Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia

The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker fragments places upper limits of 7.5% for amino acids and 5.6% for carbohydrates on the contribution of primary biological aerosol particles (PBAP) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m−3. Carbohydrates and proteins (composed of amino acids) make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAP mass fraction of about 20% to the submicron organic aerosol measured in Amazonia during AMAZE-08

Energy dissipation in the time domain governed by bosons in a correlated material

In complex materials various interactions play important roles in determining the material properties. Angle Resolved Photoelectron Spectroscopy (ARPES) has been used to study these processes by resolving the complex single particle self energy $\Sigma(E)$ and quantifying how quantum interactions modify bare electronic states. However, ambiguities in the measurement of the real part of the self energy and an intrinsic inability to disentangle various contributions to the imaginary part of the self energy often leave the implications of such measurements open to debate. Here we employ a combined theoretical and experimental treatment of femtosecond time-resolved ARPES (tr-ARPES) and show how measuring the population dynamics using tr-ARPES can be used to separate electron-boson interactions from electron-electron interactions. We demonstrate the analysis of a well-defined electron-boson interaction in the unoccupied spectrum of the cuprate Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+x}$ characterized by an excited population decay time constant $\tau_{QP}$ that maps directly to a discrete component of the equilibrium self energy not readily isolated by static ARPES experiments.Comment: 19 pages with 6 figure

In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity

International audiencePublished by Copernicus Publications on behalf of the European Geosciences Union. 9578 M. Beekmann et al.: Evidence for a dominant regional contribution to fine particulate matter levels Abstract. A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radio-carbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin , i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant , flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies

In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity

A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies

In situ formation and spatial variability of particle number concentration in a European megacity

Ambient particle number size distributions were measured in Paris, France, during summer (1-31 July 2009) and winter (15 January to 15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation (MEGAPOLI) project. New particle formation (NPF) was observed only during summer on approximately 50% of the campaign days, assisted by the low condensation sink (about 10.7 +/- 5.9 x 10(-3) s(-1)). NPF events inside the Paris plume were also observed at 600m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from the Paris center during summer. The number concentration of particles with diameters exceeding 2.5 nm measured on the surface at the Paris center was on average 6.9 +/- 8.7 x 10(4) and 12.1 +/- 8.6 x 10(4) cm(-3) during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer, one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of 3 when it was downwind of Paris.Peer reviewe

Micromechanical study of the load transfer in a polycaprolactone-collagen hybrid scaffold when subjected to unconfined and confined compression

Scaffolds are used in diverse tissue engineering applications as hosts for cell proliferation and extracellular matrix formation. One of the most used tissue engineering materials is collagen, which is well known to be a natural biomaterial, also frequently used as cell substrate, given its natural abundance and intrinsic biocompatibility. This study aims to evaluate how the macroscopic biomechanical stimuli applied on a construct made of polycaprolactone scaffold embedded in a collagen substrate translate into microscopic stimuli at the cell level. Eight poro-hyperelastic finite element models of 3D printed hybrid scaffolds from the same batch were created, along with an equivalent model of the idealized geometry of that scaffold. When applying an 8% confined compression at the macroscopic level, local fluid flow of up to 20 [Formula: see text]m/s and octahedral strain levels mostly under 20% were calculated in the collagen substrate. Conversely unconfined compression induced fluid flow of up to 10 [Formula: see text]m/s and octahedral strain from 10 to 35%. No relevant differences were found amongst the scaffold-specific models. Following the mechanoregulation theory based on Prendergast et al. (J Biomech 30:539-548, 1997. https://doi.org/10.1016/S0021-9290(96)00140-6 ), those results suggest that mainly cartilage or fibrous tissue formation would be expected to occur under unconfined or confined compression, respectively. This in silico study helps to quantify the microscopic stimuli that are present within the collagen substrate and that will affect cell response under in vitro bioreactor mechanical stimulation or even after implantation

Quantitative single-particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data

Single-particle mass spectrometry has proven a valuable tool for gaining information on the mixing state of aerosol particles. With the Aerodyne aerosol mass spectrometer (AMS) equipped with a light-scattering probe, nonrefractory components of submicron particles with diameters larger than about 300 nm can even be quantified on a single-particle basis. Here, we present a new method for the analysis of AMS single-particle mass spectra. The developed algorithm classifies the particles according to their components (e. g. sulphate, nitrate, different types of organics) and simultaneously provides quantitative information about the composition of the single particles. This classification algorithm was validated by applying it to data acquired in laboratory experiments with particles of known composition, and applied to field data acquired during the MEGAPOLI summer campaign (July 2009) in Paris. As shown, it is not only possible to directly measure the mixing state of atmospheric particles, but also to directly observe repartitioning of semi-volatile species between gas and particle phase during the course of the day