Search

The SU(1,1) interferometer was originally conceived as a Mach-Zehnder interferometer with the beam-splitters replaced by parametric amplifiers. The parametric amplifiers produce states with correlations that result in enhanced phase sensitivity. $F=1$ spinor Bose-Einstein condensates (BECs) can serve as the parametric amplifiers for an atomic version of such an interferometer by collisionally producing entangled pairs of $\left

A unique dataset of airborne in situ observations of HCl, O3, HNO3, H2O, CO, CO2 and CH3Cl has been made in and near the tropical tropopause layer (TTL). A total of 16 profiles across the tropopause were obtained at latitudes between 10degN and 3degs from the NASA WB-57F high-altitude aircraft flying from Costa Rica. Few in situ measurements of these gases, particularly HCl and HNO3, have been reported for the TTL. The general features of the trace gas vertical profiles are consistent with the concept of the TTL as distinct from the lower troposphere and lower stratosphere. A combination of the tracer profiles and correlations with O3 is used to show that a measurable amount of stratospheric air is mixed into this region. The HCl measurements offer an important constraint on stratospheric mixing into the TTL because once the contribution from halocarbon decomposition is quantified, the remaining HCl (>60% in this study) must have a stratospheric source. Stratospheric HCl in the TTL brings with it a proportional amount of stratospheric O3. Quantifying the sources of O3 in the TTL is important because O3 is particularly effective as a greenhouse gas in the tropopause region.

In situ observations in a tropical subvisible cirrus cloud during the Costa Rica Aura Validation Experiment on 2 February 2006 show the presence of condensed-phase nitric acid. The cloud was observed near the tropopause at altitudes of 16.3-17.7 km in an extremely cold (183-191 K) and dry 5 ppm H2O) air mass. Relative humidities with respect to ice ranged from 150-250% throughout most of the cloud. Optical particle measurements indicate the presence of ice crystals as large as 90 microns in diameter. Condensed RN031H20 molar ratios observed in the cloud particles were 1-2 orders of magnitude greater than ratios observed previously in cirrus clouds at similar RN03 partial pressures. Nitric acid trihydrate saturation ratios were 10 or greater during much of the cloud encounter, indicating that RN03 may be present in the cloud particles as a stable condensate and not simply physically adsorbed on or trapped in the particles.

Large (5 to >20 micron diameter) nitric-acid-containing polar stratospheric cloud (PSC) particles were observed in the Arctic stratosphere during the winter of 1999-2000. We use a particle growth and sedimentation model to investigate the environment in which these particles grew and the likely phase of the largest particles. Particle trajectory calculations show that, while simulated nitric acid dihydrate (NAD) particle sizes are significantly smaller than the observed maximum particle sizes, nitric acid trihydrate (NAT) particle trajectories are consistent with the largest observed particle sizes.

Extensive airborne measurements of the reactive nitrogen reservoir (NOY) and its component nitric oxide (NO) have been made in the lower stratosphere. Box model. simulations that are constrained by observations of radical and longlived species and which include heterogeneous chemistry systematically underpredict the NO(x) (= NO + NO2) to NOY ratio. The model agreement is substantially improved if newly measured rate coefficients for the OH + NO2 and OH + HNO3 reactions are used. When included in 2-D models, the new rate coefficients significantly increase the calculated ozone loss due to NO(x) and modestly change the calculated ozone abundances in the lower stratosphere. Ozone changes associated with the emissions of a fleet of supersonic aircraft are also altered. phase chemistry linking NO(x) and nitric acid (HNO3), which is generally the most abundant NOY species. Because the continuous daylight present at summer high latitudes limits the heterogeneous production of HNO3 by N2O5 hydrolysis, gas-phase reactions primarily control the balance between NO(x) and NO(y). Outside summer polar regions, the N2O5 hydrolysis reaction occurring on stratospheric sulfate aerosols is a more important sink of NO(x), particularly in the lower stratosphere during winter when heterogeneous pathways account for most of the HNO3 production.

Measurements of the ratio OH/HO2, NO, O3, ClO, and BrO were obtained at altitudes from 15-20 km and latitudes from 15-60 deg N. A method is presented for interpreting the rates of chemical transformations that (1) are responsible for over half the ozone removal rate in the lower stratosphere via reactions of HO2; and (2) control the abundance of HO2 through coupling to nitrogen and halogen radicals. The results show our understanding of the chemical reactions controlling the partitioning of OH and HO2 is complete and accurate and that the potential effects of 'missing chemistry' are strickly constrained in the region of the atmosphere encompassed by the observations. The analysis demonstrates that the sensitivity of the ratio OH/HO2 to changes in NO is described to within 12% by current models. This reduces by more than a factor of 2 the effect of uncertainty in the coupling of hydrogen and nitrogen radicals on the analysis of the potential effects of perturbations to odd notrogen in the lower statosphere.

In situ measurements of hydrogen, nitrogen, and chlorine radicals obtained in the lower statosphere during SPADE are compared to results from a photochemical model that assimilates measurements of radical precursors and environmental conditions. Models allowing for heterogeneous hydrolysis of N2O5 agree well with measured concentrations of NO and ClO, but concentrations of HO2 and OH are underestimated by 10 to 25%, concentrations of NO2 are overestimated by 10 to 30%, and concentrations of HCl are overestimated by a factor of 2. Discrepancies for (OH) and (HO2) are reduced if we allow for higher yields of O((1)D) from O2 photolysis and for heterogeneous production of HNO2. The data suggest more efficent catalytic removal of O3 by hydrogen and halogen radicals relative to nitrogen oxide radicals than predicted by models using recommendend rates and cross sections. Increased in (O3) in the lower stratosphere may be larger in response to inputs of NO(y) from supersonic aircraft than estimated by current assessment 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.

Back trajectory analysis of Arctic and Antarctic aircraft data reveals that high ClO concentrations are associated with predicted polar stratospheric cloud (PSCs) encounters. The ClO concentrations within the Arctic and Antarctic polar vortices vary widely but appear to be inversely related to parcel solar exposure since the last PSC interaction. These results imply that production of NO(x) from HNO3 photolysis and reaction with OH is the mechanism for the loss of chlorine radicals through the reformation of chlorine nitrate. Highly denitrified air parcels show no change in ClO with solar exposure. The recovery process is quantitatively duplicated using a model of chemistry along trajectories. Although PSC processing is the primary mechanism for producing elevated ClO amounts, back trajectories apparently unperturbed by PSC's also show slightly elevated ClO levels in 1992 compared to Arctic 1989 and Antarctic 1987 measurements presumably due to the presence of Pinatubo aerosol.

A mountain wave event, observed at the southern tip of Greenland on January 6, 1992, was corroborated by three experiments: the Meteorological Measurement System (MMS), the Microwave Temperature Profiler (MTP), and the Reactive Nitrogen Instrument (NO/NO(y)). Gravity wave signatures with classical phase relationship between wind and temperature were observed on both the outbound and inbound legs at different altitudes. The waves showed both vertically propagating and evanescent properties. Characteristics of the dominant wave mode are: wavelength about = 35 km; vertical displacement about = 0.8 km, and peak-to-peak vertical wind about = 6/ms. With the prevailing wind at about = 37/ms, the stratospheric temperature was reduced by 6K to 195.5 K within 8 minutes. The implication and potential impact of mountain lee waves on the formation of polar stratospheric clouds (PSC's) are discussed.

During the Airborne Arctic Stratospheric Expedition 2 (AASE 2), September 1991 through March 1992, in situ measurements of reactive nitrogen (NO(y) and N20 were made in the Northern Hemisphere lower stratosphere. We present an analysis of this new data and compare it with results from similar data taken during AASE in the winter of 1989. In the Northern Hemisphere there is consistent linear correlation of N2O and NO(y) which shows no interannual variation. Cases of departure from a linear correlation are examined and classified as being due to denitrification (NO(y) loss) or sampling air from a region where the photochemical lifetime of NO(y) is decreased. The latter case was observed for the first time in the winter of 1992.

In situ measurements of NO and NO(y) are used to derive the ratio NO(x)/NO(y) along the flight track of the NASA ER-2 aircraft. Data are presented for two flights at midlatitudes in October 1991 during the Airborne Arctic Stratospheric Expedition-2 (AASE-2). Aerosol particle surface area was concurrently measured. The observations are compared with a photochemical model integrated along back trajectories from the aircraft flight track. Comparison of observations with the model run along trajectories and at a fixed position clearly and quantitatively demonstrates the importance of an air parcel's dynamic history in interpretation of local chemical observations. Comparison of the data with model runs under different assumptions regarding heterogeneous chemistry further reinforces the case for occurrence of the reaction of N2O5 + H2O on sulfate aerosol surfaces in the atmosphere. Finally, comparisons for which relative changes in the model and the data are not consistent caution that our ability to resolve all the observations is not yet complete.

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.

The pairwise correlation of NO(y) and N2O data from the Southern and Northern Hemispheres is presented. Both data sets show a linear correlation region, defined as a reference state, and regions of denitrification where the correlation breaks down. Using two-dimensional photochemical model simulations of the atmosphere, a similar linear correlation is found between NO(y) and N2O, thereby establishing a theoretical framework for the reference state. This general approach, which can be extended to other pairs of molecules, should prove to be powerful in further comparisons of aircraft data with numerical models.

It is argued that denitrification of the Arctic stratosphere can be explained by the selective growth and sedimentation of aerosol particles rich in nitric acid. Because reactive nitrogen species moderate the destruction of ozone by chlorine-catalyzed reactions by sequestering chlorine in reservoir species such as ClONO2, the possibility of the removal of reactive nitrogen without dehydration should be allowed for in attempts to model ozone depletion in the Arctic. Indeed, denitrification along with elevated concentrations of reactive chlorine observed in 1989 indicate that the Arctic was chemically primed for ozone destruction without an extended period of temperatures below the frost point, as is characteristic of the Antarctic.

Composite distributions of measured total reactive nitrogen NO(y), from the NASA ER-2 during the Airborne Arctic Stratospheric Expedition are presented. The observed features of these distributions are discussed in terms of the controlling dynamical, chemical and microphysical processes. In the latitudinal profile from 58 deg N to within about 4 deg poleward of the polar vortex boundary, NO(y) conforms closely to predictions of NO(y) based on N2O measurements. Poleward of 5 deg of latitude within the boundary, the average NO(y) decreases sharply and is significantly lower than that predicted from N2O. This feature is consistent with loss of NO(y) through sedimentation of particles containing NO(y) in polar stratospheric clouds.

Calculations of ozone depletion during the 1988/89 Arctic winter using a Lagrangian coupled photochemical-microphysical model are presented. Abundances of ClO in excess of 1 ppbv were observed at the end of the Airborne Arctic Stratospheric Expedition on February 10, 1989. These are shown to be consistent with the removal of more than 90 percent of the reactive nitrogen and the conversion of more than 80 percent of reservoir chlorine to active forms. This chemical state implies that ozone losses of more than 20 ppbv/day can be sustained in heavily denitrified air throughout much of February according to current photochemistry. As much as 74 percent of the loss is calculated to be due to ClO dimer photolysis. Following the warming of the vortex in mid-February 1989, ozone loss through ClO dimer photolysis becomes less effective as the rate of thermal decomposition of the ClO dimer increases. Thus, model results suggest that thermal decomposition of the dimer plays an important role in limiting ozone loss in the Arctic spring.