This work describes the development and testing of a new instrument for in situ measurements of sulfur dioxide (SO2) on airborne platforms in the upper troposphere and lower stratosphere (UTLS). The ...instrument is based on the laser-induced fluorescence technique and uses the fifth harmonic of a tunable fiber-amplified semiconductor diode laser system at 1084.5 nm to excite SO2 at 216.9 nm. Sensitivity and background checks are achieved in flight by additions of SO2 calibration gas and zero air, respectively. Aircraft demonstration was performed during the NASA Volcano Plume Investigation Readiness and Gas-Phase and Aerosol Sulfur (VIRGAS) experiment, which was a series of flights using the NASA WB-57F during October 2015 based at Ellington Field and Harlingen, Texas. During these flights, the instrument successfully measured SO2 in the UTLS at background (non-volcanic) conditions with a precision of 2 ppt at 10 s and an overall uncertainty determined primarily by instrument drifts of +/- (16% + 0.9 ppt).
This work describes aircraft‐based lidar observations of thin cirrus clouds at the tropical tropopause in the central Pacific obtained during the Tropical Ozone Transport Experiment/Vortex Ozone ...Transport Experiment (TOTE/VOTE) in December 1995 and February 1996. Thin cirrus clouds were found at the tropopause on each of the four flights which penetrated within 15° of the equator at 200–210 east longitude. South of 15°N, thin cirrus were detected above the aircraft about 65% of the time that data were available. The altitudes of these clouds exceeded 18 km at times. The cirrus observations could be divided into two basic types: thin quasi‐laminar wisps and thicker, more textured structures. On the basis of trajectory analyses and temperature histories, these two types were usually formed respectively by (1) in situ cooling on both a synoptic scale and mesoscale and (2) recent (a few days) outflow from convection. There is evidence from one case that the thicker clouds can also be formed by in situ cooling. The actual presence or absence of thin cirrus clouds was also consistent with the temperature and convective histories derived from back trajectory calculations. Notably, at any given time, only a relatively small portion (at most 25%) of the west central tropical Pacific has been influenced by convection within the previous 10 days. The structures of some of the thin cirrus clouds formed in situ strongly resembled long‐wavelength (500–1000 km) gravity waves observed nearly simultaneously by the ER‐2 on one of the flights. Comparison with in situ water vapor profiles made by the NASA ER‐2 aircraft provide some observational support for the hypothesis that thin cirrus clouds play an important role in dehydrating tropospheric air as it enters the stratosphere.
Cloud condensation nuclei (CCN) can affect cloud properties and therefore the Earth’s radiative balance. New particle formation (NPF) from condensable vapours in the free troposphere has been ...suggested to contribute to CCN, especially in remote, pristine atmospheric regions, but direct evidence is sparse, and the magnitude of this contribution is uncertain. Here we use in-situ aircraft measurements of vertical profiles of aerosol size distributions to present a global-scale survey of NPF occurrence. We observed intense NPF occurring at high altitude in tropical convective regions over both the Pacific and Atlantic Oceans. Together with the results of chemical-transport models, our findings indicate that NPF persists at all longitudes as a global-scale band in the tropical upper troposphere, covering about 40% of the Earth’s surface. Furthermore, we find that this NPF in the tropical upper troposphere is a globally important source of CCN in the lower troposphere, where they can affect cloud properties. Our findings suggest that the production of CCN, as these new particles descend towards the surface, is currently not adequately captured in global models, because they tend to underestimate both the magnitude of tropical upper tropospheric NPF and the subsequent growth to CCN sizes. This has potential implications for cloud albedo and the global radiative balance.
In this study, we explore observational, experimental, methodological, and practical aspects of the flux quantification of greenhouse gases from local point sources by using in situ airborne ...observations, and suggest a series of conceptual changes to improve flux estimates. We address the major sources of uncertainty reported in previous studies by modifying (1) the shape of the typical flight path, (2) the modeling of covariance and anisotropy, and (3) the type of interpolation tools used. We show that a cylindrical flight profile offers considerable advantages compared to traditional profiles collected as curtains, although this new approach brings with it the need for a more comprehensive subsequent analysis. The proposed flight pattern design does not require prior knowledge of wind direction and allows for the derivation of an ad hoc empirical correction factor to partially alleviate errors resulting from interpolation and measurement inaccuracies. The modified approach is applied to a use-case for quantifying CH4 emission from an oil field south of San Ardo, CA, and compared to a bottom-up CH4 emission estimate.
The spatial distribution of relative humidity with respect to ice (RHI) in the boreal wintertime tropical tropopause layer (TTL, is asymptotically Equal to 14-18 km) over the Pacific is examined with ...the measurements provided by the NASA Airborne Tropical TRopopause EXperiment. We also compare the measured RHI distributions with results from a transport and microphysical model driven by meteorological analysis fields. Notable features in the distribution of RHI versus temperature and longitude include (1) the common occurrence of RHI values near ice saturation over the western Pacific in the lower to middle TTL; (2) low RHI values in the lower TTL over the central and eastern Pacific; (3) common occurrence of RHI values following a constant mixing ratio in the middle to upper TTL (temperatures between 190 and 200 K); (4) RHI values typically near ice saturation in the coldest airmasses sampled; and (5) RHI values typically near 100% across the TTL temperature range in air parcels with ozone mixing ratios less than 50 ppbv. We suggest that the typically saturated air in the lower TTL over the western Pacific is likely driven by a combination of the frequent occurrence of deep convection and the predominance of rising motion in this region. The nearly constant water vapor mixing ratios in the middle to upper TTL likely result from the combination of slow ascent (resulting in long residence times) and wave-driven temperature variability. The numerical simulations generally reproduce the observed RHI distribution features, and sensitivity tests further emphasize the strong influence of convective input and vertical motions on TTL relative humidity.
Atmospheric composition is governed by the interplay of emissions, chemistry, deposition, and transport. Substantial questions surround each of these processes, especially in forested environments ...with strong biogenic emissions. Utilizing aircraft observations acquired over a forest in the southeast U.S., we calculate eddy covariance fluxes for a suite of reactive gases and apply the synergistic information derived from this analysis to quantify emission and deposition fluxes, oxidant concentrations, aerosol uptake coefficients, and other key parameters. Evaluation of results against state‐of‐the‐science models and parameterizations provides insight into our current understanding of this system and frames future observational priorities. As a near‐direct measurement of fundamental process rates, airborne fluxes offer a new tool to improve biogenic and anthropogenic emissions inventories, photochemical mechanisms, and deposition parameterizations.
Key Points
Airborne flux observations for a suite of reactive gases
Direct constraints on production, loss, and surface‐atmosphere exchange
Comprehensive evaluation of chemical budgets over a temperate forest
We introduce a climate intervention strategy focused on decreasing water vapor (WV) concentrations near the tropopause and in the stratosphere to increase outbound longwave radiation. The mechanism ...is the targeted injection of ice-nucleating particles (INP) in air supersaturated with respect to ice at high altitudes in the tropical entryway to the stratosphere. Ice formation in this region is a critical control of stratospheric WV. Recent airborne in situ data indicate that targeting only a small fraction of air parcels in the region would be sufficient to achieve substantial removal of water. This "intentional stratospheric dehydration" (ISD) strategy would not counteract a large fraction of the forcing from carbon dioxide but may contribute to a portfolio of climate interventions by acting with different time and length scales of impact and risk than other interventions that are already under consideration. We outline the idea, its plausibility, technical hurdles, and side effects to be considered.
Numerical simulations of cirrus formation in the tropical tropopause layer (TTL) during Boreal wintertime are used to evaluate the impact of heterogeneous ice nuclei (IN) abundance on cold cloud ...microphysical properties and occurrence frequencies. The cirrus model includes homogeneous and heterogeneous ice nucleation, deposition growth/sublimation, and sedimentation. Reanalysis temperature and wind fields with high-frequency waves superimposed are used to force the simulations. The model results are constrained by comparison with in situ and satellite observations of TTL cirrus and relative humidity. Temperature variability driven by high-frequency waves has a dominant influence on TTL cirrus microphysical properties and occurrence frequencies, and inclusion of these waves is required to produce agreement between the simulated and observed abundance of TTL cirrus. With homogeneous freezing only and small-scale gravity waves included in the temperature curtains, the model produces excessive ice concentrations compared with in situ observations. Inclusion of relatively numerous heterogeneous nuclei (Nsub IN ≥ 100 Lsup -1^) in the simulations improves the agreement with observed ice concentrations. However, when IN contribute significantly to TTL cirrus ice nucleation, the occurrence frequency of large supersaturations with respect to ice is less than indicated by in situ measurements. We find that the sensitivity of TTL cirrus extinction and ice water content statistics to heterogeneous ice nuclei abundance is relatively weak. The simulated occurrence frequencies of TTL cirrus are quite insensitive to ice nuclei abundance, both in terms of cloud frequency height distribution and regional distribution throughout the tropics.
The Eddy-Covariance Method for quantifying surface-atmosphere fluxes is a foundational technique for measuring net ecosystem exchange and validating regional-to-global carbon cycle models. While ...towers or ships are the most frequent platform for measuring surface-atmosphere exchange, experiments using aircraft for flux measurements have yielded contributions to several large-scale studies including BOREAS, SMACEX, RECAB by providing local-to-regional coverage beyond towers. The low-altitude flight requirements make airborne flux measurements particularly dangerous and well suited for unmanned aircraft.
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