Climate Change, Summer Temperature, and Heat-Related Mortality in Finland: Multicohort Study with Projections for a Sustainable vs. Fossil-Fueled Future to 2050.

BACKGROUND: Climate change scenarios illustrate various pathways in terms of global warming ranging from "sustainable development" (Shared Socioeconomic Pathway SSP1-1.9), the best-case scenario, to 'fossil-fueled development' (SSP5-8.5), the worst-case scenario. OBJECTIVES: We examined the extent to which increase in daily average urban summer temperature is associated with future cause-specific mortality and projected heat-related mortality burden for the current warming trend and these two scenarios. METHODS: We did an observational cohort study of 363,754 participants living in six cities in Finland. Using residential addresses, participants were linked to daily temperature records and electronic death records from national registries during summers (1 May to 30 September) 2000 to 2018. For each day of observation, heat index (average daily air temperature weighted by humidity) for the preceding 7 d was calculated for participants' residential area using a geographic grid at a spatial resolution of 1km×1km. We examined associations of the summer heat index with risk of death by cause for all participants adjusting for a wide range of individual-level covariates and in subsidiary analyses using case-crossover design, computed the related period population attributable fraction (PAF), and projected change in PAF from summers 2000-2018 compared with those in 2030-2050. RESULTS: During a cohort total exposure period of 582,111,979 summer days (3,880,746 person-summers), we recorded 4,094 deaths, including 949 from cardiovascular disease. The multivariable-adjusted rate ratio (RR) for high (≥21°C) vs. reference (14-15°C) heat index was 1.70 (95% CI: 1.28, 2.27) for cardiovascular mortality, but it did not reach statistical significance for noncardiovascular deaths, RR=1.14 (95% CI: 0.96, 1.36), a finding replicated in case-crossover analysis. According to projections for 2030-2050, PAF of summertime cardiovascular mortality attributable to high heat will be 4.4% (1.8%-7.3%) under the sustainable development scenario, but 7.6% (3.2%-12.3%) under the fossil-fueled development scenario. In the six cities, the estimated annual number of summertime heat-related cardiovascular deaths under the two scenarios will be 174 and 298 for a total population of 1,759,468 people. DISCUSSION: The increase in average urban summer temperature will raise heat-related cardiovascular mortality burden. The estimated magnitude of this burden is >1.5 times greater if future climate change is driven by fossil fuels rather than sustainable development. https://doi.org/10.1289/EHP12080.

Global atmospheric particle formation from CERN CLOUD measurements.

Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast, gas-phase chemistry models have been based on laboratory kinetics measurements for decades. We built a global model of aerosol formation by using extensive laboratory measurements of rates of nucleation involving sulfuric acid, ammonia, ions, and organic compounds conducted in the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present-day atmosphere involves ammonia or biogenic organic compounds, in addition to sulfuric acid. A considerable fraction of nucleation involves ions, but the relatively weak dependence on ion concentrations indicates that for the processes studied, variations in cosmic ray intensity do not appreciably affect climate through nucleation in the present-day atmosphere.

Ecosystem impacts of geoengineering: a review for developing a science plan.

Geoengineering methods are intended to reduce climate change, which is already having demonstrable effects on ecosystem structure and functioning in some regions. Two types of geoengineering activities that have been proposed are: carbon dioxide (CO(2)) removal (CDR), which removes CO(2) from the atmosphere, and solar radiation management (SRM, or sunlight reflection methods), which reflects a small percentage of sunlight back into space to offset warming from greenhouse gases (GHGs). Current research suggests that SRM or CDR might diminish the impacts of climate change on ecosystems by reducing changes in temperature and precipitation. However, sudden cessation of SRM would exacerbate the climate effects on ecosystems, and some CDR might interfere with oceanic and terrestrial ecosystem processes. The many risks and uncertainties associated with these new kinds of purposeful perturbations to the Earth system are not well understood and require cautious and comprehensive research.

A thermodynamically consistent determination of surface tension of small Lennard-Jones clusters from simulation and theory.

We have determined the surface tension of small Lennard-Jones clusters using molecular dynamics and Monte Carlo simulation methods as well as density functional theory calculations. For the two simulation methods the surface tension is calculated via a rigorous thermodynamic route using simulation data as input. The capillary approximation of the classical nucleation theory, where the surface tension of a planar surface is used for cluster surface, is found to be quite reasonable even when the cluster size is as small as 100-150 atoms. For smaller cluster sizes the cluster surface tension is considerably lower than the planar value. We have also obtained an approximative value for the Tolman length by extrapolating to the planar limit the difference between the equimolar radius and the radius of the surface of tension. A negative Tolman length is suggested by all the methods used.

Equilibrium sizes and formation energies of small and large Lennard-Jones clusters from molecular dynamics: a consistent comparison to Monte Carlo simulations and density functional theories.

We have performed molecular dynamics simulations of Lennard-Jones argon clusters in equilibrium with a surrounding vapor and combined them with simulations of nucleation events in supersaturated vapor to investigate the dependence of critical cluster size on the vapor density in the cluster size range of 20-300 atoms. The simulations are performed at reduced temperature T(') = 0.662, which with the parameter values of Lennard-Jones argon corresponds to 80 K. We obtain bulk equilibrium values by simulating a planar liquid-vapor interface. In the studied cluster size range, we find a linear relation between critical size Delta N(*) and Delta mu(-3), where Delta mu is the chemical potential difference between supersaturated vapor and saturated vapor, but the slope of the line is not given by the Kelvin relation of classical nucleation theory. With this relation, along with the known formation energy of the small critical cluster of the nucleation simulations, we proceed to calculate the formation energies for larger critical sizes by integrating the nucleation theorem. We compare the molecular dynamics results to results from Monte Carlo simulations and both perturbative density functional theory and square gradient theory calculations. We find that the molecular dynamics results are in excellent agreement with the density functional and square gradient values. However, the Monte Carlo critical sizes and formation energies are somewhat lower than the molecular dynamics ones.

Connection between the virial equation of state and physical clusters in a low density vapor.

We carry out Monte Carlo simulations of physical Lennard-Jones and water clusters and show that the number of physical clusters in vapor is directly related to the virial equation of state. This relation holds at temperatures clearly below the critical temperatures, in other words, as long as the cluster-cluster interactions can be neglected--a typical assumption used in theories of nucleation. Above a certain threshold cluster size depending on temperature and interaction potential, the change in cluster work of formation can be calculated analytically with the recently proposed scaling law. The breakdown of the scaling law below the threshold sizes is accurately modeled with the low order virial coefficients. Our results indicate that high order virial coefficients can be analytically calculated from the lower order coefficients when the scaling law for cluster work of formation is valid. The scaling law also allows the calculation of the surface tension and equilibrium vapor density with computationally efficient simulations of physical clusters. Our calculated values are in good agreement with those obtained with other methods. We also present our results for the curvature dependent surface tension of water clusters.

Origin of the failure of classical nucleation theory: incorrect description of the smallest clusters.

We carry out molecular Monte Carlo simulations of clusters in an imperfect vapor. We show that down to very small cluster sizes, classical nucleation theory built on the liquid drop model can be used very accurately to describe the work required to add a monomer to the cluster. However, the error made in modeling the smallest of clusters as liquid drops results in an erroneous absolute value for the cluster work of formation throughout the size range. We calculate factors needed to correct the cluster formation work given by the liquid drop model. The corrected work of formation results in nucleation rates in good agreement with recent nucleation experiments on argon and water.

Analysis of nucleation ability of cluster configurations with Monte Carlo simulations of argon.

We determine the nucleation ability of argon clusters from Monte Carlo simulations. The nucleation rate appears to be defined by a sole characteristic of the clusters, namely, the stability. The stability is calculated as the ratio of grand canonical growth and decay rates and can be assigned to individual cluster configurations. We study the connection between the stability of the cluster configurations and their volume and total potential energy. Neither the potential energy nor the volume of a cluster configuration has a clear relation to its stability, and thus to the nucleation ability. On the other hand, we show that it is possible to use a specific volume for each cluster size to calculate the work of the cluster formation. These clusters with a unique volume have the same average stability as the full set of clusters. Our simulation method allows us to study the effect of possible deviations from equilibrium in the cluster configuration distributions. We argue that the nucleation process itself can produce a source for such a deviation. We show that even a small deviation from equilibrium in the cluster configuration distribution can lead to a dramatic deceleration of the nucleation rate. Although our simulations may overestimate the magnitude of the effect, they give qualitative estimates for its importance.

Monte Carlo simulations of critical cluster sizes and nucleation rates of water.

We have calculated the critical cluster sizes and homogeneous nucleation rates of water at temperatures and vapor densities corresponding to experiments by Wolk and Strey [J. Phys. Chem B 105, 11683 (2001)]. The calculations have been done with an expanded version of a Monte Carlo method originally developed by Vehkamaki and Ford [J. Chem. Phys. 112, 4193 (2000)]. Their method calculates the statistical growth and decay probabilities of molecular clusters. We have derived a connection between these probabilities and kinetic condensation and evaporation rates, and introduce a new way for the calculation of the work of formation of clusters. Three different interaction potential models of water have been used in the simulations. These include the unpolarizable SPC/E [J. Phys. Chem. 91, 6269 (1987)] and TIP4P [J. Chem. Phys. 79, 926 (1983)] models and a polarizable model by Guillot and Guissani [J. Chem. Phys. 114, 6720 (2001)]. We show that TIP4P produces critical cluster sizes and a temperature and vapor density dependence for the nucleation rate that agree well with the experimental data, although the magnitude of nucleation rate is constantly overestimated by a factor of 2 x 10(4). Guissani and Guillot's model is somewhat less successful, but both the TIP4P and Guillot and Guissani models are able to reproduce a much better experimental temperature dependency of the nucleation rate than the classical nucleation theory. Using SPC/E results in dramatically too small critical clusters and high nucleation rates. The water models give different average binding energies for clusters. We show that stronger binding between cluster molecules suppresses the decay probability of a cluster, while the growth probability is not affected. This explains the differences in results from different water models.