Time-resolved diffraction with femtosecond electron pulses has become a promising technique to directly provide insights into photo induced primary dynamics at the atomic level in molecules and ...solids. Ultrashort pulse duration as well as extensive spatial coherence are desired, however, space charge effects complicate the bunching of multiple electrons in a single pulse. We experimentally investigate the interplay between spatial and temporal aspects of resolution limits in ultrafast electron diffraction (UED) on our highly compact transmission electron diffractometer. To that end, the initial source size and charge density of electron bunches are systematically manipulated and the resulting bunch properties at the sample position are fully characterized in terms of lateral coherence, temporal width and diffracted intensity. We obtain a so far not reported measured overall temporal resolution of 130 fs (full width at half maximum) corresponding to 60 fs (root mean square) and transversal coherence lengths up to 20 nm. Instrumental impacts on the effective signal yield in diffraction and electron pulse brightness are discussed as well. The performance of our compact UED setup at selected electron pulse conditions is finally demonstrated in a time-resolved study of lattice heating in multilayer graphene after optical excitation.
This study investigates the use of total column CH4 (XCH4) retrievals from the SCIAMACHY satellite instrument for quantifying large-scale emissions of methane. A unique data set from SCIAMACHY is ...available spanning almost a decade of measurements, covering a period when the global CH4 growth rate showed a marked transition from stable to increasing mixing ratios. The TM5 4DVAR inverse modelling system has been used to infer CH4 emissions from a combination of satellite and surface measurements for the period 2003–2010. In contrast to earlier inverse modelling studies, the SCIAMACHY retrievals have been corrected for systematic errors using the TCCON network of ground-based Fourier transform spectrometers. The aim is to further investigate the role of bias correction of satellite data in inversions. Methods for bias correction are discussed, and the sensitivity of the optimized emissions to alternative bias correction functions is quantified. It is found that the use of SCIAMACHY retrievals in TM5 4DVAR increases the estimated inter-annual variability of large-scale fluxes by 22% compared with the use of only surface observations. The difference in global methane emissions between 2-year periods before and after July 2006 is estimated at 27–35 Tg yr−1. The use of SCIAMACHY retrievals causes a shift in the emissions from the extra-tropics to the tropics of 50 ± 25 Tg yr−1. The large uncertainty in this value arises from the uncertainty in the bias correction functions. Using measurements from the HIPPO and BARCA aircraft campaigns, we show that systematic errors in the SCIAMACHY measurements are a main factor limiting the performance of the inversions. To further constrain tropical emissions of methane using current and future satellite missions, extended validation capabilities in the tropics are of critical importance.
The 2018 drought was one of the worst European droughts of the twenty-first century in terms of its severity, extent and duration. The effects of the drought could be seen in a reduction in harvest ...yields in parts of Europe, as well as an unprecedented browning of vegetation in summer. Here, we quantify the effect of the drought on net ecosystem exchange (NEE) using five independent regional atmospheric inversion frameworks. Using a network of atmospheric CO
mole fraction observations, we estimate NEE with at least monthly and 0.5° × 0.5° resolution for 2009-2018. We find that the annual NEE in 2018 was likely more positive (less CO
uptake) in the temperate region of Europe by 0.09 ± 0.06 Pg C yr
(mean ± s.d.) compared to the mean of the last 10 years of -0.08 ± 0.17 Pg C yr
, making the region close to carbon neutral in 2018. Similarly, we find a positive annual NEE anomaly for the northern region of Europe of 0.02 ± 0.02 Pg C yr
compared the 10-year mean of -0.04 ± 0.05 Pg C yr
. In both regions, this was largely owing to a reduction in the summer CO
uptake. The positive NEE anomalies coincided spatially and temporally with negative anomalies in soil water. These anomalies were exceptional for the 10-year period of our study. This article is part of the theme issue 'Impacts of the 2018 severe drought and heatwave in Europe: from site to continental scale'.
Traditional techniques for measuring the mole fractions of greenhouse gases in the well-mixed atmosphere have required dry sample gas streams (dew point < −25 °C) to achieve the inter-laboratory ...compatibility goals set forth by the Global Atmosphere Watch programme of the World Meteorological Organisation (WMO/GAW) for carbon dioxide (±0.1 ppm in the Northern Hemisphere and ±0.05 ppm in the Southern Hemisphere) and methane (±2 ppb). Drying the sample gas to low levels of water vapour can be expensive, time-consuming, and/or problematic, especially at remote sites where access is difficult. Recent advances in optical measurement techniques, in particular cavity ring down spectroscopy, have led to the development of greenhouse gas analysers capable of simultaneous measurements of carbon dioxide, methane and water vapour. Unlike many older technologies, which can suffer from significant uncorrected interference from water vapour, these instruments permit accurate and precise greenhouse gas measurements that can meet the WMO/GAW inter-laboratory compatibility goals (WMO, 2011a) without drying the sample gas. In this paper, we present laboratory methodology for empirically deriving the water vapour correction factors, and we summarise a series of in-situ validation experiments comparing the measurements in humid gas streams to well-characterised dry-gas measurements. By using the manufacturer-supplied correction factors, the dry-mole fraction measurements have been demonstrated to be well within the GAW compatibility goals up to a water vapour concentration of at least 1%. By determining the correction factors for individual instruments once at the start of life, this water vapour concentration range can be extended to at least 2% over the life of the instrument, and if the correction factors are determined periodically over time, the evidence suggests that this range can be extended up to and even above 4% water vapour concentrations.
The causes of renewed growth in the atmospheric CH4 burden since 2007 are still poorly understood and subject of intensive scientific discussion. We present a reanalysis of global CH4 emissions ...during the 2000s, based on the TM5‐4DVAR inverse modeling system. The model is optimized using high‐accuracy surface observations from NOAA ESRL's global air sampling network for 2000–2010 combined with retrievals of column‐averaged CH4 mole fractions from SCIAMACHY onboard ENVISAT (starting 2003). Using climatological OH fields, derived global total emissions for 2007–2010 are 16–20 Tg CH4/yr higher compared to 2003–2005. Most of the inferred emission increase was located in the tropics (9–14 Tg CH4/yr) and mid‐latitudes of the northern hemisphere (6–8 Tg CH4/yr), while no significant trend was derived for Arctic latitudes. The atmospheric increase can be attributed mainly to increased anthropogenic emissions, but the derived trend is significantly smaller than estimated in the EDGARv4.2 emission inventory. Superimposed on the increasing trend in anthropogenic CH4 emissions are significant inter‐annual variations (IAV) of emissions from wetlands (up to ±10 Tg CH4/yr), and biomass burning (up to ±7 Tg CH4/yr). Sensitivity experiments, which investigated the impact of the SCIAMACHY observations (versus inversions using only surface observations), of the OH fields used, and of a priori emission inventories, resulted in differences in the detailed latitudinal attribution of CH4 emissions, but the IAV and trends aggregated over larger latitude bands were reasonably robust. All sensitivity experiments show similar performance against independent shipboard and airborne observations used for validation, except over Amazonia where satellite retrievals improved agreement with observations in the free troposphere.
Key Points
A reanalysis of global CH4 emissions during the 2000s is presented
derived global total emissions 2007‐2010 16‐20 Tg CH4/yr higher than 2003‐2005
increase mainly in the tropics and NH mid‐latitudes
We introduce a tool to determine surface fluxes from atmospheric concentration data in the midst of distributed sources or sinks over land, the Stochastic Time‐Inverted Lagrangian Transport (STILT) ...model, and illustrate the use of the tool with CO2 data over North America. Anthropogenic and biogenic emissions of trace gases at the surface cause large variations of atmospheric concentrations in the planetary boundary layer (PBL) from the “near field,” where upstream sources and sinks have strong influence on observations. Transport in the near field often takes place on scales not resolved by typical grid sizes in transport models. STILT provides the capability to represent near‐field influences, transforming this noise to signal useful in diagnosing surface emissions. The model simulates transport by following the time evolution of a particle ensemble, interpolating meteorological fields to the subgrid scale location of each particle. Turbulent motions are represented by a Markov chain process. Significant computational savings are realized because the influence of upstream emissions at different times is modeled using a single particle simulation backward in time, starting at the receptor and sampling only the portion of the domain that influences the observations. We assess in detail the physical and numerical requirements of STILT and other particle models necessary to avoid inconsistencies and to preserve time symmetry (reversibility). We show that source regions derived from backward and forward time simulations in STILT are similar, and we show that deviations may be attributed to violation of mass conservation in currently available analyzed meterological fields. Using concepts from information theory, we show that the particle approach can provide significant gains in information compared to conventional gridcell models, principally during the first hours of transport backward in time, when PBL observations are strongly affected by surface sources and sinks.
One of the dominant uncertainties in inverse estimates of regional CO2 surface-atmosphere fluxes is related to model errors in vertical transport within the planetary boundary layer (PBL). In this ...study we present the results from a synthetic experiment using the atmospheric model WRF-VPRM to realistically simulate transport of CO2 for large parts of the European continent at 10 km spatial resolution. To elucidate the impact of vertical mixing error on modeled CO2 mixing ratios we simulated a month during the growing season (August 2006) with different commonly used parameterizations of the PBL (Mellor-Yamada-Janjic (MYJ) and Yonsei-University (YSU) scheme). To isolate the effect of transport errors we prescribed the same CO2 surface fluxes for both simulations. Differences in simulated CO2 mixing ratios (model bias) were on the order of 3 ppm during daytime with larger values at night. We present a simple method to reduce this bias by 70-80% when the true height of the mixed layer is known.
Accurate simulation of the spatial and temporal variability of tracer mixing ratios over complex terrain is challenging, but essential in order to utilize measurements made in complex orography (e.g. ...mountain and coastal sites) in an atmospheric inverse framework to better estimate regional fluxes of these trace gases. This study investigates the ability of high-resolution modeling tools to simulate meteorological and CO2 fields around Ochsenkopf tall tower, situated in Fichtelgebirge mountain range- Germany (1022 m a.s.l.; 50°1'48" N, 11°48'30" E). We used tower measurements made at different heights for different seasons together with the measurements from an aircraft campaign. Two tracer transport models - WRF (Eulerian based) and STILT (Lagrangian based), both with a 2 km horizontal resolution - are used together with the satellite-based biospheric model VPRM to simulate the distribution of atmospheric CO2 concentration over Ochsenkopf. The results suggest that the high-resolution models can capture diurnal, seasonal and synoptic variability of observed mixing ratios much better than coarse global models. The effects of mesoscale transports such as mountain-valley circulations and mountain-wave activities on atmospheric CO2 distributions are reproduced remarkably well in the high-resolution models. With this study, we emphasize the potential of using high-resolution models in the context of inverse modeling frameworks to utilize measurements provided from mountain or complex terrain sites.
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