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Time-resolved particle emissions from a conventional wood stove were investigated with aerosol mass spectrometry to provide links between combustion conditions, emission factors, mixing state of refractory black carbon and implications for organic tracer methods. The addition of a new batch of fuel results in low temperature pyrolysis as the fuel heats up, resulting in strong, short-lived, variable emission peaks of organic aerosol-containing markers of anhydrous sugars, such as levoglucosan (fragment at m/z 60). Flaming combustion results in emissions dominated by refractory black carbon co-emitted with minor fractions of organic aerosol and markers of anhydrous sugars. Full cycle emissions are an external mixture of larger organic aerosol-dominated and smaller thinly coated refractory black carbon particles. A very high burn rate results in increased full cycle mass emission factors of 66, 2.7, 2.8 and 1.3 for particulate polycyclic aromatic hydrocarbons, refractory black carbon, total organic aerosol and m/z 60, respectively, compared to nominal burn rate. Polycyclic aromatic hydrocarbons are primarily associated with refractory black carbon-containing particles. We hypothesize that at very high burn rates, the central parts of the combustion zone become air starved, leading to a locally reduced combustion temperature that reduces the conversion rates from polycyclic aromatic hydrocarbons to refractory black carbon. This facilitates a strong increase of polycyclic aromatic hydrocarbons emissions. At nominal burn rates, full cycle emissions based on m/z 60 correlate well with organic aerosol, refractory black carbon and particulate matter. However, at higher burn rates, m/z 60 does not correlate with increased emissions of polycyclic aromatic hydrocarbons, refractory black carbon and organic aerosol in the flaming phase. The new knowledge can be used to advance source apportionment studies, reduce emissions of genotoxic compounds and model the climate impacts of refractory black carbon, such as absorption enhancement by lensing. (C) 2017 The Authors. Published by Elsevier Ltd.

A series of sensitivity studies were performed with a spectral radiative transfer model using aerosol data from the Global Aerosol Data Set (GADS, data available at http://www.meteo.physik.uni-muenchen.de/strahlung/aerosol/aerosol.htm) in order to investigate and quantify the relative role of key climatic parameters on clear-sky ultraviolet-visible direct aerosol radiative forcing at the top of the atmosphere (TOA), within the atmosphere and at the Earth's surface. The model results show that relative humidity and aerosol single-scattering albedo are the most important climatic parameters that determine aerosol forcing at the TOA and at the Earth's surface and atmosphere, respectively. Relative humidity exerts a non-linear positive radiative effect, i.e. increasing humidity amplifies the magnitude of the forcing in the atmosphere and at the surface. Our model sensitivity studies show that increasing relative humidity by 10%, in relative terms, increases the aerosol forcing by factors of 1.42 at the TOA, 1.02 in the atmosphere and 1.17 at the surface. An increase in aerosol single-scattering albedo by 10%, in relative terms, increased the aerosol forcing at the TOA by 1.29, while it decreased the forcing in the atmosphere and at the surface by factors of 0.2 and 0.69, respectively. Our results show that an increase in relative humidity enhances the planetary cooling effect of aerosols (increased reflection of solar radiation to space) over oceans and low-albedo land areas, whilst over polar regions and highly reflecting land surfaces the warming effect of aerosols changes to a cooling effect. Thus, global warming and an associated increase in relative humidity would lead to enhanced aerosol cooling worldwide. The sensitivity results also demonstrate that an increase in surface albedo due to, for example, a reduction in land vegetation cover, would lead to enhanced atmospheric warming by aerosols leading to a reduction in cloud formation and enhancement of the desertification process. On the contrary, a decrease in surface albedo over polar regions due to, for example, ice-melting associated with global warming, would reduce the planetary warming effect of aerosols over polar areas. Aerosol forcing is found to be quite sensitive to cloud cover, as well as to aerosol optical thickness and the asymmetry parameter, and to the wavelength dependence of the aerosol optical properties. Tellus Series B-Chemical and Physical Meteorology