Abstract. Ice nucleation of volcanic ash controls both ash aggregation and cloud glaciation, which affect atmospheric transport and global climate. Previously, it has been suggested that there is one characteristic ice nucleation efficiency for all volcanic ash, regardless of its composition, when accounting for surface area; however, this claim is derived from data from only two volcanic eruptions. In this work, we have studied the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman microscopy coupled to an environmental cell. Ash from the Fuego (basaltic ash, Guatemala), Soufrière Hills (andesitic ash, Montserrat), and Taupo (Oruanui eruption, rhyolitic ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. In the present study, we find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice from 225 to 235 K at ice saturation ratios of 1.05 ± 0.01, comparable to the mineral dust proxy kaolinite. Since depositional ice nucleation will be more important at colder temperatures, fine volcanic ash may represent a global source of cold-cloud ice nuclei. For immersion freezing relevant to mixed-phase clouds, however, only the Oruanui ash exhibited appreciable heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.

Volcanic ash particles can be remelted by the high temperatures induced in volcanic lightning discharges. The molten particles can round under surface tension then quench to produce glass spheres. Melting and rounding timescales for volcanic materials are strongly dependent on heating duration and peak temperature and are shorter for small particles than for large particles. Therefore, the size distribution of glass spheres recovered from ash deposits potentially record the short duration, high‐temperature conditions of volcanic lightning discharges, which are hard to measure directly. We use a 1‐D numerical solution to the heat equation to determine the timescales of heating and cooling of volcanic particles during and after rapid heating and compare these with the capillary timescale for rounding an angular particle. We define dimensionless parameters—capillary, Fourier, Stark, Biot, and Peclet numbers—to characterize the competition between heat transfer within the particle, heat transfer at the particle rim, and capillary motion, for particles of different sizes. We apply this framework to the lightning case and constrain a maximum size for ash particles susceptible to surface tension‐driven rounding, as a function of lightning temperature and duration, and ash properties. The size limit agrees well with maximum sizes of glass spheres found in volcanic ash that has been subjected to lightning or experimental discharges, demonstrating that the approach that we develop can be used to obtain a first‐order estimate of lightning conditions in volcanic plumes.

Glass spherules have been documented in many geologic deposits and are formed during high-temperature processes that include cloud-to-ground lightning strikes, volcanic eruptions of low-viscosity magmas, and meteorite impacts. This study reviews the known glass spheruleforming processes and proposes, for the first time, a mechanism induced through the heat generated by volcanic lightning in eruptive columns and plumes (laterally spreading clouds) during explosive eruptions. Ash-fall samples were collected from two eruptions where volcanic lightning was extensively documented: the A.D. 2009 eruption of Mount Redoubt, Alaska (USA), and the 2010 eruption of Eyjafjallajökull, Iceland. These samples reveal individual glass spherules ~50 mm in average diameter that compose <5% of the examined portion of the deposit. Textures include smooth, hollow, or cracked spherules, as well as aggregates, which suggest melting of ash particles as a result of proximity to the electrical discharge channel and subsequent re-solidification of the particles into spherical morphologies. The natural ash-fall samples are compared with pseudo-ash samples collected from high-voltage insulator experiments in order to test our hypothesis that volcanic ash particles can be transformed into glass spherules through the heat generated by electrical discharge. We refer to this new morphological classification of ash grains as lightning-induced volcanic spherules and hypothesize that this texture not only provides direct physical evidence of lightning occurrence during explosive eruptions, but will also increase settling velocities and reduce aggregation of these particles, affecting ash transport dynamics.