The RHAPS (Redox-Activity And Health-Effects Of Atmospheric Primary And Secondary Aerosol) project was launched in 2019 with the major objective of identifying specific properties of the fine atmospheric aerosol from combustion sources that are responsible for toxicological effects and can be used as new metrics for health-related outdoor pollution studies. In this paper, we present the overall methodology of RHAPS and introduce the phenomenology and the first data observed. A comprehensive physico-chemical aerosol characterization has been achieved by means of high-time resolution measurements (e.g., number size distributions, refractory chemical components, elemental composition) and low-time resolution analyses (e.g., oxidative potential, toxicological assays, chemical composition). Preliminary results indicate that, at the real atmospheric conditions observed (i.e., daily PM₁ from less than 4 to more than 50 μg m⁻³), high/low mass concentrations of PM₁, as well as black carbon (BC) and water soluble Oxidative Potential (WSOP,) do not necessarily translate into high/low toxicity. Notably, these findings were observed during a variety of atmospheric conditions and aerosol properties and with different toxicological assessments. Findings suggest a higher complexity in the relations observed between atmospheric aerosol and toxicological endpoints that go beyond the currently used PM₁ metrics. Finally, we provide an outlook to companion papers where data will be analyzed in more detail, with the focus on source apportionment of PM₁ and the role of source emissions on aerosol toxicity, the OP as a predictive variable for PM₁ toxicity, and the related role of SOA possessing redox-active capacity, exposure-response relationships for PM₁, and air quality models to forecast PM₁ toxicity.

In this work, an FPGA-based plain delay line TDC is presented, together with a theoretical model on its timing properties. The TDC features an automated calibration system implemented in the on-chip processor of a SoC-FPGA, uses a low amount of FPGA resources and is therefore suitable for applications requiring a high number of channels such as Time-of-Flight Positron Emission Tomography. We first investigated the importance of calibration and validated the theoretical model on the TDC timing properties. Finally, the device has been embodied into a two channel Positron Emission Tomography acquisition system and tested. We found the calibration essential to obtain a good time resolution (38 ps FWHM in comparison with a 78 ps FWHM obtained with the uncalibrated device). The model we developed is able to predict the TDC timing properties. They are shown to be related to the fundamental parameters of the used FPGA technology. In particular, the best achievable time resolution of this specific architecture (plain tapped delay line on FPGA) is set to about 30 ps by the sum of the setup and hold times of the registers in the FPGA. The timing resolution of the two-channel setup is about 118 ps.

While more and more studies are being conducted on carbonaceous fractions—organic carbon (OC) and elemental carbon (EC)—in urban areas, there are still too few studies about these species and their effects in polar areas due to their very low concentrations; further, studies in the literature report only data from intensive campaigns, limited in time. We present here for the first time EC–OC concentration long-time data records from the sea-level sampling site of Ny-Ålesund, in the High Arctic (5 years), and from Dome C, in the East Antarctic Plateau (1 year). Regarding the Arctic, the median (and the interquartile range (IQR)) mass concentrations for the years 2011–2015 are 352 (IQR: 283–475) ng/m³ for OC and 4.8 (IQR: 4.6–17.4) ng/m³ for EC, which is responsible for only 3% of total carbon (TC). From both the concentration data sets and the variation of the average monthly concentrations, the influence of the Arctic haze on EC and OC concentrations is evident. Summer may be interested by high concentration episodes mainly due to long-range transport (e.g., from wide wildfires in the Northern Hemisphere, as happened in 2015). The average ratio of EC/OC for the summer period is 0.05, ranging from 0.02 to 0.10, and indicates a clean environment with prevailing biogenic (or biomass burning) sources, as well as aged, highly oxidized aerosol from long-range transport. Contribution from ship emission is not evident, but this result may be due to the sampling time resolution. In Antarctica, a 1 year-around data set from December 2016 to February 2018 is shown, which does not present a clear seasonal trend. The OC median (and IQR) value is 78 (64–106) ng/m³; for EC, it is 0.9 (0.6–2.4) ng/m³, weighing for 3% on TC values. The EC/OC ratio mean value is 0.20, with a range of 0.06–0.35. Due to the low EC and OC concentrations in polar areas, correction for the blank is far more important than in campaigns carried out in other regions, largely affecting uncertainties in measured concentrations. Through the years, we have thus developed a new sampling strategy that is presented here for the first time: samplers were modified in order to collect a larger amount of particulates on a small surface, enhancing the capability of the analytical method since the thermo-optical analyzer is sensitive to carbonaceous aerosol areal density. Further, we have recently coupled such modified samplers with a sampling strategy that makes a more reliable blank correction of every single sample possible.