Ice-nucleating particle concentrations of the past: Insights from a 600-year-old Greenland ice core

Abstract

Ice-nucleating particles (INPs) affect the microphysics in cloud and precipitation processes. Hence, they modulate the radiative properties of clouds. However, atmospheric INP concentrations of the past are basically unknown. Here, we present INP measurements from an ice core in Greenland, which dates back to the year 1370. In total 135 samples were analyzed with the FRIDGE droplet freezing assay in the temperature range from -14 to -35 C. The sampling frequency was set to 1 in 10 years from 1370 to 1960. From 1960 to 1990 the frequency was increased to one sample per year. Additionally, a few special events were probed, including volcanic episodes. The typical time coverage of a sample was on the order of a few months. Historical atmospheric INP concentrations were estimated with a conversion factor, which depends on the snow accumulation rate of the ice core, particle dry deposition velocity, and wet scavenging ratio. Typical atmospheric INP concentrations were on the order of 0.1L-1 at -25 C. The INP variability was found to be about 1-2 orders of magnitude. Yet, the short-term variability from samples over a seasonal cycle was considerably lower. INP concentrations were significantly correlated to some chemical tracers derived from continuous-flow analysis (CFA) and ion chromatography (IC) over a broad range of nucleation temperatures. The highest correlation coefficients were found for the particle concentration (spherical diameter dp 1.2m). The correlation is higher for a time period of seasonal samples, where INP concentrations follow a clear annual pattern, highlighting the importance of the annual dust input in Greenland from East Asian deserts during spring. Scanning electron microscopy (SEM) analysis of selected samples found mineral dust to be the dominant particle fraction, verifying their significance as INPs. Overall, the concentrations compare reasonably well to present-day INP concentrations, albeit they are on the lower side. However, we found that the INP concentration at medium supercooled temperatures differed before and after 1960. Average INP concentrations at -23, -24, -25, -26, and -28 C were significantly higher (and more variable) in the modern-day period, which could indicate a potential anthropogenic impact, e.g., from land-use change.