ALBERT

Description: Although quantitative isotope data from speleothems has been used to evaluate isotope-enabled model simulations, currently no consensus exists regarding the most appropriate methodology through which to achieve this. A number of modelling groups will be running isotope-enabled palaeoclimate simulations in the framework of the Coupled Model Intercomparison Project Phase 6, so it is timely to evaluate different approaches to using the speleothem data for data–model comparisons. Here, we illustrate this using 456 globally distributed speleothem δ18O records from an updated version of the Speleothem Isotopes Synthesis and Analysis (SISAL) database and palaeoclimate simulations generated using the ECHAM5-wiso isotope-enabled atmospheric circulation model. We show that the SISAL records reproduce the first-order spatial patterns of isotopic variability in the modern day, strongly supporting the application of this dataset for evaluating model-derived isotope variability into the past. However, the discontinuous nature of many speleothem records complicates the process of procuring large numbers of records if data–model comparisons are made using the traditional approach of comparing anomalies between a control period and a given palaeoclimate experiment. To circumvent this issue, we illustrate techniques through which the absolute isotope values during any time period could be used for model evaluation. Specifically, we show that speleothem isotope records allow an assessment of a model’s ability to simulate spatial isotopic trends. Our analyses provide a protocol for using speleothem isotope data for model evaluation, including screening the observations to take into account the impact of speleothem mineralogy on δ18O values, the optimum period for the modern observational baseline and the selection of an appropriate time window for creating means of the isotope data for palaeo-time-slices.

Description: A tethered-balloon system (TBS) has been developed and is being operated by Sandia National Laboratories (SNL) on behalf of the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) User Facility in order to collect in situ atmospheric measurements within mixed-phase Arctic clouds. Periodic tethered-balloon flights have been conducted since 2015 within restricted airspace at ARM's Advanced Mobile Facility 3 (AMF3) in Oliktok Point, Alaska, as part of the AALCO (Aerial Assessment of Liquid in Clouds at Oliktok), ERASMUS (Evaluation of Routine Atmospheric Sounding Measurements using Unmanned Systems), and POPEYE (Profiling at Oliktok Point to Enhance YOPP Experiments) field campaigns. The tethered-balloon system uses helium-filled 34 m3 helikites and 79 and 104 m3 aerostats to suspend instrumentation that is used to measure aerosol particle size distributions, temperature, horizontal wind, pressure, relative humidity, turbulence, and cloud particle properties and to calibrate ground-based remote sensing instruments. Supercooled liquid water content (SLWC) sondes using the vibrating-wire principle, developed by Anasphere Inc., were operated at Oliktok Point at multiple altitudes on the TBS within mixed-phase clouds for over 200 h. Sonde-collected SLWC data were compared with liquid water content derived from a microwave radiometer, Ka-band ARM zenith radar, and ceilometer at the AMF3, as well as liquid water content derived from AMF3 radiosonde flights. The in situ data collected by the Anasphere sensors were also compared with data collected simultaneously by an alternative SLWC sensor developed at the University of Reading, UK; both vibrating-wire instruments were typically observed to shed their ice quickly upon exiting the cloud or reaching maximum ice loading. Temperature sensing measurements distributed with fiber optic tethered balloons were also compared with AMF3 radiosonde temperature measurements. Combined, the results indicate that TBS-distributed temperature sensing and supercooled liquid water measurements are in reasonably good agreement with remote sensing and radiosonde-based measurements of both properties. From these measurements and sensor evaluations, tethered-balloon flights are shown to offer an effective method of collecting data to inform and constrain numerical models, calibrate and validate remote sensing instruments, and characterize the flight environment of unmanned aircraft, circumventing the difficulties of in-cloud unmanned aircraft flights such as limited flight time and in-flight icing.

Description: The Hadean Jack Hills zircons represent the oldest known terrestrial material, providing a unique and truly direct record of Hadean Earth history. This zircon population has been extensively studied via high-spatial-resolution high-throughput in situ isotopic and elemental analysis techniques, such as secondary ionization mass spectrometry (SIMS), but not by comparatively destructive, high-temporal-precision (

Description: NASA's Orbiting Carbon Observatory-2 (OCO-2) has been measuring carbon dioxide column-averaged dry-air mole fraction, XCO2, in the Earth's atmosphere for over 2 years. In this paper, we describe the comparisons between the first major release of the OCO-2 retrieval algorithm (B7r) and XCO2 from OCO-2's primary ground-based validation network: the Total Carbon Column Observing Network (TCCON). The OCO-2 XCO2 retrievals, after filtering and bias correction, agree well when aggregated around and coincident with TCCON data in nadir, glint, and target observation modes, with absolute median differences less than 0.4 ppm and RMS differences less than 1.5 ppm. After bias correction, residual biases remain. These biases appear to depend on latitude, surface properties, and scattering by aerosols. It is thus crucial to continue measurement comparisons with TCCON to monitor and evaluate the OCO-2 XCO2 data quality throughout its mission.

Description: MIPAS thermal limb emission measurements were used to derive vertically resolved profiles of carbon tetrachloride (CCl4). Level-1b data versions MIPAS/5.02 to MIPAS/5.06 were converted into volume mixing ratio profiles using the level-2 processor developed at Karlsruhe Institute of Technology (KIT) Institute of Meteorology and Climate Research (IMK) and Consejo Superior de Investigaciones Científicas (CSIC), Instituto de Astrofísica de Andalucía (IAA). Consideration of peroxyacetyl nitrate (PAN) as an interfering species, which is jointly retrieved, and CO2 line mixing is crucial for reliable retrievals. Parts of the CO2 Q-branch region that overlap with the CCl4 signature were omitted, since large residuals were still found even though line mixing was considered in the forward model. However, the omitted spectral region could be narrowed noticeably when line mixing was accounted for. A new CCl4 spectroscopic data set leads to slightly smaller CCl4 volume mixing ratios. In general, latitude–altitude cross sections show the expected CCl4 features with highest values of around 90 pptv at altitudes at and below the tropical tropopause and values decreasing with altitude and latitude due to stratospheric decomposition. Other patterns, such as subsidence in the polar vortex during winter and early spring, are also visible in the distributions. The decline in CCl4 abundance during the MIPAS Envisat measurement period (July 2002 to April 2012) is clearly reflected in the altitude–latitude cross section of trends estimated from the entire retrieved data set.

Description: Various studies have reported that the photochemical nucleation of new ultrafine particles (UFPs) in urban environments within high insolation regions occurs simultaneously with high ground ozone (O3) levels. In this work, we evaluate the atmospheric dynamics leading to summer O3 episodes in the Madrid air basin (central Iberia) by means of measuring a 3-D distribution of concentrations for both pollutants. To this end, we obtained vertical profiles (up to 1200 m above ground level) using tethered balloons and miniaturised instrumentation at a suburban site located to the SW of the Madrid Metropolitan Area (MMA), the Majadahonda site (MJDH), in July 2016. Simultaneously, measurements of an extensive number of air quality and meteorological parameters were carried out at three supersites across the MMA. Furthermore, data from O3 soundings and daily radio soundings were also used to interpret atmospheric dynamics. The results demonstrate the concatenation of venting and accumulation episodes, with relative lows (venting) and peaks (accumulation) in O3 surface levels. Regardless of the episode type, the fumigation of high-altitude O3 (arising from a variety of origins) contributes the major proportion of surface O3 concentrations. Accumulation episodes are characterised by a relatively thinner planetary boundary layer ( 2400 m a.s.l.). This orographic–meteorological setting causes the vertical recirculation of air masses and enrichment of O3 in the lower tropospheric layers. When the highly polluted urban plume from Madrid is affected by these dynamics, the highest Ox (O3+ NO2) concentrations are recorded in the MMA. Vertical O3 profiles during venting episodes, with strong synoptic winds and a deepening of the planetary boundary layer reaching 〉 2000 m a.s.l., were characterised by an upward gradient in O3 levels, whereas a reverse situation with O3 concentration maxima at lower levels was found during the accumulation episodes due to local and/or regional production. The two contributions to O3 surface levels (fumigation from high-altitude strata, a high O3 background, and/or regional production) require very different approaches for policy actions. In contrast to O3 vertical top-down transfer, UFPs are formed in the planetary boundary layer (PBL) and are transferred upwards progressively with the increase in PBL growth.

Description: New particle formation (NPF) events have different patterns of development depending on the conditions of the area in which they occur. In this study, particle size distributions in the range of 16.6–604 nm (7 years of data) were analysed and NPF events occurring at three sites of differing characteristics – rural Harwell (HAR), urban background North Kensington (NK), urban roadside Marylebone Road (MR), London, UK – were extracted and studied. The different atmospheric conditions in each study area not only have an effect on the frequency of the events, but also affect their development. The frequency of NPF events is similar at the rural and urban background locations (about 7 % of days), with a high proportion of events occurring at both sites on the same day (45 %). The frequency of NPF events at the urban roadside site is slightly less (6 % of days), and higher particle growth rates (average 5.5 nm h−1 at MR compared to 3.4 and 4.2 nm h−1 at HAR and NK respectively) must result from rapid gas-to-particle conversion of traffic-generated pollutants. A general pattern is found in which the condensation sink increases with the degree of pollution of the site, but this is counteracted by increased particle growth rates at the more polluted location. A key finding of this study is that the role of the urban environment leads to an increment of 20 % in N16–20 nm in the urban background compared to that of the rural area in NPF events occurring at both sites. The relationship of the origin of incoming air masses is also considered and an association of regional events with cleaner air masses is found. Due to lower availability of condensable species, NPF events that are associated with cleaner atmospheric conditions have lower growth rates of the newly formed particles. The decisive effect of the condensation sink in the development of NPF events and the survivability of the newly formed particles is underlined, and influences the overall contribution of NPF events to the number of ultrafine particles in an area. The other key factor identified by this study is the important role that pollution, both from traffic and other sources in the urban environment (such as heating or cooking), plays in new particle formation events.

Description: The Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme is an international collaborative project focusing on understanding the sources, processes and health effects of air pollution in the Beijing megacity. APHH-Beijing brings together leading China and UK research groups, state-of-the-art infrastructure and air quality models to work on four research themes: (1) sources and emissions of air pollutants; (2) atmospheric processes affecting urban air pollution; (3) air pollution exposure and health impacts; and (4) interventions and solutions. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 to develop cost-effective air pollution mitigation solutions. This paper provides an introduction to (i) the rationale of the APHH-Beijing programme and (ii) the measurement and modelling activities performed as part of it. In addition, this paper introduces the meteorology and air quality conditions during two joint intensive field campaigns – a core integration activity in APHH-Beijing. The coordinated campaigns provided observations of the atmospheric chemistry and physics at two sites: (i) the Institute of Atmospheric Physics in central Beijing and (ii) Pinggu in rural Beijing during 10 November–10 December 2016 (winter) and 21 May–22 June 2017 (summer). The campaigns were complemented by numerical modelling and automatic air quality and low-cost sensor observations in the Beijing megacity. In summary, the paper provides background information on the APHH-Beijing programme and sets the scene for more focused papers addressing specific aspects, processes and effects of air pollution in Beijing.

Description: Particle number size distributions have been measured simultaneously by scanning mobility particle sizers (SMPSs) at five sites in central London for a 1 month campaign in January–February 2017. These measurements were accompanied by condensation particle counters (CPCs) to measure total particle number count at four of the sites and Aethalometers measuring black carbon (BC) at five sites. The spatial distribution and inter-relationships of the particle size distribution and SMPS total number counts with CPC total number counts and black carbon measurements have been analysed in detail as well as variations in the size distributions. One site (Marylebone Road) was in a street canyon with heavy traffic, one site (Westminster University) was on a rooftop adjacent to the Marylebone Road sampler, and a further sampler was located at Regent's University within a major park to the north of Marylebone Road. A fourth sampler was located nearby at 160 m above ground level on the BT tower and a fifth sampler was located 4 km to the west of the main sampling region at North Kensington. Consistent with earlier studies it was found that the mode in the size distribution had shifted to smaller sizes at the Regent's University (park) site, the mean particle shrinkage rate being 0.04 nm s−1 with slightly lower values at low wind speeds and some larger values at higher wind speeds. There was evidence of complete evaporation of the semi-volatile nucleation mode under certain conditions at the elevated BT Tower site. While the SMPS total count and black carbon showed typical traffic-dominated diurnal profiles, the CPC count data typically peaked during night-time as did CPC∕SMPS and CPC∕BC ratios. This is thought to be due to the presence of high concentrations of small particles (2.5–15 nm diameter) probably arising from condensational growth from traffic emissions during the cooler night-time conditions. Such behaviour was most marked at the Regent's University and Westminster University sites and less so at Marylebone Road, while at the elevated BT Tower site the ratio of particle number (CPC) to black carbon peaked during the morning rush hour and not at night-time, unlike the other sites. An elevation in nucleation mode particles associated with winds from the west and WSW sector was concluded to result from emissions from London Heathrow Airport, despite a distance of 22 km from the central London sites.

Description: Three groups of aliphatic carbonyl compounds, the n-alkanals (C8–C20), n-alkan-2-ones (C8–C26), and n-alkan-3-ones (C8–C19), were measured in both particulate and vapour phases in air samples collected in London from January to April 2017. Four sites were sampled including two rooftop background sites, one ground-level urban background site, and a street canyon location on Marylebone Road in central London. The n-alkanals showed the highest concentrations, followed by the n-alkan-2-ones and the n-alkan-3-ones, the latter having appreciably lower concentrations. It seems likely that all compound groups have both primary and secondary sources and these are considered in light of published laboratory work on the oxidation products of high-molecular-weight n-alkanes. All compound groups show a relatively low correlation with black carbon and NOx in the background air of London, but in street canyon air heavily impacted by vehicle emissions, stronger correlations emerge, especially for the n-alkanals. It appears that vehicle exhaust is likely to be a major contributor for concentrations of the n-alkanals, whereas it is a much smaller contributor to the n-alkan-2-ones and n-alkan-3-ones. Other primary sources such as cooking or wood burning may be contributors for the ketones but were not directly evaluated. It seems likely that there is also a significant contribution from the photo-oxidation of n-alkanes and this would be consistent with the much higher abundance of n-alkan-2-ones relative to n-alkan-3-ones if the formation mechanism were through the oxidation of condensed-phase alkanes. Vapour–particle partitioning fitted the Pankow model well for the n-alkan-2-ones but less well for the other compound groups, although somewhat stronger relationships were seen at the Marylebone Road site than at the background sites. The former observation gives support to the n-alkane-2-ones being a predominantly secondary product, whereas primary sources of the other groups are more prominent.