186 research outputs found

    Graphical representations and cluster algorithms for critical points with fields

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    A two-replica graphical representation and associated cluster algorithm is described that is applicable to ferromagnetic Ising systems with arbitrary fields. Critical points are associated with the percolation threshold of the graphical representation. Results from numerical simulations of the Ising model in a staggered field are presented. The dynamic exponent for the algorithm is measured to be less than 0.5.Comment: Revtex, 12 pages with 2 figure

    Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments

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    Diesel particulate matter (DPM) is a significant source of aerosol in urban areas and has been linked to adverse health effects. Although newer European directives have introduced increasingly stringent standards for primary PM emissions, gaseous organics emitted from diesel cars can still lead to large amounts of secondary organic aerosol (SOA) in the atmosphere. Here we present results from smog chamber investigations characterizing the primary organic aerosol (POA) and the corresponding SOA formation at atmospherically relevant concentrations for three in-use diesel vehicles with different exhaust aftertreatment systems. One vehicle lacked exhaust aftertreatment devices, one vehicle was equipped with a diesel oxidation catalyst (DOC) and the third vehicle used both a DOC and diesel particulate filter (DPF). The experiments presented here were obtained from the vehicles at conditions representative of idle mode, and for one car in addition at a speed of 60 km/h. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was used to measure the organic aerosol (OA) concentration and to obtain information on the chemical composition. For the conditions explored in this paper, primary aerosols from vehicles without a particulate filter consisted mainly of black carbon (BC) with a low fraction of organic matter (OM, OM/BC < 0.5), while the subsequent aging by photooxidation resulted in a consistent production of SOA only for the vehicles without a DOC and with a deactivated DOC. After 5 h of aging ~80% of the total organic aerosol was on average secondary and the estimated "emission factor" for SOA was 0.23–0.56 g/kg fuel burned. In presence of both a DOC and a DPF, only 0.01 g SOA per kg fuel burned was produced within 5 h after lights on. The mass spectra indicate that POA was mostly a non-oxidized OA with an oxygen to carbon atomic ratio (O/C) ranging from 0.10 to 0.19. Five hours of oxidation led to a more oxidized OA with an O/C range of 0.21 to 0.37

    Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer

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    A series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA) concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC) instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA) production. After correcting for wall losses, the average increase in organic matter (OM) concentrations by SOA formation for the starting and flaming phase experiments with the two log wood burners was found to be a factor of 4.1&amp;plusmn;1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Including the measured SOA formation potential, average emission factors of BC+POA+SOA, calculated from CO&lt;sub&gt;2&lt;/sub&gt; emission, were found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;4&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; at mass to charge ratio &lt;i&gt;m/z&lt;/i&gt; 60, a commonly used marker for primary emissions of wood burning. This contribution at &lt;i&gt;m/z&lt;/i&gt; 60 can overcompensate for the degradation of levoglucosan leading to an overestimation of the contribution of wood burning or biomass burning to the total OM. The primary organic emissions from the three different burners showed a wide range in O:C atomic ratio (0.19&amp;minus;0.60) for the starting and flaming conditions, which also increased during aging. Primary wood burning emissions have a rather low relative contribution at &lt;i&gt;m/z&lt;/i&gt; 43 (&lt;i&gt;f&lt;/i&gt; 43) to the total organic mass spectrum. The non-oxidized fragment C&lt;sub&gt;3&lt;/sub&gt;H&lt;sub&gt;7&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; has a considerable contribution at &lt;i&gt;m/z&lt;/i&gt; 43 for the fresh OA with an increasing contribution of the oxygenated ion C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;3&lt;/sub&gt;O&lt;sup&gt;+&lt;/sup&gt; during aging. After five hours of aging, the OA has a rather low C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;3&lt;/sub&gt;O&lt;sup&gt;+&lt;/sup&gt; signal for a given CO&lt;sub&gt;2&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; fraction, possibly indicating a higher ratio of acid to non-acid oxygenated compounds in wood burning OA compared to other oxygenated organic aerosol (OOA)

    The Dynamic Exponent of the Two-Dimensional Ising Model and Monte Carlo Computation of the Sub-Dominant Eigenvalue of the Stochastic Matrix

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    We introduce a novel variance-reducing Monte Carlo algorithm for accurate determination of autocorrelation times. We apply this method to two-dimensional Ising systems with sizes up to 15×1515 \times 15, using single-spin flip dynamics, random site selection and transition probabilities according to the heat-bath method. From a finite-size scaling analysis of these autocorrelation times, the dynamical critical exponent zz is determined as z=2.1665z=2.1665 (12)

    Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles

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    A measurement campaign (IMBALANCE) conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, −30 °C, −35 °C and −40 °C. Freshly emitted diesel particles showed ice formation only at −40 °C in the deposition mode at 137% relative humidity with respect to ice (RH&lt;sub&gt;i&lt;/sub&gt;) and 92% relative humidity with respect to water (RH&lt;sub&gt;w&lt;/sub&gt;), and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at −35 °C. Wood burning particles also act as ice nuclei (IN) at −40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at −35 °C whereas no ice nucleation was observed at −30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below −40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds

    Aging induced changes on NEXAFS fingerprints in individual combustion particles

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    Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing of the combustion exhaust gases is still a subject of discussion. In this work, individual soot particles emitted from two different vehicles, a EURO 2 transporter, a EURO 3 passenger car, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using near edge X-ray absorption fine structure spectroscopy (NEXAFS) and scanning electron microscopy. Comparison of NEXAFS spectra from the unprocessed particles and those resulting from exhaust photooxidation in the chamber revealed changes in the carbon functional group content. For the wood stove emissions, these changes were minor, related to the relatively mild oxidation conditions. For the EURO 2 transporter emissions, the most apparent change was that of carboxylic carbon from oxidized organic compounds condensing on the primary soot particles. For the EURO 3 car emissions oxidation of primary soot particles upon photochemical aging has likely contributed as well. Overall, the changes in the NEXAFS fingerprints were in qualitative agreement with data from an aerosol mass spectrometer. Furthermore, by taking full advantage of our in situ microreactor concept, we show that the soot particles from all three combustion sources changed their ability to take up water under humid conditions upon photochemical aging of the exhaust. Due to the selectivity and sensitivity of the NEXAFS technique for the water mass, also small amounts of water taken up into the internal voids of agglomerated particles could be detected. Because such small amounts of water uptake do not lead to measurable changes in particle diameter, it may remain beyond the limits of volume growth measurements, especially for larger agglomerated particles

    Monte Carlo computation of correlation times of independent relaxation modes at criticality

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    We investigate aspects of universality of Glauber critical dynamics in two dimensions. We compute the critical exponent zz and numerically corroborate its universality for three different models in the static Ising universality class and for five independent relaxation modes. We also present evidence for universality of amplitude ratios, which shows that, as far as dynamic behavior is concerned, each model in a given universality class is characterized by a single non-universal metric factor which determines the overall time scale. This paper also discusses in detail the variational and projection methods that are used to compute relaxation times with high accuracy

    Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

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    PM&lt;sub&gt;1&lt;/sub&gt; (particulate matter with an aerodynamic diameter &lt;1 μm) non-refractory components and black carbon were measured continuously together with additional air quality and atmospheric parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O:C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O:C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. &lt;br&gt;&lt;/br&gt; This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at &lt;i&gt;m/z&lt;/i&gt; 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C&lt;sub&gt;3&lt;/sub&gt;H&lt;sub&gt;3&lt;/sub&gt;O&lt;sup&gt;+&lt;/sup&gt; and C&lt;sub&gt;3&lt;/sub&gt;H&lt;sub&gt;5&lt;/sub&gt;O&lt;sup&gt;+&lt;/sup&gt;, even though their contributions to &lt;i&gt;m/z&lt;/i&gt; 55 and 57 are low compared to the reduced ions C&lt;sub&gt;4&lt;/sub&gt;H&lt;sub&gt;7&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; and C&lt;sub&gt;4&lt;/sub&gt;H&lt;sub&gt;9&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt;. A simple estimation method based on the markers &lt;i&gt;m/z&lt;/i&gt; 55, 57, and 44 is developed here and allows for a first-order-estimation of COA in urban air. This study emphasizes the importance of cooking activities for ambient air quality and confirms the importance of chemical composition measurements with a high mass and time resolution

    Physical tests for Random Numbers in Simulations

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    We propose three physical tests to measure correlations in random numbers used in Monte Carlo simulations. The first test uses autocorrelation times of certain physical quantities when the Ising model is simulated with the Wolff algorithm. The second test is based on random walks, and the third on blocks of n successive numbers. We apply the tests to show that recent errors in high precision simulations using generalized feedback shift register algorithms are due to short range correlations in random number sequences. We also determine the length of these correlations.Comment: 16 pages, Post Script file, HU-TFT-94-
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