M. J. Northway

An analysis of large HNO3‐containing particles sampled in the Arctic stratosphere during the winter of 1999/2000

Large (>2 μm diameter) HNO_3-containing polar stratospheric cloud (PSC) particles were measured in situ by the NOAA NO_y instrument on board the NASA ER-2 aircraft during seven flights in the 1999/2000 Arctic winter vortex. Here we discuss the detection of these large PSC particles, their spatial distribution, the ambient conditions under which they were detected, and our methods for interpreting NO_y time series with respect to particle sizes and number concentrations. The particles were observed through the use of two NO_y inlets on a particle separator extending below the ER-2 aircraft. The particle phase is assumed to be nitric acid trihydrate (NAT) or nitric acid dihydrate (NAD). Over a 48-day period, particles were sampled in the Arctic vortex over a broad range of latitudes (60–85°N) and altitudes (15–21 km). Typically, regions of the atmosphere up to 4 km above the observed large particle clouds were saturated with respect to NAT. Occasionally, large particles were measured in air subsaturated with respect to NAT, suggesting ongoing particle evaporation. Vortex minimum temperatures in the observation period suggest that synoptic-scale ice saturation conditions are not required for the formation of this type of particle. Three analytical methods are used to estimate size and number concentrations from the NO_y time series. Results indicate particle sizes between 5 and 20 μm diameter and concentrations from 10^(−5) to 10^(−3) cm^(−3). These low number concentrations imply a selective nucleation mechanism. Particle sizes and number concentrations were greater during the midwinter flights than the late winter flights. Knowledge of the geographical extent of large particles, actual sampling conditions, and particle size distributions offers multiple constraints for atmospheric models of PSC formation, which will lead to a better understanding of the process of denitrification and improvements in modeling future ozone loss.

Large NAT particle formation by mother clouds: Analysis of SOLVE/THESEO‐2000 observations

[1] During the SOLVE/THESEO-2000 Arctic stratospheric campaign in the winter 1999/2000 widespread occurrences of very large HNO3-containing particles, probably composed of nitric acid trihydrate (NAT), were observed in situ by instruments on board the ER-2 stratospheric research aircraft. These large NAT particles were found with low number densities (n 10 4 cm 3 ) in vast regions, in air generally supersaturated with respect to NAT. Within the same campaign other instruments have performed airborne and ground-based measurements of polar stratospheric clouds (PSCs), often showing the existence of type 1a and type 1a-enh clouds. Such PSCs often occur on the mesoscale with particle number densities n ^ 10 2 cm 3 and are also mostlikelycomposedofNAT.Weuseforwardtrajectoriesfor thepathofNATparticles, whichareadvectedbywindsbased on ECMWF analyses and sediment due to gravity, to show that high number density NAT PSCs (mother clouds) could give rise to low number density NAT particle populations several daysdownstream. INDEXTERMS:0305Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Structure: Cloud physics and chemistry; 0341 Atmospheric Composition and Structure: Middle atmosphere—constituent transport and chemistry (3334)

Stratospheric Aerosol Sampling: Effect of a Blunt-Body Housing on Inlet Sampling Characteristics

During a campaign to study ozone loss mechanisms in the Arctic stratosphere (SOLVE), several instruments on NASAs ER-2 aircraft observed a very low number density (0.1 I−1) of large, nitric-acid-containing particles that form the polar stratospheric clouds (PSCs). For effective physical and chemical characterization of these particles, the measurements from these instruments have to be intercompared and integrated. In particular, proper interpretation requires knowledge of the sampling characteristics of the particles into the instruments. Here, we present the calculation of the sampling characteristics of the one of the instruments on the ER-2, the NOAA NOy instrument. This instrument sampled ambient particles and gas from two forward-facing inlets located fore and aft on a particle-separation housing (the football) and measured total NOy in the sample. In recent studies, ambient aerosol mass has been estimated by the difference of the measurements of the two inlets with the assumption that the rear inlet observations represent the gas-phase NOy and small particles and the front inlet samples represent gas-phase NOy and all particle sizes with varied efficiency (anisokinetic sampling). This knowledge was derived largely from semiempirical relations and potential flow studies of the housing. In our study, we used CFD simulations to model the compressible flow conditions and considered noncontinuum effects in calculating particle trajectories. Our simulations show that the blunt body housing the inlets has a strong and complex interaction with the flow and particles sampled by the two inlets. The simulations show that the front inlet characteristics are influenced by the effect of the blunt body on the upstream pressure field. The rear inlet sampling characteristics are influenced both by the shape and size of the inlet and its location on the blunt body. These interactions result in calculated inlet characteristics that are significantly different from previously assumed values. Analysis of the SOLVE data, considering the ambient conditions and the calculated inlet sampling characteristics, in conjunction with thermodynamic growth modeling of super-cooled ternary solution (STS) particles, provides validation of the CFD results.

Trajectory studies of large HNO3‐containing PSC particles in the Arctic: Evidence for the role of NAT

Large (5 to >20 μm 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.