<p>The oxygen emission band at 60 GHz is a commonly used frequency band for atmospheric temperature sounding. The fine structure emission lines used to retrieve temperature in the stratosphere and mesosphere are affected by the Zeeman effect, which has a characteristic influence on the spectral shape of different polarization states. As a consequence of this effect, a <span class="inline-formula"><i>V</i></span>-Stokes component is generated, indicating symmetry breaking between right and left circular polarized radiation. In this study, we present the full-rank Stokes vector of the fine structure emission lines at 53.067 and 53.596 GHz, measured with a fully polarimetric radiometer. We discuss the advantages of the fully polarimetric approach compared to single-polarization observations for temperature sounding by comparing both simulations and observations. Our findings show that using circular polarization in the retrieval algorithm improves both the upper altitude limit and vertical resolution by several kilometers. Additionally, we introduce an operational calibration method and present calibrated spectra for the four components of the Stokes polarization vector. We also provide a continuous series of retrieved temperature profiles, demonstrating that the calibration is valid for continuous observations.</p>
<p>Africa is a critical source of biomass burning (BB) aerosols, and its importance is increasing. The African Combustion Aerosol Collaborative Intercomparison Analysis (ACACIA) Pilot Project set to optically characterize BB aerosol generated from sub-Saharan African fuels. We used a photoacoustic spectrometer as a reference instrument to determine the multiple-scattering correction factor <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> for an AE33 aethalometer at three wavelengths, which produced weighted mean values of <span class="inline-formula"><i>C</i><sub>370</sub>=3.69</span>, <span class="inline-formula"><i>C</i><sub>470</sub>=5.65</span>, and <span class="inline-formula"><i>C</i><sub>520</sub>=6.39</span>. <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> increased with wavelength and <span class="inline-formula"><i>C</i><sub>370</sub></span> was statistically independent of the others, suggesting a single <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> is insufficient, especially in BB scenarios. While a dependence of <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> on burning state was not found, <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> was shown to strongly relate to particle single scattering albedo (SSA, <span class="inline-formula"><i>ω</i>)</span>. When <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> was plotted against SSA, values slowly rose at low SSA values, followed by a sharp rise around an SSA of <span class="inline-formula">∼</span> 0.9; indicating a larger correction needed for less absorbing aerosol. A number of functions operating on either SSA or <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> were explored and the best function was <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M14" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><msub><mi>C</mi><mi mathvariant="italic">λ</mi></msub><mo>/</mo><mo>(</mo><mn mathvariant="normal">1</mn><mo>-</mo><msub><mi>C</mi><mi mathvariant="italic">λ</mi></msub><mo>)</mo><mo>=</mo><mi>A</mi><mi mathvariant="italic">ω</mi><mo>+</mo><mi>B</mi></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="112pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="816afa37feb768cfd6c442b0a557c5aa"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="amt-19-307-2026-ie00001.svg" width="112pt" height="14pt" src="amt-19-307-2026-ie00001.png"/></svg:svg></span></span>. This is an important parametrization of <span class="inline-formula"><i>C</i><sub><i>λ</i></sub></span> specifically geared towards BB aerosol from African fuels under different aging states, and is of particular importance for future field work in that continent. An Ångström matrix plot shows that African BB aerosol can have values more akin to dust, which demonstrates that these fuels are distinct in their wavelength dependence from more typical BB aerosol. Lastly, we examined the mass extinction and absorbance cross sections for BB aerosol generated for the same fuels with two different tube furnace setups. Not only is this combustion method flexible, it was found to be reproducible between labs.</p>
<p>Since its launch in 2018, the European Space Agency's
Earth Explorer satellite Aeolus has provided global height resolved
measurements of horizontal wind in the troposphere and lower stratosphere
for the first time. Novel datasets such as these provide an unprecedented
opportunity for the research of atmospheric dynamics and provide new
insights into the dynamics of the upper troposphere and lower stratosphere
(UTLS) region. Aeolus measures the wind component along its horizontal
line-of-sight, but for the analysis and interpretation of atmospheric
dynamics, zonal and/or meridional wind components are most useful. In this
paper, we introduce and compare three different methods to derive zonal and
meridional wind components from the Aeolus wind measurements. We find that
the most promising method involves combining Aeolus measurements during
ascending and descending orbits. Using this method, we derive global
estimates of the zonal wind in the latitude range 79.7<span class="inline-formula"><sup>∘</sup></span> S to
84.5<span class="inline-formula"><sup>∘</sup></span> N with errors of less than 5 m s<span class="inline-formula"><sup>−1</sup></span> (at the 2<span class="inline-formula"><i>σ</i></span>
level). Due to the orbit geometry of Aeolus, the estimation of meridional
wind in the tropics and at midlatitudes is more challenging and the quality
is less reliable. However, we find that it is possible to derive meridional
winds poleward of 70<span class="inline-formula"><sup>∘</sup></span> latitude with absolute errors typically
below 5 m s<span class="inline-formula"><sup>−1</sup></span> (at the 2<span class="inline-formula"><i>σ</i></span> level). This further demonstrates the value of Aeolus wind measurements for applications in weather and climate research, in addition to their important role in numerical weather
prediction.</p>
<p>Online characterization of aerosol composition at the
near-molecular level is key to understanding chemical reaction mechanisms,
kinetics, and sources under various atmospheric conditions. The recently
developed extractive electrospray ionization time-of-flight mass
spectrometer (EESI-TOF) is capable of detecting a wide range of organic
oxidation products in the particle phase in real time with minimal
fragmentation. Quantification can sometimes be hindered by a lack of
available commercial standards for aerosol constituents, however. Good
correlations between the EESI-TOF and other aerosol speciation techniques
have been reported, though no attempts have yet been made to parameterize
the EESI-TOF response factor for different chemical species. Here, we report
the first parameterization of the EESI-TOF response factor for secondary
organic aerosol (SOA) at the near-molecular level based on its elemental
composition. SOA was formed by ozonolysis of monoterpene or OH oxidation of
aromatics inside an oxidation flow reactor (OFR) using ammonium nitrate as
seed particles. A Vocus proton-transfer reaction mass spectrometer
(Vocus-PTR) and a high-resolution aerosol mass spectrometer (AMS) were used
to determine the gas-phase molecular composition and the particle-phase bulk
chemical composition, respectively. The EESI response factors towards bulk
SOA coating and the inorganic seed particle core were constrained by
intercomparison with the AMS. The highest bulk EESI response factor was
observed for SOA produced from 1,3,5-trimethylbenzene, followed by those
produced from <span class="inline-formula"><i>d</i></span>-limonene and <span class="inline-formula"><i>o</i></span>-cresol, consistent with previous findings. The
near-molecular EESI response factors were derived from intercomparisons with
Vocus-PTR measurements and were found to vary from 10<span class="inline-formula"><sup>3</sup></span> to 10<span class="inline-formula"><sup>6</sup></span> ion counts s<span class="inline-formula"><sup>−1</sup></span> ppb<span class="inline-formula"><sup>−1</sup></span>, mostly within <span class="inline-formula">±1</span> order of magnitude of
their geometric mean of 10<span class="inline-formula"><sup>4.6</sup></span> ion counts s<span class="inline-formula"><sup>−1</sup></span> ppb<span class="inline-formula"><sup>−1</sup></span>. For aromatic
SOA components, the EESI response factors correlated with molecular weight
and oxygen content and inversely correlated with volatility. The
near-molecular response factors mostly agreed within a factor of 20 for
isomers observed across the aromatics and biogenic systems. Parameterization
of the near-molecular response factors based on the measured elemental
formulae could reproduce the empirically determined response factor for a
single volatile organic compound (VOC) system to within a factor of 5 for the configuration of our mass
spectrometers. The results demonstrate that standard-free quantification
using the EESI-TOF is possible.</p>
<p>In order to validate satellite measurements of
atmospheric composition, it is necessary to understand the range of random
and systematic uncertainties inherent in the measurements. On occasions
where measurements from two different satellite instruments do not agree
within those estimated uncertainties, a common explanation is that the
difference can be assigned to geophysical variability, i.e., differences due
to sampling the atmosphere at different times and locations. However, the
expected geophysical variability is often left ambiguous and rarely
quantified. This paper describes a case study where the geophysical
variability of O<span class="inline-formula"><sub>3</sub></span> between two satellite instruments – ACE-FTS
(Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) and
OSIRIS (Optical Spectrograph and InfraRed Imaging System) – is estimated
using simulations from climate models. This is done by sampling the models
CMAM (Canadian Middle Atmosphere Model), EMAC (ECHAM/MESSy Atmospheric
Chemistry), and WACCM (Whole Atmosphere Community Climate Model) throughout
the upper troposphere and stratosphere at times and geolocations of
coincident ACE-FTS and OSIRIS measurements. Ensemble mean values show that
in the lower stratosphere, O<span class="inline-formula"><sub>3</sub></span> geophysical variability tends to be
independent of the chosen time coincidence criterion, up to within 12 h; and
conversely, in the upper stratosphere geophysical variation tends to be
independent of the chosen distance criterion, up to within 2000 km. It was
also found that in the lower stratosphere, at altitudes where there is the
greatest difference between air composition inside and outside the polar
vortex, the geophysical variability in the southern polar region can be
double of that in the northern polar region. This study shows that the
ensemble mean estimates of geophysical variation can be used when comparing
data from two satellite instruments to optimize the coincidence criteria,
allowing for the use of more coincident profiles while providing an estimate
of the geophysical variation within the comparison results.</p>
<p>Since 2009, the Greenhouse gases Observing SATellite (GOSAT) has performed
radiance measurements in the near-infrared (NIR) and
shortwave infrared (SWIR) spectral region.
From February 2019 onward, data from GOSAT-2 have also been available.</p>
<p>We present the first results from the application of the Fast atmOspheric
traCe gAs retrievaL (FOCAL) algorithm to derive
column-averaged dry-air mole fractions of carbon dioxide (<span class="inline-formula">XCO<sub>2</sub></span>) from GOSAT and
GOSAT-2 radiances and their validation.
FOCAL was initially developed for OCO-2 <span class="inline-formula">XCO<sub>2</sub></span> retrievals and
allows simultaneous retrievals of several gases over both land and
ocean.
Because FOCAL is accurate and numerically very fast, it is currently
being considered as a candidate algorithm for the forthcoming European
anthropogenic <span class="inline-formula">CO<sub>2</sub></span> Monitoring (CO2M) mission to be launched
in 2025.</p>
<p>We present the adaptation of FOCAL to GOSAT and discuss the changes
made and GOSAT specific additions.
This particularly includes modifications in pre-processing (e.g. cloud
detection) and post-processing (bias correction and filtering).</p>
<p><span id="page3838"/>A feature of the new application of FOCAL to GOSAT and GOSAT-2 is the
independent use of both S- and P-polarisation spectra in the retrieval.
This is not possible for OCO-2, which measures only one polarisation
direction.
Additionally, we make use of GOSAT's wider spectral coverage compared
to OCO-2 and derive not only <span class="inline-formula">XCO<sub>2</sub></span>, water vapour
(<span class="inline-formula">H<sub>2</sub>O</span>), and solar-induced fluorescence (SIF) but also methane
(<span class="inline-formula">XCH<sub>4</sub>)</span>, with the potential for further atmospheric
constituents and parameters like semi-heavy water vapour (<span class="inline-formula">HDO</span>). In the case of GOSAT-2, the retrieval of nitrous oxide (<span class="inline-formula">XN<sub>2</sub>O</span>) and carbon monoxide (<span class="inline-formula">CO</span>) may also be possible.</p>
<p>Here, we concentrate on the new FOCAL <span class="inline-formula">XCO<sub>2</sub></span> data products.
We describe the generation of the products as well as applied
filtering and bias correction procedures.
GOSAT-FOCAL <span class="inline-formula">XCO<sub>2</sub></span> data have been produced for the time interval 2009 to 2019. Comparisons with other independent GOSAT data sets reveal
agreement of long-term temporal variations within about
1 <span class="inline-formula">ppm</span> over 1 decade; differences in seasonal variations of
about 0.5 <span class="inline-formula">ppm</span> are observed.
Furthermore, we obtain a station-to-station bias of the new GOSAT-FOCAL
product to the ground-based Total Carbon Column Observing Network
(TCCON) of 0.56 <span class="inline-formula">ppm</span> with a mean scatter of 1.89 <span class="inline-formula">ppm</span>.</p>
<p>The GOSAT-2-FOCAL <span class="inline-formula">XCO<sub>2</sub></span> product is generated in a similar way as the
GOSAT-FOCAL product, but with adapted settings. All GOSAT-2 data until the end of 2019 have been processed. Because of this limited time interval, the GOSAT-2 results are considered to be preliminary only, but first comparisons show that these data compare well with the GOSAT-FOCAL results and also TCCON.</p>
<p>The tropical tropopause layer (TTL; 14–18.5 km) is the gateway for
most air entering the stratosphere, and therefore processes within this
layer have an outsized influence in determining global stratospheric ozone
and water vapor concentrations. Despite the importance of this layer there
are few in situ measurements with the necessary detail to resolve the fine-scale processes within this region. Here, we introduce a novel platform for
high-resolution in situ profiling that lowers and retracts a suspended
instrument package beneath drifting long-duration balloons in the tropics.
During a 100 d circumtropical flight, the instrument collected over a hundred 2 km profiles of temperature, water vapor, and aerosol at 1 m resolution, yielding unprecedented geographic sampling and vertical
resolution. The instrument system integrates proven sensors for water vapor,
temperature, pressure, and cloud and aerosol particles with an innovative
mechanical reeling and control system. A technical evaluation of the system
performance demonstrated the feasibility of this new measurement platform
for future missions with minor modifications. Six instruments planned for
two upcoming field campaigns are expected to provide over 4000 profiles
through the TTL, quadrupling the number of high-resolution aircraft and
balloon profiles collected to date. These and future measurements will
provide the necessary resolution to diagnose the importance of competing
mechanisms for the transport of water vapor across the TTL.</p>
<p>An improved two-sphere integration (TSI) technique has been
developed to quantify black carbon (BC) concentrations in the atmosphere and
seasonal snow. The major advantage of this system is that it combines two
distinct integrated spheres to reduce the scattering effect due to
light-absorbing particles and thus provides accurate determinations of
total light absorption from BC collected on Nuclepore filters. The TSI
technique can be calibrated using a series of 15 filter samples of standard
fullerene soot. This technique quantifies the mass of BC by separating the
spectrally resolved total light absorption into BC and non-BC fractions. To
assess the accuracy of the improved system, an empirical procedure for
measuring BC concentrations with a two-step thermal–optical method is also
applied. Laboratory results indicate that the BC concentrations determined using
the TSI technique and theoretical calculations are well correlated
(<span class="inline-formula"><i>R</i><sup>2</sup>=0.99</span>), whereas the thermal–optical method underestimates BC
concentrations by 35 %–45 % compared to that measured by the TSI technique.
Assessments of the two methods for atmospheric and snow samples revealed
excellent agreement, with least-squares regression lines with slopes of 1.72
(<span class="inline-formula"><i>r</i><sup>2</sup>=0.67</span>) and 0.84 (<span class="inline-formula"><i>r</i><sup>2</sup>=0.93</span>), respectively. However, the
TSI technique is more accurate in quantifications of BC concentrations in
both the atmosphere and seasonal snow, with an overall lower uncertainty.
Using the improved TSI technique, we find that light absorption at a
wavelength of 550 nm due to BC plays a dominant role relative to non-BC
light absorption in both the atmosphere (62.76 %–91.84 % of total
light absorption) and seasonal snow (43.11 %–88.56 %) over northern
China.</p>
<p>Atmospheric gravity waves generated downstream by orography in a stratified airflow are known as lee waves. In the present study, such mesoscale patterns have been detected, over water and in clear-sky conditions, using the Advanced Infra-Red WAter Vapour Estimator (AIRWAVE) total column water vapour (TCWV) dataset, which contains about 20 years of day and night products, obtained from the thermal infrared measurements of the Along Track Scanning Radiometer (ATSR) instrument series. The high accuracy of such data, along with the native 1 km<span class="inline-formula">×1</span> km spatial resolution, allows the investigation of small-scale features such as lee waves. In this work, we focused on the Mediterranean Sea, the largest semi-enclosed basin on the Earth. The peculiarities of this area, which is characterised by complex orography and rough coastlines, lead to the development of these structures over both land and sea. We developed an automatic tool for the rapid detection of areas with high probability of lee wave occurrence, exploiting the TCWV variability in spatial regions with a <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M2" display="inline" overflow="scroll" dspmath="mathml"><mrow><mn mathvariant="normal">0.15</mn><msup><mi/><mo>∘</mo></msup><mo>×</mo><mn mathvariant="normal">0.15</mn><msup><mi/><mo>∘</mo></msup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="64pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="ee0891df08a2383d412e7b879dfcc029"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="amt-12-6683-2019-ie00001.svg" width="64pt" height="11pt" src="amt-12-6683-2019-ie00001.png"/></svg:svg></span></span> area. Through this analysis, several occurrences of structures connected with lee waves have been observed. The waves are detected in spring, autumn and summer seasons, with TCWV values usually falling in the range of 15 to 35 kg m<span class="inline-formula"><sup>−2</sup></span>. In this article, we describe some cases over the central (Italy) and the Eastern Mediterranean Basin (Greece, Turkey and Cyprus). We compared a case of perturbed AIRWAVE TCWV fields due to lee waves occurring over the Tyrrhenian Sea on 18 July 1997 with the sea surface winds from the synthetic aperture radar (SAR), which sounded the same geographical area, finding a good agreement. Another case has been investigated in detail: on 2 August 2002 the Aegean Sea region was almost simultaneously sounded by both the second sensor of the ATSR series (ATSR-2) and the Advanced ATSR (AATSR) instruments. The AIRWAVE TCWV fields derived from the two sensors were successfully compared with the vertically integrated water vapour content simulated with the Weather Research and Forecasting (WRF) numerical model for the same time period, confirming our findings. Wave parameters such as amplitude, wavelength and phase are described through the use of the Morlet continuous wavelet transformation (CWT). The performed analysis derived typical wavelengths from 6 to 8 km and amplitudes of up to 20 kg m<span class="inline-formula"><sup>−2</sup></span>.</p>
<p>Assessing the intracity spatial distribution and temporal variability in air
quality can be facilitated by a dense network of monitoring stations.
However, the cost of implementing such a network can be prohibitive if
traditional high-quality, expensive monitoring systems are used. To this end,
the Real-time Affordable Multi-Pollutant (RAMP) monitor has been developed,
which can measure up to five gases including the criteria pollutant gases
carbon monoxide (CO), nitrogen dioxide (<span class="inline-formula">NO<sub>2</sub></span>), and ozone
(<span class="inline-formula">O<sub>3</sub></span>), along with temperature and relative humidity. This study
compares various algorithms to calibrate the RAMP measurements including
linear and quadratic regression, clustering, neural networks, Gaussian
processes, and hybrid random forest–linear regression
models. Using data collected by almost 70 RAMP monitors over periods ranging
up to 18 months, we recommend the use of limited quadratic regression
calibration models for CO, neural network models for NO, and hybrid models
for <span class="inline-formula">NO<sub>2</sub></span> and <span class="inline-formula">O<sub>3</sub></span> for any low-cost monitor using
electrochemical sensors similar to those of the RAMP. Furthermore,
generalized calibration models may be used instead of individual models with
only a small reduction in overall performance. Generalized models also
transfer better when the RAMP is deployed to other locations. For long-term
deployments, it is recommended that model performance be re-evaluated and new
models developed periodically, due to the noticeable change in performance
over periods of a year or more. This makes generalized calibration models
even more useful since only a subset of deployed monitors are needed to build
these new models. These results will help guide future efforts in the
calibration and use of low-cost sensor systems worldwide.</p>
<p>Sampling the atmosphere to analyze contaminants is
different from other environmental matrices because measuring the volume of
air collected requires a mechanical flow-through device to draw the air and
measure its flow rate. The device used must have the capability of
concentrating the analytes of interest onto a different substrate because
the volumes of air needed are often on the order of hundreds of cubic meters. The use
of high-volume air samplers has grown since 1967, when recommended limits of
a large number of organic contaminants in air were developed. Equations used
for calculating the air flow through the device over time have similarly
been developed. However, the complete derivation of those equations has
never appeared in the scientific literature. Here a thorough derivation of
those equations is provided with definitions of the mechanical systems that
are used in the process, along with the method of calibrating and
calculating air flow.</p>
Accurate gas velocity measurements in emission plumes are
highly desirable for various atmospheric remote sensing applications. The
imaging technique of UV SO<sub>2</sub> cameras is commonly used to monitor
SO<sub>2</sub> emissions from volcanoes and anthropogenic sources (e.g. power
plants, ships). The camera systems capture the emission plumes at high
spatial and temporal resolution. This allows the gas velocities
in the plume to be retrieved directly from the images. The latter can be measured at a pixel
level using optical flow (OF) algorithms. This is particularly advantageous
under turbulent plume conditions. However, OF algorithms intrinsically rely
on contrast in the images and often fail to detect motion in low-contrast
image areas. We present a new method to identify ill-constrained OF
motion vectors and replace them using the local average velocity vector. The
latter is derived based on histograms of the retrieved OF motion fields. The
new method is applied to two example data sets recorded at Mt Etna (Italy)
and Guallatiri (Chile). We show that in many cases, the uncorrected OF yields
significantly underestimated SO<sub>2</sub> emission rates. We further show that our proposed correction can account for this and that it significantly
improves the reliability of optical-flow-based gas velocity retrievals.
<br><br>
In the case of Mt Etna, the SO<sub>2</sub> emissions of the north-eastern crater
are investigated. The corrected SO<sub>2</sub> emission rates range between
4.8 and 10.7 kg s<sup>−1</sup> (average of 7.1 ± 1.3 kg s<sup>−1</sup>)
and are in good agreement with previously reported values. For the Guallatiri
data, the emissions of the central crater and a fumarolic field are
investigated. The retrieved SO<sub>2</sub> emission rates are between
0.5 and 2.9 kg s<sup>−1</sup> (average of 1.3 ± 0.5 kg s<sup>−1</sup>) and
provide the first report of SO<sub>2</sub> emissions from this remotely located
and inaccessible volcano.
Oxidation flow reactors that use low-pressure mercury lamps to produce
hydroxyl (OH) radicals are an emerging technique for studying the oxidative
aging of organic aerosols. Here, ozone (O<sub>3</sub>) is photolyzed at 254 nm
to produce O(<sup>1</sup>D) radicals, which react with water vapor to produce
OH. However, the need to use parts-per-million levels of O<sub>3</sub> hinders
the ability of oxidation flow reactors to simulate NO<sub><i>x</i></sub>-dependent
secondary organic aerosol (SOA) formation pathways. Simple addition of nitric
oxide (NO) results in fast conversion of NO<sub><i>x</i></sub>
(NO + NO<sub>2</sub>) to nitric acid (HNO<sub>3</sub>), making it impossible to
sustain NO<sub><i>x</i></sub> at levels that are sufficient to compete with
hydroperoxy (HO<sub>2</sub>) radicals as a sink for organic peroxy (RO<sub>2</sub>)
radicals. We developed a new method that is well suited to the
characterization of NO<sub><i>x</i></sub>-dependent SOA formation pathways in
oxidation flow reactors. NO and NO<sub>2</sub> are produced via the reaction
O(<sup>1</sup>D) + N<sub>2</sub>O → 2NO, followed by the reaction
NO + O<sub>3</sub> → NO<sub>2</sub> + O<sub>2</sub>. Laboratory
measurements coupled with photochemical model simulations suggest that
O(<sup>1</sup>D) + N<sub>2</sub>O reactions can be used to systematically vary
the relative branching ratio of RO<sub>2</sub> + NO reactions relative to
RO<sub>2</sub> + HO<sub>2</sub> and/or RO<sub>2</sub> + RO<sub>2</sub> reactions
over a range of conditions relevant to atmospheric SOA formation. We
demonstrate proof of concept using high-resolution time-of-flight chemical
ionization mass spectrometer (HR-ToF-CIMS) measurements with nitrate
(NO<sub>3</sub><sup>−</sup>) reagent ion to detect gas-phase oxidation products of
isoprene and <i>α</i>-pinene previously observed in
NO<sub><i>x</i></sub>-influenced environments and in laboratory chamber
experiments.
Three algorithms for estimating the boundary layer heights are assessed: an
aerosol gradient method, a cluster analysis method, and a Haar wavelet
method. Over 40 daytime clear-sky radiosonde profiles are used to compare
aerosol backscatter boundary layer heights retrieved by a Vaisala CL31
ceilometer. Overall good agreement between radiosonde- and aerosol-derived
boundary layer heights was found for all methods. The cluster method was
found to be particularly sensitive to noise in ceilometer signals and lofted
aerosol layers (48.8 % of comparisons), while the gradient method showed
limitations in low-aerosol-backscatter conditions. The Haar wavelet method
was demonstrated to be the most robust, only showing limitations in 22.5 % of
all observations. Occasional differences between thermodynamically and
aerosol-derived boundary layer heights were observed.
Measuring sub-3 nm particles outside of controlled laboratory conditions is
a challenging task, as many of the instruments are operated at their limits
and are subject to changing ambient conditions. In this study, we advance the
current understanding of the operation of the Airmodus A11 nano Condensation
Nucleus Counter (nCNC), which consists of an A10 Particle Size Magnifier
(PSM) and an A20 Condensation Particle Counter (CPC). The effect of the inlet
line pressure on the measured particle concentration was measured, and two
separate regions inside the A10, where supersaturation of working fluid can
take place, were identified. The possibility of varying the lower cut-off
diameter of the nCNC was investigated; by scanning the growth tube
temperature, the range of the lower cut-off was extended from 1–2.5 to
1–6 nm. Here we present a new inlet system, which allows automated
measurement of the background concentration of homogeneously nucleated
droplets, minimizes the diffusion losses in the sampling line and is equipped
with an electrostatic filter to remove ions smaller than approximately
4.5 nm. Finally, our view of the guidelines for the optimal use of the
Airmodus nCNC is provided.
Eddy covariance using infrared gas analyzes has been a useful tool for gas
exchange measurements between soil, vegetation and the atmosphere. So far,
comparisons between the open- and closed-path eddy covariance (CP) system
have been extensively made on CO<sub>2</sub> flux estimations, while lacking in
the comparison of water vapor flux estimations. In this study, the specific
performance of water vapor flux measurements of an open-path eddy covariance
(OP) system was compared against a CP system over a tall temperate forest in
northeastern China. The results show that the fluxes from the OP system
(<i>LE</i><sub>op</sub>) were generally greater than the <i>LE</i><sub>cp</sub> though the two systems
shared one sonic anemometer. The tube delay of closed-path analyzer depended
on relative humidity, and the fixed median time lag contributed to a
significant underestimation of <i>LE</i><sub>cp</sub> between the forest and atmosphere,
while slight systematic overestimation was also found for covariance
maximization method with single broad time lag search window. After the
optimized time lag compensation was made, the average difference between the
30 min <i>LE</i><sub>op</sub> and <i>LE</i><sub>cp</sub> was generally within 6.0 %. Integrated over
the annual cycle, the CP system yielded a 5.1 % underestimation of forest
evapotranspiration as compared to the OP system measurements (493 vs. 469 mm yr<sup>−1</sup>). This study indicates the importance to
estimate the sampling tube delay accurately for water vapor flux
calculations with closed-path analyzers, and it also suggests that some of
the imbalance of the surface energy budget in flux sites is possibly
caused by the systematic underestimation of water vapor fluxes measured with
closed-path eddy covariance systems.
The microphysical properties of rainfall at the island of Réunion are analysed
and quantified according to one year of wind profiler observations collected
at Saint-Denis international airport. The statistical analysis clearly shows
important differences in rain vertical profiles as a function of the seasons.
During the dry season, the vertical structure of precipitation is driven by
trade wind and boundary-layer inversions, both of which limit the vertical
extension of the clouds. The rain rate is lower than 2.5 mm h<sup>−1</sup>
throughout the lower part of the troposphere (about 2 km) and decreases in
the higher altitudes. During the moist season, the average rain rate is
around 5 mm h<sup>−1</sup> and nearly uniform from the ground up to 4 km.
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The dynamical and microphysical properties (including drop size
distributions) of four distinct rainfall events are also investigated
through the analysis of four case studies representative of the variety of
rain events occurring on Réunion: summer deep convection,
northerly-to-northeasterly flow atmospheric pattern, cold front and winter
depression embedded in trade winds. Radar-derived rain parameters are in
good agreement with those obtained from collocated rain gauge observations
in all cases, which demonstrates that accurate qualitative and quantitative
analysis can be inferred from wind profiler data. Fluxes of kinetic energy
are also estimated from wind profiler observations in order to evaluate the
impact of rainfall on soil erosion. Results show that horizontal kinetic
energy fluxes are systematically one order of magnitude higher than vertical
kinetic energy fluxes. A simple relationship between the reflectivity factor
and vertical kinetic energy fluxes is proposed based on the results of the
four case studies.
An automated function control unit was developed to regularly check the
ambient particle number concentration derived from a mobility particle size
spectrometer as well as its zero-point behaviour. The function control allows
unattended quality assurance experiments at remote air quality monitoring or
research stations under field conditions. The automated function control also
has the advantage of being able to get a faster system stability response
than the recommended on-site comparisons with reference instruments. The
method is based on a comparison of the total particle number concentration
measured by a mobility particle size spectrometer and a condensation particle
counter while removing diffusive particles smaller than 20 nm in diameter.
In practice, the small particles are removed by a set of diffusion screens,
as traditionally used in a diffusion battery. Another feature of the
automated function control is to check the zero-point behaviour of the
ambient aerosol passing through a high-efficiency particulate air (HEPA)
filter.
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The performance of the function control is illustrated with the aid of a
1-year data set recorded at Annaberg-Buchholz, a station in the Saxon air
quality monitoring network. During the period of concern, the total particle
number concentration derived from the mobility particle size spectrometer
slightly overestimated the particle number concentration recorded by the
condensation particle counter by 2 % (grand average). Based on our first
year of experience with the function control, we developed tolerance criteria
that allow a performance evaluation of a tested mobility particle size
spectrometer with respect to the total particle number concentration. We
conclude that the automated function control enhances the quality and
reliability of unattended long-term particle number size distribution
measurements. This will have beneficial effects for intercomparison studies
involving different measurement sites, and help provide a higher data
accuracy for cohort health and climate research studies.