Microphysical properties of synoptic scale polar stratospheric clouds: in situ measurements of unexpectedly large HNO₃ containing particles in the Arctic vortex

Abstract

Abstract. In January 2010 and December 2011 synoptic scale PSC fields were probed during seven flights of the high altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction.) and the ESSenCe (ESSenCe: ESA Sounder Campaign) projects. Particle size distributions in a diameter range between 0.46 μm and 40 μm were recorded simultaneously by up to four different optical in situ instruments. Three of these particle instruments are based on the detection of forward scattered light by single particles. The fourth instrument is a grey scale optical array imaging probe. Optical particle diameters of up to 35 μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas phase and particle bound NOy were measured, as well as water vapor concentrations, and other variables. Two remote sensing particle instruments, the Miniature Aerosol Lidar (MAL) and the backscatter sonde (MAS, Multiwavelenght Aerosol Scatterometer) showed the synoptic scale of the encountered PSCs. The particle mode below 2 μm in size diameter has been identified as supercooled ternary solution droplets (STS). The PSC particles in the size range above 2 μm in diameter are considered to consist of nitric acid hydrates or ice, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. In particular, with respect to the denitrification by sedimentation of large HNO3-contaning particles, generally considered as NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Measurement uncertainties are discussed concerning probable overestimations of measured particle sizes and volumes. We hypothesize that either a strong asphericity or the particle composition (e.g. water-ice coated with NAT) could explain our observations.