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1
Sonnemann, G. R., and M. Grygalashvyly. "Effective CO<sub>2</sub> lifetime and future CO<sub>2</sub> levels based on fit function." Annales Geophysicae 31, no. 9 (2013): 1591–96. http://dx.doi.org/10.5194/angeo-31-1591-2013.
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Abstract. The estimated global CO2 emission rates and the measured atmospheric CO2 concentrations show that only a certain share of the emitted CO2 accumulates in the atmosphere. For given atmospheric emissions of CO2, the effective lifetime determines its accumulation in the atmosphere and, consequently, its impact on the future global warming. We found that on average the inferred effective lifetime of CO2 decreases as its atmospheric concentration increases, reducing the rate of its accumulation in the atmosphere. We derived a power function that fits the varying lifetimes. Based on this fitting function, we calculated the increase of CO2 for different scenarios of future global emission rates.
2
Roelofs, G. J. "A steady-state analysis of the temperature responses of water vapor and aerosol lifetimes." Atmospheric Chemistry and Physics 13, no. 16 (2013): 8245–54. http://dx.doi.org/10.5194/acp-13-8245-2013.
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Abstract. The dominant removal mechanism of soluble aerosol is wet deposition. The atmospheric lifetime of aerosol, relevant for aerosol radiative forcing, is therefore coupled to the atmospheric cycling time of water vapor. This study investigates the coupling between water vapor and aerosol lifetimes in a well-mixed atmosphere. Based on a steady-state study by Pruppacher and Jaenicke (1995) we describe the coupling in terms of the processing efficiency of air by clouds and the efficiencies of water vapor condensation, of aerosol activation, and of the transfer from cloud water to precipitation. We extend this to expressions for the temperature responses of the water vapor and aerosol lifetimes. Previous climate model results (Held and Soden, 2006) suggest a water vapor lifetime temperature response of +5.3 ± 2.0% K−1. This can be used as a first guess for the aerosol lifetime temperature response, but temperature sensitivities of the aerosol lifetime simulated in recent aerosol–climate model studies extend beyond this range and include negative values. This indicates that other influences probably have a larger impact on the computed aerosol lifetime than its temperature response, more specifically changes in the spatial distributions of aerosol (precursor) emissions and precipitation patterns, and changes in the activation efficiency of aerosol. These are not quantitatively evaluated in this study but we present suggestions for model experiments that may help to understand and quantify the different factors that determine the aerosol atmospheric lifetime.
3
Takahashi, K., T. Nakayama, Y. Matsumi, et al. "Atmospheric lifetime of SF5CF3." Geophysical Research Letters 29, no. 15 (2002): 7–1. http://dx.doi.org/10.1029/2002gl015356.
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Hoffmann, L., C. M. Hoppe, R. Müller, et al. "Stratospheric lifetime ratio of CFC-11 and CFC-12 from satellite and model climatologies." Atmospheric Chemistry and Physics 14, no. 22 (2014): 12479–97. http://dx.doi.org/10.5194/acp-14-12479-2014.
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Abstract. Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone loss and are strong infrared absorbers that contribute to global warming. The stratospheric lifetimes of CFCs are a measure of their stratospheric loss rates that are needed to determine global warming and ozone depletion potentials. We applied the tracer–tracer correlation approach to zonal mean climatologies from satellite measurements and model data to assess the lifetimes of CFCl3 (CFC-11) and CF2Cl2 (CFC-12). We present estimates of the CFC-11/CFC-12 lifetime ratio and the absolute lifetime of CFC-12, based on a reference lifetime of 52 years for CFC-11. We analyzed climatologies from three satellite missions, the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), the HIgh Resolution Dynamics Limb Sounder (HIRDLS), and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). We found a CFC-11/CFC-12 lifetime ratio of 0.47±0.08 and a CFC-12 lifetime of 112(96–133) years for ACE-FTS, a ratio of 0.46±0.07 and a lifetime of 113(97–134) years for HIRDLS, and a ratio of 0.46±0.08 and a lifetime of 114(98–136) years for MIPAS. The error-weighted, combined CFC-11/CFC-12 lifetime ratio is 0.46±0.04 and the CFC-12 lifetime estimate is 113(103–124) years. These results agree with the recent Stratosphere-troposphere Processes And their Role in Climate (SPARC) reassessment, which recommends lifetimes of 52(43–67) years and 102(88–122) years, respectively. Having smaller uncertainties than the results from other recent studies, our estimates can help to better constrain CFC-11 and CFC-12 lifetime recommendations in future scientific studies and assessments. Furthermore, the satellite observations were used to validate first simulation results from a new coupled model system, which integrates a Lagrangian chemistry transport model into a climate model. For the coupled model we found a CFC-11/CFC-12 lifetime ratio of 0.48±0.07 and a CFC-12 lifetime of 110(95–129) years, based on a 10-year perpetual run. Closely reproducing the satellite observations, the new model system will likely become a useful tool to assess the impact of advective transport, mixing, and photochemistry as well as climatological variability on the stratospheric lifetimes of long-lived tracers.
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Sodemann, Harald. "Beyond Turnover Time: Constraining the Lifetime Distribution of Water Vapor from Simple and Complex Approaches." Journal of the Atmospheric Sciences 77, no. 2 (2020): 413–33. http://dx.doi.org/10.1175/jas-d-18-0336.1.
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Abstract The time water vapor spends in the atmosphere from evaporation to precipitation, termed here the water vapor lifetime, is of fundamental relevance for characterizing the water cycle, for the turnover of mass and energy, causes of precipitation extremes, and the recycling of precipitation over land. While the global average lifetime of water vapor is commonly considered as about 8–10 days, recent work indicates that the distribution of water vapor lifetimes is highly skewed, and that a large part of the water vapor could have average lifetimes of about 4–5 days. Besides calling for scrutiny of these new estimates, these findings also prompt an investigation of the factors shaping the distribution of the lifetime of water vapor. Using idealized setups and reanalysis data, I explore the influence of heterogeneity and nonstationarity on water vapor age and lifetime. The combination of nonstationarity and heterogeneity allows for short and long local lifetimes and water vapor ages, while maintaining the global average mass balance and corresponding mean water vapor lifetime. A plausibility argument based on humidity-weighted winds suggests that median lifetimes of 4–5 days are more consistent with weather system patterns in the extratropics. I propose that the median of the lifetime is more representative, since its mean value is affected by uncertainty originating from a long, thin tail. To more comprehensively understand the water vapor lifetime, methods will need to report the full lifetime distribution. Simulations with artificial water tracers could thereby provide the framework to compare different methods consistently in the future, while stable water isotopes could serve as an observational constraint.
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Patten, K. O., and D. J. Wuebbles. "Atmospheric lifetimes and ozone depletion potentials of trans-1-chloro-3,3,3-trifluoropropylene and trans-1,2-dichloroethylene in a three-dimensional model." Atmospheric Chemistry and Physics Discussions 10, no. 7 (2010): 16637–57. http://dx.doi.org/10.5194/acpd-10-16637-2010.
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Abstract. The chloroalkenes trans-1-chloro-3,3,3-trifluoropropylene (tCFP) and trans-1,2-dichloroethylene (tDCE) have been proposed as candidate replacements for other compounds in current use that cause concerns regarding potential environmental effects including destruction of stratospheric ozone. Because tCFP and tDCE contain chlorine atoms, the effects of these short-lived compounds on stratospheric ozone must be established. In this study, we derive the atmospheric lifetimes and Ozone Depletion Potentials (ODPs) for tCFP and for tDCE assuming emissions from land surfaces at latitudes 30° N to 60° N using the MOZART 3 three-dimensional model of atmospheric chemistry and physics. Both tCFP and tDCE are shown to primarily affect ozone in the troposphere, rather than in the stratosphere as generally expected from longer-lived chlorocarbons. The atmospheric lifetime of tCFP against chemical reaction is 40.4 days, and its ODP is quite small at 0.00034. The tDCE atmospheric lifetime is 12.7 days, and its ODP is 0.00024, which is the lowest ODP found for any chlorocarbon we have studied. Our study suggests that chlorine from tCFP and tDCE are unlikely to significantly affect ozone at quantities likely to be emitted to the atmosphere.
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Roelofs, G. J. "Aerosol lifetime and climate change." Atmospheric Chemistry and Physics Discussions 12, no. 7 (2012): 16493–514. http://dx.doi.org/10.5194/acpd-12-16493-2012.
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Abstract. The dominant removal mechanism for atmospheric aerosol is activation of particles to cloud droplets and subsequent wet deposition in precipitation. The atmospheric lifetime of aerosol is thus closely coupled to the atmospheric cycling time of water vapor. Changes of hydrological cycle characteristics resulting from climate change therefore directly affect aerosol lifetime, and thus the radiative forcing exerted by aerosol. This study expresses the coupling between water vapor and aerosol lifetimes and their temperature sensitivities in fundamental equations and in terms of the efficiency of processing of air by precipitating clouds. Based on climate model simulations these temperature sensitivities are estimated to be on the order of +5.3% K−1, but this may be an overestimation. Generally, shifting spatial and temporal patterns of aerosol (precursor) emissions and precipitation, and changes in aerosol activation efficiency probably influence aerosol lifetimes more than climate change itself, resulting in a wide range of simulated aerosol lifetime sensitivities between aerosol-climate models. It is possible that the climate sensitivity of models plays a role. It can be argued that climate sensitivity is intrinsically coupled with the simulated (temperature sensitivity of the) aerosol lifetime through the distribution of water vapor and aerosol between the lower and upper troposphere. This implies a fundamental relation between various feedback forcings (water vapor, lapse rate, cloud) and the aerosol forcing, illustrating the key role of the hydrological cycle in different aspects of the climate system.
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Patten, K. O., and D. J. Wuebbles. "Atmospheric lifetimes and Ozone Depletion Potentials of trans-1-chloro-3,3,3-trifluoropropylene and trans-1,2-dichloroethylene in a three-dimensional model." Atmospheric Chemistry and Physics 10, no. 22 (2010): 10867–74. http://dx.doi.org/10.5194/acp-10-10867-2010.
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Abstract. The chloroalkenes trans-1-chloro-3,3,3-trifluoropropylene (tCFP) and trans-1,2-dichloroethylene (tDCE) have been proposed as candidate replacements for other compounds in current use that cause concerns regarding potential environmental effects including destruction of stratospheric ozone. Because tCFP and tDCE contain chlorine atoms, the effects of these short-lived compounds on stratospheric ozone must be established. In this study, we derive the atmospheric lifetimes and Ozone Depletion Potentials (ODPs) for tCFP and for tDCE assuming emissions from land surfaces at latitudes 30° N to 60° N using the MOZART 3 three-dimensional model of atmospheric chemistry and physics. 53% of the ozone loss due to tCFP and 98% of the ozone loss due to tDCE take place in the troposphere, rather than in the stratosphere as generally expected from longer-lived chlorocarbons. The atmospheric lifetime of tCFP against chemical reaction is 40.4 days, and its ODP is quite small at 0.00034. The tDCE atmospheric lifetime is 12.7 days, and its ODP is 0.00024, which is the lowest ODP found for any chlorocarbon we have studied. Our study suggests that chlorine from tCFP and tDCE are unlikely to affect ozone at quantities likely to be emitted to the atmosphere.
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Brown, A. T., C. M. Volk, M. R. Schoeberl, C. D. Boone, and P. F. Bernath. "Stratospheric lifetimes of CFC-12, CCl<sub>4</sub>, CH<sub>4</sub>, CH<sub>3</sub>Cl and N<sub>2</sub>O from measurements made by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)." Atmospheric Chemistry and Physics Discussions 13, no. 2 (2013): 4221–87. http://dx.doi.org/10.5194/acpd-13-4221-2013.
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Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer-tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the VMR from tropical ground-based AGAGE sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 195 + (−) 75 (42) yr (CH4), 69 + (−) 65 (23) yr (CH3Cl) and 123 + (−) 53 (28) yr (N2O). The errors on these values are the weighted 1-σ non-systematic errors. The stratospheric lifetime of CH3Cl represents the first calculations of the stratospheric lifetime of CH3Cl using data from a space based instrument.
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Kepros, John G., and Greg Davidson. "Atmospheric Heating and Hubble's Lifetime." Physics Today 47, no. 1 (1994): 68–69. http://dx.doi.org/10.1063/1.2808393.
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Ellis, D. A., J. W. Martin, S. A. Mabury, M. D. Hurley, M. P. Sulbaek Andersen, and T. J. Wallington. "Atmospheric Lifetime of Fluorotelomer Alcohols." Environmental Science & Technology 37, no. 17 (2003): 3816–20. http://dx.doi.org/10.1021/es034136j.
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Fischer, Gaston. "Atmospheric lifetime of carbon dioxide." Population and Environment 10, no. 3 (1989): 177–81. http://dx.doi.org/10.1007/bf01257903.
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Hoffmann, L., C. M. Hoppe, R. Müller, et al. "Stratospheric lifetime ratio of CFC-11 and CFC-12 from satellite and model climatologies." Atmospheric Chemistry and Physics Discussions 14, no. 11 (2014): 16865–906. http://dx.doi.org/10.5194/acpd-14-16865-2014.
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Abstract. Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone loss and are strong infrared absorbers that contribute to global warming. The stratospheric lifetimes of CFCs are a measure of their global loss rates that are needed to determine global warming and ozone depletion potentials. We applied the tracer-tracer correlation approach to zonal mean climatologies from satellite measurements and model data to assess the lifetimes of CFCl3 (CFC-11) and CF2Cl2 (CFC-12). We present estimates of the CFC-11/CFC-12 lifetime ratio and the absolute lifetime of CFC-12, based on a reference lifetime of 52 yr for CFC-11. We analyzed climatologies from three satellite missions, the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), the HIgh Resolution Dynamics Limb Sounder (HIRDLS), and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). We found a CFC-11/CFC-12 lifetime ratio of 0.47±0.08 and a CFC-12 lifetime of 111(96–132) yr for ACE-FTS, a ratio of 0.46±0.07 and a lifetime of 112(97–133) yr for HIRDLS, and a ratio of 0.46±0.08 and a lifetime of 112(96–135) yr for MIPAS. The error-weighted, combined CFC-11/CFC-12 lifetime ratio is 0.47±0.04 and the CFC-12 lifetime estimate is 112(102–123) yr. These results agree with the recent Stratosphere-troposphere Processes And their Role in Climate (SPARC) reassessment, which recommends lifetimes of 52(43–67) yr and 102(88–122) yr, respectively. Having smaller uncertainties than the results from other recent studies, our estimates can help to better constrain CFC-11 and CFC-12 lifetime recommendations in future scientific studies and assessments. Furthermore, the satellite observations were used to validate first simulation results from a new coupled model system, which integrates a Lagrangian chemistry transport model into a climate model. For the coupled model we found a CFC-11/CFC-12 lifetime ratio of 0.48±0.07 and a CFC-12 lifetime of 110(95–129) yr, based on a ten-year perpetual run. Closely reproducing the satellite observations, the new model system will likely become a useful tool to assess the impact of advective transport, mixing, and photochemistry as well as climatological variability on the stratospheric lifetimes of long-lived tracers.
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Wang, Peidong, Jeffery R. Scott, Susan Solomon, et al. "On the effects of the ocean on atmospheric CFC-11 lifetimes and emissions." Proceedings of the National Academy of Sciences 118, no. 12 (2021): e2021528118. http://dx.doi.org/10.1073/pnas.2021528118.
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The ocean is a reservoir for CFC-11, a major ozone-depleting chemical. Anthropogenic production of CFC-11 dramatically decreased in the 1990s under the Montreal Protocol, which stipulated a global phase out of production by 2010. However, studies raise questions about current overall emission levels and indicate unexpected increases of CFC-11 emissions of about 10 Gg ⋅ yr−1 after 2013 (based upon measured atmospheric concentrations and an assumed atmospheric lifetime). These findings heighten the need to understand processes that could affect the CFC-11 lifetime, including ocean fluxes. We evaluate how ocean uptake and release through 2300 affects CFC-11 lifetimes, emission estimates, and the long-term return of CFC-11 from the ocean reservoir. We show that ocean uptake yields a shorter total lifetime and larger inferred emission of atmospheric CFC-11 from 1930 to 2075 compared to estimates using only atmospheric processes. Ocean flux changes over time result in small but not completely negligible effects on the calculated unexpected emissions change (decreasing it by 0.4 ± 0.3 Gg ⋅ yr−1). Moreover, it is expected that the ocean will eventually become a source of CFC-11, increasing its total lifetime thereafter. Ocean outgassing should produce detectable increases in global atmospheric CFC-11 abundances by the mid-2100s, with emission of around 0.5 Gg ⋅ yr−1; this should not be confused with illicit production at that time. An illustrative model projection suggests that climate change is expected to make the ocean a weaker reservoir for CFC-11, advancing the detectable change in the global atmospheric mixing ratio by about 5 yr.
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Williams, Jonathan, and Akima Ringsdorf. "Human odour thresholds are tuned to atmospheric chemical lifetimes." Philosophical Transactions of the Royal Society B: Biological Sciences 375, no. 1800 (2020): 20190274. http://dx.doi.org/10.1098/rstb.2019.0274.
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In this study, the odour thresholds (OT) and atmospheric lifetimes (AL) were compared for a suite of volatile organic compounds. It was found that odour threshold, as determined by the triangle bag method, correlated surprisingly well with atmospheric lifetime for a given chemical family. Molecules with short atmospheric lifetimes with respect to the primary atmospheric oxidant OH tend to be more sensitively detected by the human nose. Overall the correlation of odour threshold with atmospheric lifetime was better than with mass and vapour pressure. Several outliers from the correlations for particular chemical families were examined in detail. For example, diacetyl was an outlier in the ketone dataset that fitted the trend when its more important photolysis lifetime was included; and similarly, the relatively low odour threshold of carbonyl sulfide (OCS) was interpreted in terms of uptake by vegetation. The OT/AL relationship suggests that OH rate constants can be used as a first-order estimate for odour thresholds (and vice versa ). We speculate that the nose's high sensitivity to chemicals that are reactive in the air is likely an evolved rather than a learned condition. This is based on the lack of dependence on ozone in the aliphatics, that the anthropogenically emitted aromatic compounds had the worst correlation, and that OCS had a much lower than predicted OT. Finally, we use the OT/AL relationships derived to predict odour thresholds and rate constants that have not yet been determined in order to provide a test to this hypothesis. This article is part of the Theo Murphy meeting issue ‘Olfactory communication in humans’.
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Rigby, M., R. G. Prinn, S. O'Doherty, et al. "Re-evaluation of the lifetimes of the major CFCs and CH<sub>3</sub>CCl<sub>3</sub> using atmospheric trends." Atmospheric Chemistry and Physics 13, no. 5 (2013): 2691–702. http://dx.doi.org/10.5194/acp-13-2691-2013.
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Abstract. Since the Montreal Protocol on Substances that Deplete the Ozone Layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH3CCl3, have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to relatively low levels, therefore the rate at which this recovery occurs will depend largely on the atmospheric lifetime of these compounds. The first ODS measurements began in the early 1970s along with the first lifetime estimates calculated by considering their atmospheric trends. We now have global mole fraction records spanning multiple decades, prompting this lifetime re-evaluation. Using surface measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration Global Monitoring Division (NOAA GMD) from 1978 to 2011, we estimated the lifetime of CFC-11, CFC-12, CFC-113 and CH3CCl3 using a multi-species inverse method. A steady-state lifetime of 45 yr for CFC-11, currently recommended in the most recent World Meteorological Organisation (WMO) Scientific Assessments of Ozone Depletion, lies towards the lower uncertainty bound of our estimates, which are 544861 yr (1-sigma uncertainty) when AGAGE data were used and 524561 yr when the NOAA network data were used. Our derived lifetime for CFC-113 is significantly higher than the WMO estimates of 85 yr, being 10999121 (AGAGE) and 10997124 (NOAA). New estimates of the steady-state lifetimes of CFC-12 and CH3CCl3 are consistent with the current WMO recommendations, being 11195132 and 11295136 yr (CFC-12, AGAGE and NOAA respectively) and 5.044.925.20 and 5.044.875.23 yr (CH3CCl3, AGAGE and NOAA respectively).
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Kopylov, S. N., P. S. Kopylov, I. P. Eltyshev, and I. R. Begishev. "Characteristics of Impact on the Atmosphere of Perfluorisohexenes - Promising Components of Gas Extinguishing Compositions." Journal of Physics: Conference Series 2389, no. 1 (2022): 012003. http://dx.doi.org/10.1088/1742-6596/2389/1/012003.
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Abstract Ecological properties of perfluorohexenes are studied in the paper. C6F12 atmospheric lifetime of 17.4 days was obtained using one-dimensional photochemical model. It was shown that the substance disappears in the atmosphere due to its reactions mostly with OH radicals. Absorption spectra of C6F12 in the short-wavelength ultraviolet region of 110-200 nm and in the infrared region were calculated using the Gaussian 09 quantum mechanical calculation program. Calculations revealed that C6F12 has significant absorption in the infrared region but due to short atmospheric lifetime of this substance its global warming potential GWP is as low as 28.64. Ozone depleting potential (ODP) of perfluoroisohexenes is equal to zero due to short chain length for the chain processes of ozone destruction involving fluorine atoms. Thus, perfluoroisohexenes with their zero ODP, short atmospheric lifetime and low GWP meet all modern environmental requirements and can be considered as effective substitutes for high-GWP HFCs in fire suppression.
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Miller-Ricci, Eliza, Sara Seager, and Dimitar Sasselov. "The Atmospheres of Extrasolar Super-Earths." Proceedings of the International Astronomical Union 4, S253 (2008): 263–71. http://dx.doi.org/10.1017/s1743921308026483.
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AbstractExtrasolar super-Earths (1-10 M⊕) are likely to exist with a wide range of atmospheres. While a number of these planets have already been discovered through radial velocities and microlensing, it will be the discovery of the firsttransitingsuper-Earths that will open the door to a variety of follow-up observations aimed at characterizing their atmospheres. Super-Earths may fill a large range of parameter space in terms of their atmospheric composition and mass. Specifically, some of these planets may have high enough surface gravities to be able to retain large hydrogen-rich atmosphseres, while others will have lost most of their hydrogen to space over the planet's lifetime, leaving behind an atmosphere more closely resembling that of Earth or Venus. The resulting composition of the super-Earth atmosphere will therefore depend strongly on factors such as atmospheric escape history, outgassing history, and the level of stellar irradiation that it receives. Here we present theoretical models of super-Earth emission and transmission spectra for a variety of possible outcomes of super-Earth atmospheric composition ranging from hydrogen-rich to hydrogen-poor. We focus on how observations can be used to differentiate between the various scenarios and constrain atmospheric composition.
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Larin, I. K. "Odd oxygen and its atmospheric lifetime." Russian Journal of Physical Chemistry B 11, no. 2 (2017): 375–79. http://dx.doi.org/10.1134/s1990793117020075.
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Cape, J. N., M. Coyle, and P. Dumitrean. "The atmospheric lifetime of black carbon." Atmospheric Environment 59 (November 2012): 256–63. http://dx.doi.org/10.1016/j.atmosenv.2012.05.030.
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Kennett, E. J., and R. Toumi. "Temperature dependence of atmospheric moisture lifetime." Geophysical Research Letters 32, no. 19 (2005): n/a. http://dx.doi.org/10.1029/2005gl023936.
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Jäggi, Noah, Diana Gamborino, Dan J. Bower, et al. "Evolution of Mercury’s Earliest Atmosphere." Planetary Science Journal 2, no. 6 (2021): 230. http://dx.doi.org/10.3847/psj/ac2dfb.
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Abstract MESSENGER observations suggest a magma ocean formed on proto-Mercury, during which evaporation of metals and outgassing of C- and H-bearing volatiles produced an early atmosphere. Atmospheric escape subsequently occurred by plasma heating, photoevaporation, Jeans escape, and photoionization. To quantify atmospheric loss, we combine constraints on the lifetime of surficial melt, melt composition, and atmospheric composition. Consideration of two initial Mercury sizes and four magma ocean compositions determines the atmospheric speciation at a given surface temperature. A coupled interior–atmosphere model determines the cooling rate and therefore the lifetime of surficial melt. Combining the melt lifetime and escape flux calculations provides estimates for the total mass loss from early Mercury. Loss rates by Jeans escape are negligible. Plasma heating and photoionization are limited by homopause diffusion rates of ∼106 kg s−1. Loss by photoevaporation depends on the timing of Mercury formation and assumed heating efficiency and ranges from ∼106.6 to ∼109.6 kg s−1. The material for photoevaporation is sourced from below the homopause and is therefore energy limited rather than diffusion limited. The timescale for efficient interior–atmosphere chemical exchange is less than 10,000 yr. Therefore, escape processes only account for an equivalent loss of less than 2.3 km of crust (0.3% of Mercury’s mass). Accordingly, ≤0.02% of the total mass of H2O and Na is lost. Therefore, cumulative loss cannot significantly modify Mercury’s bulk mantle composition during the magma ocean stage. Mercury’s high core:mantle ratio and volatile-rich surface may instead reflect chemical variations in its building blocks resulting from its solar-proximal accretion environment.
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Hou, Pei, Shiliang Wu, Jessica L. McCarty, and Yang Gao. "Sensitivity of atmospheric aerosol scavenging to precipitation intensity and frequency in the context of global climate change." Atmospheric Chemistry and Physics 18, no. 11 (2018): 8173–82. http://dx.doi.org/10.5194/acp-18-8173-2018.
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Abstract. Wet deposition driven by precipitation is an important sink for atmospheric aerosols and soluble gases. We investigate the sensitivity of atmospheric aerosol lifetimes to precipitation intensity and frequency in the context of global climate change. Our sensitivity model simulations, through some simplified perturbations to precipitation in the GEOS-Chem model, show that the removal efficiency and hence the atmospheric lifetime of aerosols have significantly higher sensitivities to precipitation frequencies than to precipitation intensities, indicating that the same amount of precipitation may lead to different removal efficiencies of atmospheric aerosols. Combining the long-term trends of precipitation patterns for various regions with the sensitivities of atmospheric aerosol lifetimes to various precipitation characteristics allows us to examine the potential impacts of precipitation changes on atmospheric aerosols. Analyses based on an observational dataset show that precipitation frequencies in some regions have decreased in the past 14 years, which might increase the atmospheric aerosol lifetimes in those regions. Similar analyses based on multiple reanalysis meteorological datasets indicate that the changes of precipitation intensity and frequency over the past 30 years can lead to perturbations in the atmospheric aerosol lifetimes by 10 % or higher at the regional scale.
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Sun, Xiaomin, Chenxi Zhang, Yuyang Zhao, Jing Bai, and Maoxia He. "Kinetic study on the linalool ozonolysis reaction in the atmosphere." Canadian Journal of Chemistry 90, no. 4 (2012): 353–61. http://dx.doi.org/10.1139/v2012-001.
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In the atmosphere, linalool ozonolysis will generate a series of oxidation products and then form particles through nucleation. In this study, the linalool ozonolysis mechanisms were studied and some of the main products detected from experiment are verified. The Rice–Ramsperger–Kassel–Marcus (RRKM) theory and the canonical variational transition state theory (CVT) with small curvature tunneling effect (SCT) are used to calculate rate constants over the temperature range of 200∼800 K. The total rate constant for the reaction of ozone with linalool is 4.50 × 10−16 cm3 molecule–l s–l, and the addition of ozone to (CH3)2C=CH– is the main ozone addition position. Furthermore, the Arrhenius formulas are fitted and the lifetimes of reaction species in the troposphere are discussed for the first time. The total atmospheric lifetime of linalool relative to O3 is 2.30 h. The O3-initiated atmospheric lifetimes of P1, P3, and P6 are 2.64 months, 16.67 days, and 15.5 h, respectively.
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Croft, B., J. R. Pierce, and R. V. Martin. "Interpreting aerosol lifetimes using the GEOS-Chem model and constraints from radionuclide measurements." Atmospheric Chemistry and Physics 14, no. 8 (2014): 4313–25. http://dx.doi.org/10.5194/acp-14-4313-2014.
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Abstract. Aerosol removal processes control global aerosol abundance, but the rate of that removal remains uncertain. A recent study of aerosol-bound radionuclide measurements after the Fukushima Daiichi nuclear power plant accident documents 137Cs removal (e-folding) times of 10.0–13.9 days, suggesting that mean aerosol lifetimes in the range of 3–7 days in global models might be too short by a factor of two. In this study, we attribute this discrepancy to differences between the e-folding and mean aerosol lifetimes. We implement a simulation of 137Cs and 133Xe into the GEOS-Chem chemical transport model and examine the removal rates for the Fukushima case. We find a general consistency between modelled and measured e-folding times. The simulated 137Cs global burden e-folding time is about 14 days. However, the simulated mean lifetime of aerosol-bound 137Cs over a 6-month post-accident period is only 1.8 days. We find that the mean lifetime depends strongly on the removal rates in the first few days after emissions, before the aerosols leave the boundary layer and are transported to altitudes and latitudes where lifetimes with respect to wet removal are longer by a few orders of magnitude. We present sensitivity simulations that demonstrate the influence of differences in altitude and location of the radionuclides on the mean lifetime. Global mean lifetimes are shown to strongly depend on the altitude of injection. The global mean 137Cs lifetime is more than one order of magnitude greater for the injection at 7 km than into the boundary layer above the Fukushima site. Instantaneous removal rates are slower during the first few days after the emissions for a free tropospheric versus boundary layer injection and this strongly controls the mean lifetimes. Global mean aerosol lifetimes for the GEOS-Chem model are 3–6 days, which is longer than that for the 137Cs injected at the Fukushima site (likely due to precipitation shortly after Fukushima emissions), but similar to the mean lifetime of 3.9 days for the 137Cs emissions injected with a uniform spread through the model's Northern Hemisphere boundary layer. Simulated e-folding times were insensitive to emission parameters (altitude, location, and time), suggesting that these measurement-based e-folding times provide arobust constraint on simulated e-folding times. Despite the reasonable global mean agreement of GEOS-Chem with measurement e-folding times, site by site comparisons yield differences of up to a factor of two, which suggest possible deficiencies in either the model transport, removal processes or the representation of 137Cs removal, particularly in the tropics and at high latitudes. There is an ongoing need to develop constraints on aerosol lifetimes, but these measurement-based constraints must be carefully interpreted given the sensitivity of mean lifetimes and e-folding times to both mixing and removal processes.
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Wuebbles, D. J., K. O. Patten, D. Wang, D. Youn, M. Martínez-Avilés, and J. S. Francisco. "Three-dimensional model evaluation of the Ozone Depletion Potentials for n-propyl bromide, trichloroethylene and perchloroethylene." Atmospheric Chemistry and Physics 11, no. 5 (2011): 2371–80. http://dx.doi.org/10.5194/acp-11-2371-2011.
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Abstract. The existing solvents trichloroethylene (TCE) and perchloroethylene (PCE) and proposed solvent n-propyl bromide (nPB) have atmospheric lifetimes from days to a few months, but contain chlorine or bromine that could affect stratospheric ozone. Several previous studies estimated the Ozone Depletion Potentials (ODPs) for various assumptions of nPB emissions location, but these studies used simplified modeling treatments. The primary purpose of this study is to reevaluate the ODP for n-propyl bromide (nPB) using a current-generation chemistry-transport model of the troposphere and stratosphere. For the first time, ODPs for TCE and PCE are also evaluated in a three-dimensional, global atmospheric chemistry-transport model. Emissions representing industrial use of each compound are incorporated on land surfaces from 30° N to 60° N. The atmospheric chemical lifetime obtained for nPB is 24.7 days, similar to past literature, but the ODP is 0.0049, lower than in our past study of nPB. The derived atmospheric lifetime for TCE is 13.0 days and for PCE is 111 days. The corresponding ODPs are 0.00037 and 0.0050, respectively.
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Wuebbles, D. J., K. O. Patten, D. Wang, D. Youn, M. Martínez-Avilés, and J. S. Francisco. "Three-dimensional model evaluation of the Ozone Depletion Potentials for n-propyl bromide, trichloroethylene and perchloroethylene." Atmospheric Chemistry and Physics Discussions 10, no. 7 (2010): 17889–910. http://dx.doi.org/10.5194/acpd-10-17889-2010.
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Abstract. The existing solvents trichloroethylene (TCE) and perchloroethylene (PCE) and proposed solvent n-propyl bromide (nPB) have atmospheric lifetimes from days to a few months, but contain chlorine or bromine that could affect stratospheric ozone. Several previous studies estimated the Ozone Depletion Potentials (ODPs) for various assumptions for location of nPB emissions, but these studies used simplified modeling treatments. The primary purpose of this study is to reevaluate the ODP for nPB using a current-generation chemistry-transport model of the troposphere and stratosphere. For the first time, ODPs for TCE and PCE are also evaluated. Emissions representing industrial use of each compound are incorporated on land surfaces from 30° N to 60° N. The atmospheric chemical lifetime obtained for nPB is 24.7 days, similar to past literature, but the ODP is 0.0049, lower than in past studies. The derived atmospheric lifetime for TCE is 13.0 days and for PCE is 111 days. The corresponding ODPs are 0.00035 and 0.0060, respectively.
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Kristiansen, N. I., A. Stohl, D. J. L. Olivié, et al. "Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models." Atmospheric Chemistry and Physics 16, no. 5 (2016): 3525–61. http://dx.doi.org/10.5194/acp-16-3525-2016.
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Abstract. Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.
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Saiz-Lopez, Alfonso, Oleg Travnikov, Jeroen E. Sonke, et al. "Photochemistry of oxidized Hg(I) and Hg(II) species suggests missing mercury oxidation in the troposphere." Proceedings of the National Academy of Sciences 117, no. 49 (2020): 30949–56. http://dx.doi.org/10.1073/pnas.1922486117.
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Mercury (Hg), a global contaminant, is emitted mainly in its elemental form Hg0to the atmosphere where it is oxidized to reactive HgIIcompounds, which efficiently deposit to surface ecosystems. Therefore, the chemical cycling between the elemental and oxidized Hg forms in the atmosphere determines the scale and geographical pattern of global Hg deposition. Recent advances in the photochemistry of gas-phase oxidized HgIand HgIIspecies postulate their photodissociation back to Hg0as a crucial step in the atmospheric Hg redox cycle. However, the significance of these photodissociation mechanisms on atmospheric Hg chemistry, lifetime, and surface deposition remains uncertain. Here we implement a comprehensive and quantitative mechanism of the photochemical and thermal atmospheric reactions between Hg0, HgI, and HgIIspecies in a global model and evaluate the results against atmospheric Hg observations. We find that the photochemistry of HgIand HgIIleads to insufficient Hg oxidation globally. The combined efficient photoreduction of HgIand HgIIto Hg0competes with thermal oxidation of Hg0, resulting in a large model overestimation of 99% of measured Hg0and underestimation of 51% of oxidized Hg and ∼66% of HgIIwet deposition. This in turn leads to a significant increase in the calculated global atmospheric Hg lifetime of 20 mo, which is unrealistically longer than the 3–6-mo range based on observed atmospheric Hg variability. These results show that the HgIand HgIIphotoreduction processes largely offset the efficiency of bromine-initiated Hg0oxidation and reveal missing Hg oxidation processes in the troposphere.
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Brown, A. T., C. M. Volk, M. R. Schoeberl, C. D. Boone, and P. F. Bernath. "Stratospheric lifetimes of CFC-12, CCl<sub>4</sub>, CH<sub>4</sub>, CH<sub>3</sub>Cl and N<sub>2</sub>O from measurements made by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)." Atmospheric Chemistry and Physics 13, no. 14 (2013): 6921–50. http://dx.doi.org/10.5194/acp-13-6921-2013.
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Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long-term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer–tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the volume mixing ratio (VMR) from tropical ground based AGAGE (Advanced Global Atmospheric Gases Experiment) sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 69 + (−) 65 (23) yr (CH3Cl), 123 + (−) 53 (28) yr (N2O) and 195 + (−) 75 (42) yr (CH4). The errors on these values are the weighted 1σ non-systematic errors. Systematic errors were estimated by recalculating lifetimes using VMRs which had been modified to reflect differences between ACE-FTS retrieved VMRs and those from other instruments. The results of these calculations, including systematic errors, were as follows: 113 + (−) 32 (20) for CFC-12, 123 + (−) 83 (35) for N2O, 195 + (−) 139 (57) for CH4, 35 + (−) 14 (8) for CCl4 and 69 + (−) 2119 (34) yr for CH3Cl. For CH3Cl &amp; CH4 this represents the first calculation of the stratospheric lifetime using data from a space based instrument.
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Keßel, Stephan, David Cabrera-Perez, Abraham Horowitz, et al. "Atmospheric chemistry, sources and sinks of carbon suboxide, C<sub>3</sub>O<sub>2</sub>." Atmospheric Chemistry and Physics 17, no. 14 (2017): 8789–804. http://dx.doi.org/10.5194/acp-17-8789-2017.
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Abstract. Carbon suboxide, O = C = C = C = O, has been detected in ambient air samples and has the potential to be a noxious pollutant and oxidant precursor; however, its lifetime and fate in the atmosphere are largely unknown. In this work, we collect an extensive set of studies on the atmospheric chemistry of C3O2. Rate coefficients for the reactions of C3O2 with OH radicals and ozone were determined as kOH = (2.6 ± 0.5) × 10−12 cm3 molecule−1 s−1 at 295 K (independent of pressure between ∼ 25 and 1000 mbar) and kO3 < 1.5 × 10−21 cm3 molecule−1 s−1 at 295 K. A theoretical study on the mechanisms of these reactions indicates that the sole products are CO and CO2, as observed experimentally. The UV absorption spectrum and the interaction of C3O2 with water (Henry's law solubility and hydrolysis rate constant) were also investigated, enabling its photodissociation lifetime and hydrolysis rates, respectively, to be assessed. The role of C3O2 in the atmosphere was examined using in situ measurements, an analysis of the atmospheric sources and sinks and simulation with the EMAC atmospheric chemistry–general circulation model. The results indicate sub-pptv levels at the Earth's surface, up to about 10 pptv in regions with relatively strong sources, e.g. influenced by biomass burning, and a mean lifetime of ∼ 3.2 days. These predictions carry considerable uncertainty, as more measurement data are needed to determine ambient concentrations and constrain the source strengths.
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Archer, David, Michael Eby, Victor Brovkin, et al. "Atmospheric Lifetime of Fossil Fuel Carbon Dioxide." Annual Review of Earth and Planetary Sciences 37, no. 1 (2009): 117–34. http://dx.doi.org/10.1146/annurev.earth.031208.100206.
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Moore, Berrien, and B. H. Braswell. "The lifetime of excess atmospheric carbon dioxide." Global Biogeochemical Cycles 8, no. 1 (1994): 23–38. http://dx.doi.org/10.1029/93gb03392.
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Archer, David, and Victor Brovkin. "The millennial atmospheric lifetime of anthropogenic CO2." Climatic Change 90, no. 3 (2008): 283–97. http://dx.doi.org/10.1007/s10584-008-9413-1.
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Wang, Jian, Lei Xue, Qianyao Ma, et al. "The role of oceanic ventilation and terrestrial outflow in atmospheric non-methane hydrocarbons over the Chinese marginal seas." Atmospheric Chemistry and Physics 24, no. 15 (2024): 8721–36. http://dx.doi.org/10.5194/acp-24-8721-2024.
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Abstract. Non-methane hydrocarbons (NMHCs) in the marine atmosphere have been studied extensively due to their important roles in regulating atmospheric chemistry and climate. However, very little is known about the distribution and sources of NMHCs in the lower atmosphere over the marginal seas of China. Herein, we characterized the atmospheric NMHCs (C2–C5) in both the coastal cities and the marginal seas of China in the spring of 2021, with a focus on identifying the sources of NMHCs in the coastal atmosphere. The NMHCs in urban atmospheres, especially alkanes, were significantly higher compared to those in the marine atmosphere, suggesting that terrestrial NMHCs may be an important reservoir/source in the marine atmosphere. A significant correlation was observed between the alkane concentrations and the distances from sampling sites to the nearest land or retention of air mass over land, indicating that alkanes in the marine atmosphere are largely influenced by terrestrial inputs through air mass transport. For alkenes, a greater impact from oceanic emissions was determined due to the lower terrestrial concentrations, short atmospheric lifetime, and substantial sea-to-air fluxes of alkenes compared to alkanes (489 ± 454 vs. 129 ± 106 nmol m−2 d−1). As suggested by the positive matrix factorization, terrestrial inputs contributed to 89 % of alkanes and 69.6 % of alkenes in Chinese marginal seas, subsequently contributing to 84 % of the ozone formation potential associated with C2–C5 NMHCs. These findings underscore the significance of terrestrial outflow in controlling the distribution and composition of atmospheric NMHCs in the marginal seas of China.
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Yates, Jack S., Paul I. Palmer, James Manners, et al. "Ozone chemistry on tidally locked M dwarf planets." Monthly Notices of the Royal Astronomical Society 492, no. 2 (2020): 1691–705. http://dx.doi.org/10.1093/mnras/stz3520.
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ABSTRACT We use the Met Office Unified Model to explore the potential of a tidally locked M dwarf planet, nominally Proxima Centauri b irradiated by a quiescent version of its host star, to sustain an atmospheric ozone layer. We assume a slab ocean surface layer, and an Earth-like atmosphere of nitrogen and oxygen with trace amounts of ozone and water vapour. We describe ozone chemistry using the Chapman mechanism and the hydrogen oxide (HOx, describing the sum of OH and HO2) catalytic cycle. We find that Proxima Centauri radiates with sufficient UV energy to initialize the Chapman mechanism. The result is a thin but stable ozone layer that peaks at 0.75 parts per million at 25 km. The quasi-stationary distribution of atmospheric ozone is determined by photolysis driven by incoming stellar radiation and by atmospheric transport. Ozone mole fractions are smallest in the lowest 15 km of the atmosphere at the substellar point and largest in the nightside gyres. Above 15 km the ozone distribution is dominated by an equatorial jet stream that circumnavigates the planet. The nightside ozone distribution is dominated by two cyclonic Rossby gyres that result in localized ozone hotspots. On the dayside the atmospheric lifetime is determined by the HOx catalytic cycle and deposition to the surface, with nightside lifetimes due to chemistry much longer than time-scales associated with atmospheric transport. Surface UV values peak at the substellar point with values of 0.01 W m−2, shielded by the overlying atmospheric ozone layer but more importantly by water vapour clouds.
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Deters, B., J. P. Burrows, S. Himmelmann, and C. Blindauer. "Gas phase spectra of HOBr and Br2O and their atmospheric significance." Annales Geophysicae 14, no. 4 (1996): 468–75. http://dx.doi.org/10.1007/s00585-996-0468-x.
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Abstract. The HOBr molecule is a potential reservoir of Br compounds in the atmosphere. In this work, the UV-visible spectrum of HOBr was measured over the range 242–400 nm. Its absorption consists of two maxima at 280 nm (σmax=2.7±0.4×10–19 cm2 molecules–1) and 355 nm (σmax=7.0±1.1×10–20 cm2 molecules–1), respectively, where the error is ±1Σ. Atmospheric photolysis lifetime calculations for HOBr in the lower stratosphere have been made using the PHOTOGT model. The results show a strong dependence on the solar zenith angle (SZA) implying a longer lifetime at high latitudes and a relatively short lifetime at low latitudes for example 714 s (albedo of 25%, SZA of 20° and an altitude of 17 km), and 3226 s (albedo of 25%, SZA of 88° and an altitude of 17 km). The UV-visible absorption spectrum of Br2O, which is an intermediate in the preparation, used in this study and is together with H2O in equilibrium with HOBr, was measured from 205 to 450 nm. The spectrum shows a maximum at 315 nm (σmax=2.3±0.3×10–18 cm2 molecules–1) with a shoulder at 355 nm. From the results of the atmospheric lifetime calculations for Br2O, it is clear that this molecule has a short stratospheric lifetime and is not likely to have a large daytime concentration, for example, 20 s (albedo of 25%, SZA of 20° and an altitude of 17 km), and 83 s (albedo and 25%, SZA of 88° and an altitude of 17 km).
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Kovács, Tamás, Wuhu Feng, Anna Totterdill, et al. "Determination of the atmospheric lifetime and global warming potential of sulfur hexafluoride using a three-dimensional model." Atmospheric Chemistry and Physics 17, no. 2 (2017): 883–98. http://dx.doi.org/10.5194/acp-17-883-2017.
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Abstract. We have used the Whole Atmosphere Community Climate Model (WACCM), with an updated treatment of loss processes, to determine the atmospheric lifetime of sulfur hexafluoride (SF6). The model includes the following SF6 removal processes: photolysis, electron attachment and reaction with mesospheric metal atoms. The Sodankylä Ion Chemistry (SIC) model is incorporated into the standard version of WACCM to produce a new version with a detailed D region ion chemistry with cluster ions and negative ions. This is used to determine a latitude- and altitude-dependent scaling factor for the electron density in the standard WACCM in order to carry out multi-year SF6 simulations. The model gives a mean SF6 lifetime over an 11-year solar cycle (τ) of 1278 years (with a range from 1120 to 1475 years), which is much shorter than the currently widely used value of 3200 years, due to the larger contribution (97.4 %) of the modelled electron density to the total atmospheric loss. The loss of SF6 by reaction with mesospheric metal atoms (Na and K) is far too slow to affect the lifetime. We investigate how this shorter atmospheric lifetime impacts the use of SF6 to derive stratospheric age of air. The age of air derived from this shorter lifetime SF6 tracer is longer by 9 % in polar latitudes at 20 km compared to a passive SF6 tracer. We also present laboratory measurements of the infrared spectrum of SF6 and find good agreement with previous studies. We calculate the resulting radiative forcings and efficiencies to be, on average, very similar to those reported previously. Our values for the 20-, 100- and 500-year global warming potentials are 18 000, 23 800 and 31 300, respectively.
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Al-Zaidi, H. K., M. J. Al-Bermani, and A. M. Taleb. "Estimating the lifetime and Reentry of the Aluminum Space Debris of Sizes (1 and 10 cm) in LEO under Atmosphere Drag Effects." Journal of Kufa-Physics 12, no. 02 (2020): 66–75. http://dx.doi.org/10.31257/2018/jkp/2020/120207.
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This study attempts to address the lifetime and reentry of the space debris in low earth orbit LEO which extends from 200 to 1200 km. In this study a new Computer programs were designed to simulate the orbit dynamics of space debris lifetime and reentry under atmospheric drag force using Runge-Kutta Method to solve the differential equations of drag force. This model was adapted with the Drag Thermosphere Model (DTM78, 94), the Aluminum 2024 space debris in certain size (1&10 cm) were used in this study, which is frequently employed in the structure of spacecraft and aerospace designs. The selected atmospheric model for this investigation was the drag thermospheric models DTM78 and DTM94, because of this dependence on solar and geomagnetic activities. It was found that the lifetime of the space debris increases with increasing perigee altitudes. It was also found that the elliptical shape of the debris orbit would change gradually into a circular shape, then its kinetic energy would be transformed into heat and hence the debris might be destroyed in the dense atmosphere.
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Al-Zaidi, H. K., M. J. Al-Bermani, and A. M. Taleb. "Estimating the lifetime and Reentry of the Aluminum Space Debris of Sizes (1 and 10 cm) in LEO under Atmosphere Drag Effects." Journal of Kufa-Physics 12, no. 02 (2020): 66–75. http://dx.doi.org/10.31257/2018/jkp/2020/120207.
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This study attempts to address the lifetime and reentry of the space debris in low earth orbit LEO which extends from 200 to 1200 km. In this study a new Computer programs were designed to simulate the orbit dynamics of space debris lifetime and reentry under atmospheric drag force using Runge-Kutta Method to solve the differential equations of drag force. This model was adapted with the Drag Thermosphere Model (DTM78, 94), the Aluminum 2024 space debris in certain size (1&10 cm) were used in this study, which is frequently employed in the structure of spacecraft and aerospace designs. The selected atmospheric model for this investigation was the drag thermospheric models DTM78 and DTM94, because of this dependence on solar and geomagnetic activities. It was found that the lifetime of the space debris increases with increasing perigee altitudes. It was also found that the elliptical shape of the debris orbit would change gradually into a circular shape, then its kinetic energy would be transformed into heat and hence the debris might be destroyed in the dense atmosphere.
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Rigby, M., R. G. Prinn, S. O'Doherty, et al. "Re-evaluation of the lifetimes of the major CFCs and CH<sub>3</sub>CCl<sub>3</sub> using atmospheric trends." Atmospheric Chemistry and Physics Discussions 12, no. 9 (2012): 24469–99. http://dx.doi.org/10.5194/acpd-12-24469-2012.
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Abstract. Since the Montreal Protocol on substances that deplete the ozone layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH3CCl3, have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to relatively low levels, therefore the rate at which this recovery occurs will depend largely on the atmospheric lifetime of these compounds. The first ODS measurements began in the early 1970s along with the first lifetime estimates calculated by considering their atmospheric trends. We now have global mole fraction records spanning multiple decades, prompting this lifetime re-evaluation. Using surface measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration Global Monitoring Division (NOAA GMD) from 1978 to 2011, we estimated the lifetime of CFC-11, CFC-12, CFC-113 and CH3CCl3 using a multi-species inverse method. The CFC-11 lifetime of 45 yr, currently recommended in the World Meteorological Organisation (WMO) Scientific Assessment of Ozone Depletion, lies at the lower uncertainty bound of our estimates which are 524066 yr (1-sigma uncertainty) when AGAGE data were used, and 504066 yr when the NOAA network data were used. Our derived lifetime for CFC-113 is higher than the WMO estimates of 85 yr (10488123 using AGAGE, 10387122 using NOAA). Our estimates of the lifetime of CFC-12 and CH3CCl3 agree well with other recent estimates being 10885137 and 10484135 yr (CFC-12, AGAGE and NOAA, respectively) and 5.24.85.6 and 5.24.85.7 yr (CH3CCl3, AGAGE and NOAA, respectively).
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Stevenson, D. S., C. E. Johnson, E. J. Highwood, V. Gauci, W. J. Collins, and R. G. Derwent. "Atmospheric impact of the 1783–1784 Laki eruption: Part I Chemistry modelling." Atmospheric Chemistry and Physics 3, no. 3 (2003): 487–507. http://dx.doi.org/10.5194/acp-3-487-2003.
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Abstract. Results from the first chemistry-transport model study of the impact of the 1783–1784 Laki fissure eruption (Iceland: 64°N, 17°W) upon atmospheric composition are presented. The eruption released an estimated 61 Tg(S) as SO2 into the troposphere and lower stratosphere. The model has a high resolution tropopause region, and detailed sulphur chemistry. The simulated SO2 plume spreads over much of the Northern Hemisphere, polewards of ~40°N. About 70% of the SO2 gas is directly deposited to the surface before it can be oxidised to sulphuric acid aerosol. The main SO2 oxidants, OH and H2O2, are depleted by up to 40% zonally, and the lifetime of SO2 consequently increases. Zonally averaged tropospheric SO2 concentrations over the first three months of the eruption exceed 20 ppbv, and sulphuric acid aerosol reaches ~2 ppbv. These compare to modelled pre-industrial/present-day values of 0.1/0.5 ppbv SO2 and 0.1/1.0 ppbv sulphate. A total sulphuric acid aerosol yield of 17–22 Tg(S) is produced. The mean aerosol lifetime is 6–10 days, and the peak aerosol loading of the atmosphere is 1.4–1.7 Tg(S) (equivalent to 5.9–7.1 Tg of hydrated sulphuric acid aerosol). These compare to modelled pre-industrial/present-day sulphate burdens of 0.28/0.81 Tg(S), and lifetimes of 6/5 days, respectively. Due to the relatively short atmospheric residence times of both SO2 and sulphate, the aerosol loading approximately mirrors the temporal evolution of emissions associated with the eruption. The model produces a reason-able simulation of the acid deposition found in Greenland ice cores. These results appear to be relatively insensitive to the vertical profile of emissions assumed, although if more of the emissions reached higher levels (>12 km), this would give longer lifetimes and larger aerosol yields. Introducing the emissions in episodes generates similar results to using monthly mean emissions, because the atmospheric lifetimes are similar to the repose periods between episodes. Most previous estimates of the global aerosol loading associated with Laki did not use atmospheric models; this study suggests that these earlier estimates have been generally too large in magnitude, and too long-lived. Environmental effects following the Laki eruption may have been dominated by the widespread deposition of SO2 gas rather than sulphuric acid aerosol.
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Dalsøren, Stig B., Cathrine L. Myhre, Gunnar Myhre, et al. "Atmospheric methane evolution the last 40 years." Atmospheric Chemistry and Physics 16, no. 5 (2016): 3099–126. http://dx.doi.org/10.5194/acp-16-3099-2016.
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Abstract. Observations at surface sites show an increase in global mean surface methane (CH4) of about 180 parts per billion (ppb) (above 10 %) over the period 1984–2012. Over this period there are large fluctuations in the annual growth rate. In this work, we investigate the atmospheric CH4 evolution over the period 1970–2012 with the Oslo CTM3 global chemical transport model (CTM) in a bottom-up approach. We thoroughly assess data from surface measurement sites in international networks and select a subset suited for comparisons with the output from the CTM. We compare model results and observations to understand causes for both long-term trends and short-term variations. Employing Oslo CTM3 we are able to reproduce the seasonal and year-to-year variations and shifts between years with consecutive growth and stagnation, both at global and regional scales. The overall CH4 trend over the period is reproduced, but for some periods the model fails to reproduce the strength of the growth. The model overestimates the observed growth after 2006 in all regions. This seems to be explained by an overly strong increase in anthropogenic emissions in Asia, having global impact. Our findings confirm other studies questioning the timing or strength of the emission changes in Asia in the EDGAR v4.2 emission inventory over recent decades. The evolution of CH4 is not only controlled by changes in sources, but also by changes in the chemical loss in the atmosphere and soil uptake. The atmospheric CH4 lifetime is an indicator of the CH4 loss. In our simulations, the atmospheric CH4 lifetime decreases by more than 8 % from 1970 to 2012, a significant reduction of the residence time of this important greenhouse gas. Changes in CO and NOx emissions, specific humidity, and ozone column drive most of this, and we provide simple prognostic equations for the relations between those and the CH4 lifetime. The reduced lifetime results in substantial growth in the chemical CH4 loss (relative to its burden) and dampens the CH4 growth.
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Liu, Y., L. Huang, S. M. Li, T. Harner, and J. Liggio. "OH-initiated heterogeneous oxidation of tris-2-butoxyethyl phosphate: implications for its fate in the atmosphere." Atmospheric Chemistry and Physics 14, no. 22 (2014): 12195–207. http://dx.doi.org/10.5194/acp-14-12195-2014.
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Abstract. A particle-phase relative rates technique is used to investigate the heterogeneous reaction between OH radicals and tris-2-butoxyethyl phosphate (TBEP) at 298 K by combining aerosol time-of-flight mass spectrometry (C-ToF-MS) data and positive matrix factor (PMF) analysis. The derived second-order rate constants (k2) for the heterogeneous loss of TBEP is (4.44 ± 0.45) × 10−12 cm3 molecule−1 s−1, from which an approximate particle-phase lifetime was estimated to be 2.6 (2.3–2.9) days. However, large differences in the rate constants for TBEP relative to a reference compound were observed when comparing internally and externally mixed TBEP/organic particles, and upon changes in the RH. The heterogeneous degradation of TBEP was found to be depressed or enhanced depending upon the particle mixing state and phase, highlighting the complexity of heterogeneous oxidation in the atmosphere. The effect of gas-particle partitioning on the estimated overall lifetime (gas + particle) for several organophosphate esters (OPEs) was also examined through the explicit modeling of this process. The overall atmospheric lifetimes of TBEP, tris-2-ethylhexyl phosphate (TEHP) and tris-1,3-dichloro-2-propyl phosphate (TDCPP) were estimated to be 1.9, 1.9 and 2.4 days respectively, and are highly dependent upon particle size. These results demonstrate that modeling the atmospheric fate of particle-phase toxic compounds for the purpose of risk assessment must include the gas-particle partitioning process, and in the future include the effect of other particulate components on the evaporation kinetics and/or the heterogeneous loss rates.
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Prather, Michael J., Lucien Froidevaux, and Nathaniel J. Livesey. "Observed changes in stratospheric circulation: decreasing lifetime of N2O, 2005–2021." Atmospheric Chemistry and Physics 23, no. 2 (2023): 843–49. http://dx.doi.org/10.5194/acp-23-843-2023.
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Abstract. Using Aura Microwave Limb Sounder satellite observations of stratospheric nitrous oxide (N2O), ozone, and temperature from 2005 through 2021, we calculate the atmospheric lifetime of N2O to be decreasing at a rate of −2.1 ± 1.2 %/decade. This decrease is occurring because the N2O abundances in the middle tropical stratosphere, where N2O is photochemically destroyed, are increasing at a faster rate than the bulk N2O in the lower atmosphere. The cause appears to be a more vigorous stratospheric circulation, which models predict to be a result of climate change. If the observed trends in lifetime and implied emissions continue, then the change in N2O over the 21st century will be 27 % less than those projected with a fixed lifetime, and the impact on global warming and ozone depletion will be proportionately lessened. Because global warming is caused in part by N2O, this finding is an example of a negative climate–chemistry feedback.
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Kristiansen, N. I., A. Stohl, D. J. L. Olivié, et al. "Evaluation of observed and modelled aerosol lifetimes using radioactive tracers of opportunity and an ensemble of 19 global models." Atmospheric Chemistry and Physics Discussions 15, no. 17 (2015): 24513–85. http://dx.doi.org/10.5194/acpd-15-24513-2015.
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Abstract. Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulphate aerosols were the main carriers for the cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulphate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulphate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulphate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 37Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between two and nine weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast removal in most models. Because sufficient measurement data were only available from about two weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first two weeks was quicker (lifetimes between 1–5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the Arctic aerosol underestimates.
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Yanchukovsky, Valery. "MUON INTENSITY VARIATIONS AND ATMOSPHERIC TEMPERATURE." Solar-Terrestrial Physics 6, no. 1 (2020): 108–15. http://dx.doi.org/10.12737/stp-61202013.
Texto completo da fonteResumo:
Muons in the atmosphere are formed during the decay of pions resulting from nuclear interactions of cosmic rays with nuclei of air atoms. The resulting muons are also unstable particles with a short lifetime. Therefore, not all of them reach the level of observation in the atmosphere. When the atmospheric temperature changes, the distance to the observation level changes too, thus leading to variations in the intensity of muons of temperature origin. These variations, caused by atmospheric temperature variations, are superimposed on continuous observations of muon telescopes. Their exclusion is, therefore, extremely necessary, especially in the data from modern muon telescopes whose statistical accuracy is very high. The contribution of various atmospheric layers to the total temperature effect is not the same for muons. This contribution is characterized by the distribution of the density of temperature coefficients for muons in the atmosphere. Using this distribution and the continuous intensity observations from the muon telescope in Novosibirsk, the inverse problem has been solved, from the solution of which the atmospheric temperature variations over a long period from 2004 to 2011 have been found. The results obtained are compared with aerological sounding data.
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Yanchukovsky, Valery. "MUON INTENSITY VARIATIONS AND ATMOSPHERIC TEMPERATURE." Solnechno-Zemnaya Fizika 6, no. 1 (2020): 134–41. http://dx.doi.org/10.12737/szf-61202013.
Texto completo da fonteResumo:
Muons in the atmosphere are formed during the decay of pions resulting from nuclear interactions of cosmic rays with nuclei of air atoms. The resulting muons are also unstable particles with a short lifetime. Therefore, not all of them reach the level of observation in the atmosphere. When the atmospheric temperature changes, the distance to the observation level changes too, thus leading to variations in the intensity of muons of temperature origin. These variations, caused by atmospheric temperature variations, are superimposed on continuous observations of muon telescopes. Their exclusion is, therefore, extremely necessary, especially in the data from modern muon telescopes whose statistical accuracy is very high. The contribution of various atmospheric layers to the total temperature effect is not the same for muons. This contribution is characterized by the distribution of the density of temperature coefficients for muons in the atmosphere. Using this distribution and the continuous intensity observations from the muon telescope in Novosibirsk, the inverse problem has been solved, from the solution of which the atmospheric temperature variations over a long period from 2004 to 2011 have been found. The results obtained are compared with aerological sounding data.
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Youn, D., K. O. Patten, D. J. Wuebbles, H. Lee, and C. W. So. "Potential impact of iodinated replacement compounds CF<sub>3</sub>I and CH<sub>3</sub>I on atmospheric ozone: a three-dimensional modeling study." Atmospheric Chemistry and Physics 10, no. 20 (2010): 10129–44. http://dx.doi.org/10.5194/acp-10-10129-2010.
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Abstract. The concept of Ozone Depletion Potentials (ODPs) is extensively used in policy considerations related to concerns about the effects of various halocarbons and other gases on stratospheric ozone. Many of the recent candidate replacement compounds have atmospheric lifetimes shorter than one year in order to limit their environmental effects, especially on stratospheric ozone. Using a three-dimensional global chemistry-transport model (CTM) of the troposphere and the stratosphere, the purpose of this study is to evaluate the potential effects of several very short-lived iodinated substances, namely iodotrifluoromethane (CF3I) and methyl iodide (CH3I), on atmospheric ozone. Like other chemicals with extremely short lifetimes, the stratospheric halogen loading and resulting ozone effects from these compounds are strongly dependent on the location of emissions. For CF3I, a possible replacement candidate for bromotrifluoromethane (CF3Br), ODPs derived by the three-dimensional model are 0.008 with chemical lifetime of 5.03 days and 0.016 with a lifetime of 1.13 days for emissions assumed to be evenly distributed over land surfaces at mid-latitudes and the tropics, respectively. While this is the first time the ODPs have been evaluated with a three-dimensional model, these values are in good agreement with those derived previously. The model calculations suggest that tropical convection could deliver a larger portion of the gas and their breakdown products to the upper troposphere and lower stratosphere if emission source is located in the tropics. The resulting ODP for CH3I, emitted from mid-latitudes, is 0.017 with lifetime of 13.59 days. Valid simulations of convective transport, vertical mixing and degradation chemistry of CH3I are shown that have good qualitative agreement between the model derived distribution of background CH3I, based on global source emission fluxes from previous studies, and available observations especially in vertical profiles.
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Bluvshtein, Nir, Ulrich K. Krieger, and Thomas Peter. "Photophoretic spectroscopy in atmospheric chemistry – high-sensitivity measurements of light absorption by a single particle." Atmospheric Measurement Techniques 13, no. 6 (2020): 3191–203. http://dx.doi.org/10.5194/amt-13-3191-2020.
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Abstract. Light-absorbing organic atmospheric particles, termed brown carbon, undergo chemical and photochemical aging processes during their lifetime in the atmosphere. The role these particles play in the global radiative balance and in the climate system is still uncertain. To better quantify their radiative forcing due to aerosol–radiation interactions, we need to improve process-level understanding of aging processes, which lead to either “browning” or “bleaching” of organic aerosols. Currently available laboratory techniques aim to simulate atmospheric aerosol aging and measure the evolving light absorption, but they suffer from low sensitivity and precision. This study describes the use of electrodynamic balance photophoretic spectroscopy (EDB-PPS) for high-sensitivity and high-precision measurements of light absorption by a single particle. We demonstrate the retrieval of the time-evolving imaginary part of the refractive index for a single levitated particle in the range of 10−4 to 10−5 with uncertainties of less than 25 % and 60 %, respectively. The experimental system is housed within an environmental chamber, in which aging processes can be simulated in realistic atmospheric conditions and lifetimes of days to weeks. This high level of sensitivity enables future studies to explore the major processes responsible for formation and degradation of brown carbon aerosols.