Background:Although epidemiologic studies have shown associations between particle mass and daily mortality, evidence on other particle metrics is weak.Objectives:We investigated associations of size-specific particle number concentration (PNC) and lung-deposited particle surface area concentration (PSC) with cause-specific daily mortality in contrast to .Methods:We used time-series data (March 2009–December 2014) on daily natural, cardiovascular, and respiratory mortality (NM, CVM, RM) of three adjacent cities in the Ruhr Area, Germany. Size-specific PNC (electric mobility diameter of ), PSC, and were measured at an urban background monitoring site. In single- and multipollutant Poisson regression models, we estimated percentage change (95% confidence interval) [% (95% CI)] in mortality per interquartile range (IQR) in exposure at single-day (0–7) and aggregated lags (0–1, 2–3, 4–7), accounting for time trend, temperature, humidity, day of week, holidays, period of seasonal population decrease, and influenza.Results: and PSC were highly correlated and had similar immediate (lag0–1) and delayed (lag4–7) associations with NM and CVM, for example, 1.12% (95% CI: 0.09, 2.33) and 1.56% (95% CI: 0.22, 2.92) higher NM with IQR increases in at lag0–1 and lag4–7, respectfully, which were slightly stronger then associations with IQR increases in . Positive associations between PNC and NM were strongest for accumulation mode particles (PNC ), and for larger UFPs (PNC ). Associations between NM and changed little after adjustment for or , but were more sensitive to adjustment for .Conclusion:Size-specific PNC () and lung-deposited PSC were associated with natural and cardiovascular mortality in the Ruhr Area. Although associations were similar to those estimated for an IQR increase in , particle number size distributions can be linked to emission sources, and thus may be more informative for potential public health interventions. Moreover, PSC could be used as an alternative metric that integrates particle size distribution as well as deposition efficiency. https://doi.org/10.1289/EHP2054
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