗

Balloon-borne in situ measurements of ClO and ozone - Implications for heterogeneous chemistry and mid-latitude ozone loss

In situ measurements of chlorine oxide (ClO) obtained on 31 March 1991 with a new balloon-borne instrument are compared to results from a photochemical model which incorporates hydrolysis of N2O5 on sulfate aerosols. With the addition of this process, there is better agreement between calculation and measurement over most of the profile, except below 20 km where observed ClO is greater by as much as a factor of four. In a model which is constrained to reproduce the observed ClO below 20 km, ozone loss by catalytic cycles involving halogen oxides becomes larger than that from NO(x), which would dominate under gas-phase or standard heterogeneous conditions.

Avallone, L. M.↗

In situ measurements of the ClO/HCl ratio: Heterogeneous processing on sulfate aerosols and polar stratospheric clouds

Simultaneous in situ measurements of stratospheric ClO and HCl have been made for the first time, during numerous flights of the ER-2 aircraft covering latitudes 24-90 deg N from October 1991 through March 1992. The ClO/HCl ratio is identified as a key indicator of heterogeneous processing both outside and within the Arctic polar vortex. For ClO mixing ratios below about 120 pptv, remarkably constant ClO/HCl values of about 15% characterize the lower stratosphere. The observed values are significantly higher than those derived from a 2-D model using either gas phase photochemistry alone (2%), or including heterogeneous sulfate chemistry (5-10%). During the Arctic early spring, after conversion of HCl into reactive chlorine has taken place, the vortex edge is poorly defined by ClO levels. Loss of HCl and its slow recovery following low-temperature polar heterogeneous chemistry distinguishes HCl as a new and unique dynamical tracer of polar stratospheric clouds (PSC)-processed air.

Webster, C. R.↗

In Situ Measurements of the ClO/HCl Ratio: Heterogeneous Processing on Sulfate Aerosols and Polar Stratospheric Clouds

Simultaneous in situ measurements of stratospheric ClO and HCl have been made for the first time, during numerous flights of the ER-2 aircraft covering latitudes 24-90 deg. N from October 1991 through March 1992. The ClO/HCl ratio is identified as a key indicator of heterogeneous processing both outside and within the Arctic polar vortex. For ClO mixing ratios below about 120 pptv, remarkably constant ClO/HCl values of about 15% characterize the lower stratosphere. The observed values are significantly higher than those derived from a 2-D model using either gas phase photochemistry alone (2%), or including heterogeneous sulfate chemistry (5-10%). During the Arctic early spring, after conversion of HCl into reactive chlorine has taken place, the vortex edge is poorly defined by ClO levels. Loss of HCl and its slow recovery following low-temperature polar heterogeneous chemistry distinguishes HCl as a new and unique dynamical tracer of PSC-processed air.

Webster, C. R.↗

In Situ Measurements of the ClO/HCl Ratio: Heterogeneous Processing on Sulfate Aerosols and Polar Stratospheric Clouds

Simultaneous in situ measurements of stratospheric ClO and HCl have been made for the first time, during numerous flights of the ER-2 aircraft covering latitudes 24-90 deg N from October 1991 through March 1992. The ClO/HCl ratio is identified as a key indicator of heterogeneous processing both outside and within the Arctic polar vortex. For ClO mixing ratios below about 120 pptv, remarkably constant ClO/HCl values of about 15% characterize the lower stratosphere. The observed values are significantly higher than those derived from a 2-D model using either gas phase photochemistry alone (2%), or including heterogeneous sulfate chemistry (5-10%). During the Arctic early spring, after conversion of HCl into reactive chlorine has taken place, the vortex edge is poorly defined by ClO levels. Loss of HCl and its slow recovery following low-temperature polar heterogeneous chemistry distinguishes HCl as a new and unique dynamical tracer of PSC-processed air.

Webster, C. R.↗

A Novel Instrument and Methodology for the In-Situ Measurement of the Stress in Thin Films

We introduce a novel methodology for the in-situ measurement of mechanical stress during thin film growth utilizing a highly sensitive non-contact variation of the classic spherometer. By exploiting the known spherical deformation of the substrate the value of the stress induced curvature is inferred by measurement of only one point on the substrate's surface-the sagittal. From the known curvature the stress can be calculated using the well-known Stoney equation. Based on this methodology, a stress sensor has been designed which is simple, highly sensitive, compact, and low cost. As a result of its compact nature, the sensor can be mounted in any orientation to accommodate a given deposition geometry without the need for extensive modification to an already existing deposition system. The technique employs the use of a double side polished substrate that offers good specular reflectivity and is isotropic in its mechanical properties, such as <111> oriented crystalline silicon or amorphous soda lime glass, for example. The measurement of the displacement of the uncoated side during deposition is performed with a high resolution (i.e. 5nm), commercially available, inexpensive, fiber optic sensor which can be used in both high vacuum and high temperature environments (i.e. 10(exp-7) Torr and 480oC, respectively). A key attribute of this instrument lies in its potential to achieve sensitivity that rivals other measurement techniques such as the micro cantilever method but, due to the comparatively larger substrate area, offers a more robust and practical alternative for subsequent measurement of additional characteristics of the film that can might be correlated to film stress. We present measurement results of nickel films deposited by magnetron sputtering which show good qualitative agreement to the know behavior of polycrystalline films previously reported by Hoffman.

Broadway, David M.↗

Quantifying the Impacts of PM2.5 Constituents and Relative Humidity on Visibility Impairment in a Suburban Area of Eastern Asia Using Long-Term In-Situ Measurements.

The deterioration of visibility due to air pollutants and relative humidity has been a serious environmental problem in eastern Asia. In most previous studies, chemical compositions of atmospheric particles were provided using filter-based offline analyses, which were unable to provide long-term and in-situ measurements that resolve sufficient temporal variations of air pollution and meteorology, hindering the resolution of the relationship between air quality and visibility. Here, we present a year-long continuously measured data from a comprehensive suite of online instruments to investigate diurnal and seasonal impacts of the aerosol chemical compositions in PM2.5 on visibility seasonally and diurnally. The measured dry aerosol extinction at λ = 550 nm reached a closure with that predicted by aerosol compositions within 12%. However, the hygroscopic growth of particles under ambient RH could enhance the aerosol extinction by a factor of 2 – 6, matching the perceptive visibility of the public. Particulate ammonium nitrate was most sensitive to reducing visibility, while ammonium sulfate contributed the most to the light extinction. In spring and winter, the monsoon and stagnant air masses reduced the visibility and increased PM2.5 (> 35 μg m-3).The moisture was found to substantially enhance the light extinction under RH = 60 – 90%,reducing visibility by approximately 15 km, largely attributed to hygroscopic inorganic salts.This study serves as a metric to highlight the need to consider the influence of RH, and aqueous reactions in producing secondary inorganic aerosols on atmospheric visibility, underpinning the more accurate mitigation strategies of air pollution.

visibility↗