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Non-volatile memory (NVM), also known as persistent memory, is an emerging paradigm for memory that preserves its contents even after power loss. NVM is widely expected to become ubiquitous, and hardware architectures are already providing support for NVM programming. This has stimulated interest in the design of novel concepts ensuring correctness of concurrent programming abstractions in the face of persistency and in the development of associated verification approaches. Software transactional memory (STM) is a key programming abstraction that supports concurrent access to shared state. In a fashion similar to linearizability as the correctness condition for concurrent data structures, there is an established notion of correctness for STMs known as opacity. We have recently proposed durable opacity as the natural extension of opacity to a setting with non-volatile memory. Together with this novel correctness condition, we designed a verification technique based on refinement. In this paper, we extend this work in two directions. First, we develop a durably opaque version of NOrec (no ownership records), an existing STM algorithm proven to be opaque. Second, we modularise our existing verification approach by separating the proof of durability of memory accesses from the proof of opacity. For NOrec, this allows us to re-use an existing opacity proof and complement it with a proof of the durability of accesses to shared state.

Hyperproperties are correctness conditions for labelled transition systems that are more expressive than traditional trace properties, with particular relevance to security. Recently, Attiya and Enea studied a notion of strong observational refinement that preserves all hyperproperties. They analyse the correspondence between forward simulation and strong observational refinement in a setting with finite traces only. We study this correspondence in a setting with both finite and infinite traces. In particular, we show that forward simulation does not preserve hyperliveness properties in this setting. We extend the forward simulation proof obligation with a progress condition, and prove that this progressive forward simulation does imply strong observational refinement., LIPIcs, Vol. 209, 35th International Symposium on Distributed Computing (DISC 2021), pages 55:1-55:4

Hyperproperties are correctness conditions for labelled transition systems that are more expressive than traditional trace properties, with particular relevance to security. Recently, Attiya and Enea studied a notion of strong observational refinement that preserves all hyperproperties. They analyse the correspondence between forward simulation and strong observational refinement in a setting with finite traces only. We study this correspondence in a setting with both finite and infinite traces. In particular, we show that forward simulation does not preserve hyperliveness properties in this setting. We extend the forward simulation proof obligation with a progress condition, and prove that this progressive forward simulation does imply strong observational refinement., Comment: Full version of the paper to appear in DISC 2021

Weak memory presents a new challenge for program verification and has resulted in the development of a variety of specialised logics. For C11-style memory models, our previous work has shown that it is possible to extend Hoare logic and Owicki-Gries reasoning to verify correctness of weak memory programs. The technique introduces a set of high-level assertions over C11 states together with a set of basic Hoare-style axioms over atomic weak memory statements (e.g., reads/writes), but retains all other standard proof obligations for compound statements. This paper takes this line of work further by showing Nipkow and Nieto's encoding of Owicki-Gries in the Isabelle theorem prover can be extended to handle C11-style weak memory models in a straightforward manner. We exemplify our techniques over several litmus tests from the literature and a non-trivial example: Peterson's algorithm adapted for C11. For the examples we consider, the proof outlines can be automatically discharged using the existing Isabelle tactics developed by Nipkow and Nieto. The benefit here is that programs can be written using a familiar pseudocode syntax with assertions embedded directly into the program.

This note relates axioms for partial semigroups and monoids with those for small object-free categories, either with multiple monoidal units or with source and target maps. We discuss the adjunction of a zero element to both kinds of category and provide examples that separate the algebras considered.

Owicki-Gries reasoning for concurrent programs uses Hoare logic together with an interference freedom rule for concurrency. In this paper, we develop a new proof calculus for the C11 RAR memory model (a fragment of C11 with both relaxed and release-acquire accesses) that allows all Owicki-Gries proof rules for compound statements, including non-interference, to remain unchanged. Our proof method features novel assertions specifying thread-specific views on the state of programs. This is combined with a set of Hoare logic rules that describe how these assertions are affected by atomic program steps. We demonstrate the utility of our proof calculus by verifying a number of standard C11 litmus tests and Peterson’s algorithm adapted for C11. Our proof calculus and its application to program verification have been fully mechanised in the theorem prover Isabelle., LIPIcs, Vol. 166, 34th European Conference on Object-Oriented Programming (ECOOP 2020), pages 11:1-11:26

The paper "Owicki-Gries Reasoning for C11 RAR" introduces a new proof calculus for the C11 RAR memory model that allows Owicki-Gries proof rules for compound statements, including non-interference, to remain unchanged. The proof method features novel assertions specifying thread-specific views on the state of programs. This is combined with a set of Hoare logic rules that describe how these assertions are affected by atomic program steps. The artifact includes the Isabelle formalisation of the proof method introduced in the paper. It also contains the formalisation and proof of all case studies presented in the paper. All of the theorems are accompanied with their respective proofs., DARTS, Vol. 6, Special Issue of the 34th European Conference on Object-Oriented Programming (ECOOP 2020), pages 15:1-15:2

Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). HCFC consumption and production are currently regulated under the Montreal Protocol on Substances that Deplete the Ozone Layer and their emissions have started to stabilize or even decrease. As HCFC-22 (CHClF2) is by far the most abundant HCFC in today's atmosphere, it is crucial to continue to monitor the evolution of its atmospheric concentration. In this study, we describe an improved HCFC-22 retrieval strategy from ground-based high-resolution Fourier transform infrared (FTIR) solar spectra recorded at the high-altitude scientific station of Jungfraujoch, the Swiss Alps, 3580 m a.m.s.l. (above mean sea level). This new strategy distinguishes tropospheric and lower-stratospheric partial columns. Comparisons with independent datasets, such as the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), supported by models, such as the Belgian Assimilation System for Chemical ObErvation (BASCOE) and the Whole Atmosphere Community Climate Model (WACCM), demonstrate the validity of our tropospheric and lower-stratospheric long-term time series. A trend analysis on the datasets used here, now spanning 30 years, confirms the last decade's decline in the HCFC-22 growth rate. This updated retrieval strategy can be adapted for other ozone-depleting substances (ODSs), such as CFC-12. Measuring or retrieving ODS atmospheric concentrations is essential for scrutinizing the fulfilment of the globally ratified Montreal Protocol.

Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). HCFC consumption and production are currently regulated under the Montreal Protocol on Substances that Deplete the Ozone Layer and their emissions have started to stabilize or even decrease. As HCFC-22 (CHClF2) is by far the most abundant HCFC in today's atmosphere, it is crucial to continue to monitor the evolution of its atmospheric concentration. In this study, we describe an improved HCFC-22 retrieval strategy from ground-based high-resolution Fourier transform infrared (FTIR) solar spectra recorded at the high-altitude scientific station of Jungfraujoch, the Swiss Alps, 3580 m a.m.s.l. (above mean sea level). This new strategy distinguishes tropospheric and lower-stratospheric partial columns. Comparisons with independent datasets, such as the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), supported by models, such as the Belgian Assimilation System for Chemical ObErvation (BASCOE) and the Whole Atmosphere Community Climate Model (WACCM), demonstrate the validity of our tropospheric and lower-stratospheric long-term time series. A trend analysis on the datasets used here, now spanning 30 years, confirms the last decade's decline in the HCFC-22 growth rate. This updated retrieval strategy can be adapted for other ozone-depleting substances (ODSs), such as CFC-12. Measuring or retrieving ODS atmospheric concentrations is essential for scrutinizing the fulfilment of the globally ratified Montreal Protocol.

We present a compact and versatile cryofocusing–thermodesorption unit, which we developed for quantitative analysis of halogenated trace gases in ambient air. Possible applications include aircraft-based in situ measurements, in situ monitoring and laboratory operation for the analysis of flask samples. Analytes are trapped on adsorptive material cooled by a Stirling cooler to low temperatures (e.g. −80 °C) and subsequently desorbed by rapid heating of the adsorptive material (e.g. +200 °C). The set-up involves neither the exchange of adsorption tubes nor any further condensation or refocusing steps. No moving parts are used that would require vacuum insulation. This allows for a simple and robust design. Reliable operation is ensured by the Stirling cooler, which neither contains a liquid refrigerant nor requires refilling a cryogen. At the same time, it allows for significantly lower adsorption temperatures compared to commonly used Peltier elements. We use gas chromatography – mass spectrometry (GC–MS) for separation and detection of the preconcentrated analytes after splitless injection. A substance boiling point range of approximately −80 to +150 °C and a substance mixing ratio range of less than 1 ppt (pmol mol−1) to more than 500 ppt in preconcentrated sample volumes of 0.1 to 10 L of ambient air is covered, depending on the application and its analytical demands. We present the instrumental design of the preconcentration unit and demonstrate capabilities and performance through the examination of analyte breakthrough during adsorption, repeatability of desorption and analyte residues in blank tests. Examples of application are taken from the analysis of flask samples collected at Mace Head Atmospheric Research Station in Ireland using our laboratory GC–MS instruments and by data obtained during a research flight with our in situ aircraft instrument GhOST-MS (Gas chromatograph for the Observation of Tracers – coupled with a Mass Spectrometer).

Palladium nanoparticles stabilized by heteroatom donor‐modified polystyrene‐based polymer immobilized ionic liquids (PdNP@HAD‐PIILP; HAD‐PPh2, OMe, NH2, CN, pyrrolidone) are highly efficient catalysts for the Suzuki‐Miyaura cross‐coupling in aqueous media under mild conditions. Catalyst modified with phosphine was consistently the most efficient as it gave high yields across a range of substrates under mild conditions at low catalyst loadings. Incorporation of polyethylene glycol into the phosphine modified immobilised ionic liquid support improved catalyst efficacy by improving dispersibility and facilitating access to the active site. Moreover, each of the heteroatom modified catalysts was more active than the corresponding unsubstituted imidazolium‐based polystyrene benchmark as well as commercial samples of Pd/C. Catalyst generated in situ from either [PdCl4]@PPh2‐PIILP or its PEGylated counterpart [PdCl4]@PPh2‐PEGPIILP, by reduction with phenylboronic acid, outperformed their pre‐formed counterparts for the vast majority of substrates examined. The turnover frequency of 16,300 h−1 obtained at room temperature is one of the highest to be reported for palladium nanoparticle‐catalysed Suzuki‐Miyaura cross‐coupling between 4‐bromoacetophenone and phenylboronic acid in aqueous media under such mild conditions.

In the interleaving model of concurrency, where events are totally ordered, linearizability is compositional: the composition of two linearizable objects is guaranteed to be linearizable. However, linearizability is not compositional when events are only partially ordered, as in many weak-memory models that describe multicore memory systems. In this paper, we present causal linearizability, a correctness condition for concurrent objects implemented in weak-memory models. We abstract from the details of specific memory models by defining our condition using Lamport's execution structures. We apply our condition to the C11 memory model, providing a correctness condition for C11 objects. We develop a proof method for verifying objects implemented in C11 and related models. Our method is an adaptation of simulation-based methods, but in contrast to other such methods, it does not require that the implementation totally order its events. We also show that causal linearizability reduces to linearizability in the totally ordered case.

Correctness conditions like linearizability and opacity describe some form of atomicity imposed on concurrent objects. In this paper, we propose a correctness condition (called causal atomicity) for concurrent objects executing in a weak memory model, where the histories of the objects in question are partially ordered. We establish compositionality and abstraction results for causal atomicity and develop an associated refinement-based proof technique.

Phosphino-decorated polymer immobilised ionic liquid phase stabilised palladium nanoparticles (PdNP@PPh2-PIILP) and their PEGylated counterparts (PdNP@PPh2-PEGPIILP) are remarkably active and exceptionally selective catalysts for the aqueous phase hydrogenation of α,β-unsaturated aldehydes, ketones, esters and nitriles with PdNP@PPh2-PEGPIILP giving complete conversion and 100% selectivity for reduction of the C[double bond, length as m-dash]C bond, under mild conditions. This is the most selective PdNP-based system to be reported for the aqueous phase hydrogenation of this class of substrates.

Changes of atmospheric methane total columns (CH4) since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns of 0.31 ± 0.03 % year−1 (2σ level of uncertainty) for the 2005–2014 period. Comparisons with in situ methane measurements at both local and global scales show good agreement. We used the GEOS-Chem chemical transport model tagged simulation, which accounts for the contribution of each emission source and one sink in the total methane, simulated over 2005–2012. After regridding according to NDACC vertical layering using a conservative regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane total columns of 0.35 ± 0.03 % year−1 between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30 ± 0.04 % year−1, averaged over 10 stations). Analysis of the GEOS-Chem-tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the interannual variability of methane. However, anthropogenic emissions, such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem-tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained.

Most work on the verification of concurrent objects for shared memory assumes sequential consistency, but most multicore processors support only weak memory models that do not provide sequential consistency. Furthermore, most verification efforts focus on the linearizability of concurrent objects, but there are existing implementations optimized to run on weak memory models that are not linearizable. In this paper, we address these problems by introducing causal linearizability, a correctness condition for concurrent objects running on weak memory models. Like linearizability itself, causal linearizability enables concurrent objects to be composed, under weak constraints on the client's behaviour. We specify these constraints by introducing a notion of operation-race freedom, where programs that satisfy this property are guaranteed to behave as if their shared objects were in fact linearizable. We apply these ideas to objects from the Linux kernel, optimized to run on TSO, the memory model of the x86 processor family., Full version of submission to SEFM 2016

Transactional memory is a mechanism that manages thread synchronisation on behalf of a programmer so that blocks of code execute with an illusion of atomicity. The main safety criterion for transactional memory is opacity, which defines conditions for serialising concurrent transactions. Proving opacity is complicated because it allows concurrent transactions to observe distinct memory states, while TM implementations are typically based on one single shared store. This paper presents a sound and complete method, based on coarse-grained abstraction, for reducing proofs of opacity to the relatively simpler correctness condition: linearizability. We use our methods to verify TML and NORec from the literature and show our techniques extend to relaxed memory models by showing that both are opaque under TSO without requiring additional fences. Our methods also elucidate TM designs at higher level of abstraction; as an application, we develop a variation of NORec with fast-path reads transactions. All our proofs have been mechanised, either in the Isabelle theorem prover or the PAT model checker.

International audience; Vaccination procedures within the cattle industry are important disease control tools to minimize economic and welfare burdens associated with respiratory pathogens. However, new vaccine, antigen and carrier technologies are required to combat emerging viral strains and enhance the efficacy of respiratory vaccines, particularly at the point of pathogen entry. New technologies, specifically metabolomic profiling, could be applied to identify metabolite immune-correlates representative of immune protection following vaccination aiding in the design and screening of vaccine candidates. This study for the first time demonstrates the ability of untargeted UPLC-MS metabolomic profiling to identify metabolite immune correlates characteristic of immune responses following mucosal vaccination in calves. Male Holstein Friesian calves were vaccinated with Pfizer Rispoval® PI3 + RSV intranasal vaccine and metabolomic profiling of post-vaccination plasma revealed 12 metabolites whose peak intensities differed significantly from controls. Plasma levels of glycocholic acid, N-[(3α,5β,12α)-3,12-Dihydroxy-7,24-dioxocholan-24-yl]glycine, uric acid and biliverdin were found to be significantly elevated in vaccinated animals following secondary vaccine administration, whereas hippuric acid significantly decreased. In contrast, significant upregulation of taurodeoxycholic acid and propionylcarnitine levels were confined to primary vaccine administration. Assessment of such metabolite markers may provide greater information on the immune pathways stimulated from vaccine formulations and benchmarking early metabolomic responses to highly immunogenic vaccine formulations could provide a means for rapidly assessing new vaccine formulations. Furthermore, the identification of metabolic systemic immune response markers which relate to specific cell signaling pathways of the immune system could allow for targeted vaccine design to stimulate key pathways which can be assessed at the metabolic level.

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH₄) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH₄ emissions. The GCP dataset integrates results from topdown studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH₄ yr⁻¹ higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all topdown studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric ¹³CH₄. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH₄ growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH₄ emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric ¹³CH₄ observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (similar to biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558 TgCH(4) yr(-1), range 540-568. About 60% of global emissions are anthropogenic (range 50-65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 TgCH(4) yr(-1), range 596-884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (similar to 64% of the global budget, amp;lt;30 degrees N) as compared to mid (similar to 32 %, 30-60 degrees N) and high northern latitudes (similar to 4 %, 60-90 degrees N). Top-down inversions consistently infer lower emissions in China (similar to 58 TgCH(4) yr(-1), range 51-72, -14 %) and higher emissions in Africa (86 TgCH(4) yr(-1), range 73-108, + 19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30-40% on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project. Funding Agencies|Swiss National Science Foundation; NASA [NNX14AF93G, NNX14AO73G]; National Environmental Science Program - Earth Systems and Climate Change Hub; European Commission [283576, 633080]; ESA Climate Change Initiative Greenhouse Gases Phase 2 project; US Department of Energy, BER [DE-AC02-05CH11231]; FAO member countries; Environment Research and Technology Development Fund of the Ministry of the Environment, Japan [2-1502]; ERC [322998]; NERC [NE/J00748X/1]; Swedish Research Council VR; Research Council of Norway [244074]; NSF [1243232, 1243220]; National Science and Engineering Research Council of Canada (NSERC); Chinas QianRen Program; CSIRO Australia; Australian Bureau of Meteorology; Australian Institute of Marine Science; Australian Antarctic Division; NOAA USA; Meteorological Service of Canada; National Aeronautic and Space Administration (NASA) [NAG5-12669, NNX07AE89G, NNX11AF17G, NNX07AE87G, NNX07AF09G, NNX11AF15G, NNX11AF16G]; Department of Energy and Climate Change (DECC, UK) [GA01081]; Commonwealth Scientific and Industrial Research Organization (CSIRO Australia); Bureau of Meteorology (Australia); Joint DECC/Defra Met Office Hadley Centre Climate Programme [GA01101]