1,069 research outputs found
Atmospheric histories, growth rates and solubilities in seawater and other natural waters of the potential transient tracers HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 and PFC-116
We present consistent annual mean atmospheric histories and growth rates for the mainly anthropogenic halogenated compounds HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 and PFC-116, which are all potentially useful oceanic transient tracers (tracers of water transport within the ocean), for the Northern and Southern Hemisphere with the aim of providing input histories of these compounds for the equilibrium between the atmosphere and surface ocean. We use observations of these halogenated compounds made by the Advanced Global Atmospheric Gases Experiment (AGAGE), the Scripps Institution of Oceanography (SIO), the Commonwealth Scientific and Industrial Research Organization (CSIRO), the National Oceanic and Atmospheric Administration (NOAA) and the University of East Anglia (UEA). Prior to the direct observational record, we use archived air measurements, firn air measurements and published model calculations to estimate the atmospheric mole fraction histories. The results show that the atmospheric mole fractions for each species, except HCFC-141b and HCFC-142b, have been increasing since they were initially produced. Recently, the atmospheric growth rates have been decreasing for the HCFCs (HCFC-22, HCFC-141b and HCFC-142b), increasing for the HFCs (HFC-134a, HFC-125, HFC-23) and stable with little fluctuation for the PFCs (PFC-14 and PFC-116) investigated here. The atmospheric histories (source functions) and natural background mole fractions show that HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125 and HFC-23 have the potential to be oceanic transient tracers for the next few decades only because of the recently imposed bans on production and consumption. When the atmospheric histories of the compounds are not monotonically changing, the equilibrium atmospheric mole fraction (and ultimately the age associated with that mole fraction) calculated from their concentration in the ocean is not unique, reducing their potential as transient tracers. Moreover, HFCs have potential to be oceanic transient tracers for a longer period in the future than HCFCs as the growth rates of HFCs are increasing and those of HCFCs are decreasing in the background atmosphere. PFC-14 and PFC-116, however, have the potential to be tracers for longer periods into the future due to their extremely long lifetimes, steady atmospheric growth rates and no explicit ban on their emissions. In this work, we also derive solubility functions for HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 and PFC-116 in water and seawater to facilitate their use as oceanic transient tracers. These functions are based on the Clark-Glew-Weiss (CGW) water solubility function fit and salting-out coefficients estimated by the poly-parameter linear free-energy relationships (pp-LFERs). Here we also provide three methods of seawater solubility estimation for more compounds. Even though our intention is for application in oceanic research, the work described in this paper is potentially useful for tracer studies in a wide range of natural waters, including freshwater and saline lakes, and, for the more stable compounds, groundwaters
Evaluation of stratospheric age of air from CF, CF, CF, CHF, HFC-125, HFC-227ea and SF; Implications for the calculations of halocarbon lifetimes, fractional release factors and ozone depletion potentials
In a changing climate, potential stratospheric circulation changes require long-term monitoring. Stratospheric trace gas measurements are often used as a proxy for stratospheric circulation changes via the “mean age of air” values derived from them. In this study, we investigated five potential age of air tracers – the perfluorocarbons CF4, C2F6 and C3F8 and the hydrofluorocarbons CHF3 (HFC-23) and HFC-125 – and compare them to the traditional tracer SF6 and a (relatively) shorter-lived species, HFC-227ea. A detailed uncertainty analysis was performed on mean ages derived from these “new” tracers to allow us to confidently compare their efficacy as age tracers to the existing tracer, SF6. Our results showed that uncertainties associated with the mean age derived from these new age tracers are similar to those derived from SF6, suggesting that these alternative compounds are suitable in this respect for use as age tracers. Independent verification of the suitability of these age tracers is provided by a comparison between samples analysed at the University of East Anglia and the Scripps Institution of Oceanography. All five tracers give younger mean ages than SF6, a discrepancy that increases with increasing mean age. Our findings qualitatively support recent work that suggests that the stratospheric lifetime of SF6 is significantly less than the previous estimate of 3200 years. The impact of these younger mean ages on three policy-relevant parameters – stratospheric lifetimes, fractional release factors (FRFs) and ozone depletion potentials – is investigated in combination with a recently improved methodology to calculate FRFs. Updates to previous estimations for these parameters are provided
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Evaluation of stratospheric age of air from CF4, C2F6, C3F8, CHF3, HFC-125, HFC-227ea and SF6; implications for the calculations of halocarbon lifetimes, fractional release factors and ozone depletion potentials
In a changing climate,
potential stratospheric circulation changes require long-term monitoring.
Stratospheric trace gas measurements are often used as a proxy for
stratospheric circulation changes via the <q>mean age of air</q> values derived
from them. In this study, we investigated five potential age of air tracers
– the perfluorocarbons CF<sub>4</sub>, C<sub>2</sub>F<sub>6</sub> and C<sub>3</sub>F<sub>8</sub> and the
hydrofluorocarbons CHF<sub>3</sub> (HFC-23) and HFC-125 – and compare them to the
traditional tracer SF<sub>6</sub> and a (relatively) shorter-lived species,
HFC-227ea. A detailed uncertainty analysis was performed on mean ages derived
from these <q>new</q> tracers to allow us to confidently compare their efficacy
as age tracers to the existing tracer, SF<sub>6</sub>. Our results showed that
uncertainties associated with the mean age derived from these new age tracers
are similar to those derived from SF<sub>6</sub>, suggesting that these alternative
compounds are suitable in this respect for use as age tracers. Independent
verification of the suitability of these age tracers is provided by a
comparison between samples analysed at the University of East Anglia and the
Scripps Institution of Oceanography. All five tracers give younger mean ages
than SF<sub>6</sub>, a discrepancy that increases with increasing mean age. Our
findings qualitatively support recent work that suggests that the
stratospheric lifetime of SF<sub>6</sub> is significantly less than the previous
estimate of 3200Â years. The impact of these younger mean ages on three
policy-relevant parameters – stratospheric lifetimes, fractional release
factors (FRFs) and ozone depletion potentials – is investigated in
combination with a recently improved methodology to calculate FRFs. Updates
to previous estimations for these parameters are provided
Transcriptional slippage occurs during elongation at runs of adenine or thymine in Escherichia coli
A run of 11 adenine or thymine residues at the 5' end of an out-of-fram
Rising Perfluorocyclobutane (PFC-318, c-C4F8) Emissions in China from 2011 to 2020 Inferred from Atmospheric Observations
Global atmospheric emissions of perfluorocyclobutane (c-C4F8, PFC-318), a potent greenhouse gas, have increased rapidly in recent years. Combining atmospheric observations made at nine Chinese sites with a Lagrangian dispersion model-based Bayesian inversion technique, we show that PFC-318 emissions in China grew by approximately 70% from 2011 to 2020, rising from 0.65 (0.54–0.72) Gg year–1 in 2011 to 1.12 (1.05–1.19) Gg year–1 in 2020. The PFC-318 emission increase from China played a substantial role in the overall increase in global emissions during the study period, contributing 58% to the global total emission increase. This growth predominantly originated in eastern China. The regions with high emissions of PFC-318 in China overlap with areas densely populated with polytetrafluoroethylene (PTFE) factories, implying that fluoropolymer factories are important sources of PFC-318 emissions in China. Our investigation reveals an emission factor of approximately 3.02 g of byproduct PFC-318 emissions per kg of hydrochlorofluorocarbon-22 (HCFC-22) feedstock use in the production of tetrafluoroethylene (TFE) (for PTFE production) and hexafluoropropylene (HFP) if we assume all HCFC-22 produced for feedstock uses in China are pyrolyzed to produce PTFE and HFP. Further facility-level sampling and analysis are needed for a more precise evaluation of emissions from these factories
Changing trends and emissions of hydrochlorofluorocarbons (HCFCs) and their hydrofluorocarbon (HFCs) replacements
United States. National Aeronautics and Space Administration (NAG5-12669)United States. National Aeronautics and Space Administration (NNX07AE89G)United States. National Aeronautics and Space Administration (NNX11AF17G)United States. National Aeronautics and Space Administration (NNX16AC98G
Stochastic Inflation:The Quantum Phase Space Approach
In this paper a quantum mechanical phase space picture is constructed for
coarse-grained free quantum fields in an inflationary Universe. The appropriate
stochastic quantum Liouville equation is derived. Explicit solutions for the
phase space quantum distribution function are found for the cases of power law
and exponential expansions. The expectation values of dynamical variables with
respect to these solutions are compared to the corresponding cutoff regularized
field theoretic results (we do not restrict ourselves only to \VEV{\F^2}).
Fair agreement is found provided the coarse-graining scale is kept within
certain limits. By focusing on the full phase space distribution function
rather than a reduced distribution it is shown that the thermodynamic
interpretation of the stochastic formalism faces several difficulties (e.g.,
there is no fluctuation-dissipation theorem). The coarse-graining does not
guarantee an automatic classical limit as quantum correlations turn out to be
crucial in order to get results consistent with standard quantum field theory.
Therefore, the method does {\em not} by itself constitute an explanation of the
quantum to classical transition in the early Universe. In particular, we argue
that the stochastic equations do not lead to decoherence.Comment: 43 page
Global emissions of refrigerants HCFC-22 and HFC-134a: Unforeseen seasonal contributions
HCFC-22 (CHClF[subscript 2]) and HFC-134a (CH[subscript 2]FCF[subscript 3]) are two major gases currently used worldwide in domestic and commercial refrigeration and air conditioning. HCFC-22 contributes to stratospheric ozone depletion, and both species are potent greenhouse gases. In this work, we study in situ observations of HCFC-22 and HFC-134a taken from research aircraft over the Pacific Ocean in a 3-y span [HIaper-Pole-to-Pole Observations (HIPPO) 2009–2011] and combine these data with long-term ground observations from global surface sites [National Oceanic and Atmospheric Administration (NOAA) and Advanced Global Atmospheric Gases Experiment (AGAGE) networks]. We find the global annual emissions of HCFC-22 and HFC-134a have increased substantially over the past two decades. Emissions of HFC-134a are consistently higher compared with the United Nations Framework Convention on Climate Change (UNFCCC) inventory since 2000, by 60% more in recent years (2009–2012). Apart from these decadal emission constraints, we also quantify recent seasonal emission patterns showing that summertime emissions of HCFC-22 and HFC-134a are two to three times higher than wintertime emissions. This unforeseen large seasonal variation indicates that unaccounted mechanisms controlling refrigerant gas emissions are missing in the existing inventory estimates. Possible mechanisms enhancing refrigerant losses in summer are (i) higher vapor pressure in the sealed compartment of the system at summer high temperatures and (ii) more frequent use and service of refrigerators and air conditioners in summer months. Our results suggest that engineering (e.g., better temperature/vibration-resistant system sealing and new system design of more compact/efficient components) and regulatory (e.g., reinforcing system service regulations) steps to improve containment of these gases from working devices could effectively reduce their release to the atmosphere
Generalized quantum Fokker-Planck, diffusion and Smoluchowski equations with true probability distribution functions
Traditionally, the quantum Brownian motion is described by Fokker-Planck or
diffusion equations in terms of quasi-probability distribution functions, e.g.,
Wigner functions. These often become singular or negative in the full quantum
regime. In this paper a simple approach to non-Markovian theory of quantum
Brownian motion using {\it true probability distribution functions} is
presented. Based on an initial coherent state representation of the bath
oscillators and an equilibrium canonical distribution of the quantum mechanical
mean values of their co-ordinates and momenta we derive a generalized quantum
Langevin equation in -numbers and show that the latter is amenable to a
theoretical analysis in terms of the classical theory of non-Markovian
dynamics. The corresponding Fokker-Planck, diffusion and the Smoluchowski
equations are the {\it exact} quantum analogues of their classical
counterparts. The present work is {\it independent} of path integral
techniques. The theory as developed here is a natural extension of its
classical version and is valid for arbitrary temperature and friction
(Smoluchowski equation being considered in the overdamped limit).Comment: RevTex, 16 pages, 7 figures, To appear in Physical Review E (minor
revision
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